Two-dimensional single- and multiple-quantum correlation spectroscopy in zero-field nuclear magnetic resonance.

We present single- and multiple-quantum correlation $J$-spectroscopy detected in zero ($<\!\!1$~$\mu$G) magnetic field using a \Rb vapor-cell magnetometer. At zero field the spectrum of ethanol appears as a mixture of \carbon isotopomers, and correlation spectroscopy is useful in separating the two composite spectra. We also identify and observe the zero-field equivalent of a double-quantum transition in ${}^{13}$C$_2$-acetic acid, and show that such transitions are of use in spectral assignment. Two-dimensional spectroscopy further improves the high resolution attained in zero-field NMR since selection rules on the coherence-transfer pathways allow for the separation of otherwise overlappi…

Robust optical readout and characterization of nuclear spin transitions in nitrogen-vacancy ensembles in diamond

Nuclear spin ensembles in diamond are promising candidates for quantum sensing applications, including rotation sensing. Here we perform a characterization of the optically detected nuclear-spin transitions associated with the 14N nuclear spin within diamond nitrogen vacancy (NV) centers. We observe nuclear-spin-dependent fluorescence with the contrast of optically detected 14N nuclear Rabi oscillations comparable to that of the NV electron spin. Using Ramsey spectroscopy, we investigate the temperature and magnetic-field dependence of the nuclear spin transitions in the 77.5-420 K and 350-675 G range, respectively. The nuclear quadrupole coupling constant Q was found to vary with temperatu…

Photoluminescence at the ground-state level anticrossing of the nitrogen-vacancy center in diamond: A comprehensive study

Physical review / B 103(3), 035307 (2021). doi:10.1103/PhysRevB.103.035307

Quantitative measurements of non-covalent interactions with diamond based magnetic imaging

We present a technique employing dielectrophoretic (DEP) manipulation of surface immobilized complexes integrated with a magnetic imaging platform based on nitrogen-vacancy (NV) centers in diamond for the quantitative measurements of non-covalent interactions. The interdigitated microelectrodes closely spaced to the functionalized surface of the diamond plate provide a wide range of applied DEP forces for noninvasive manipulation of various molecular interactions, while the NV layer under the surface reports the unbinding dynamics. Given that biological samples do not present significant magnetic background and do not screen magnetic fields, our approach has many advantages over the fluores…

Fast apparent oscillations of fundamental constants

Precision spectroscopy of atoms and molecules allows one to search for and to put stringent limits on the variation of fundamental constants. These experiments are typically interpreted in terms of variations of the fine structure constant $\alpha$ and the electron to proton mass ratio $\mu=m_e/m_p$. Atomic spectroscopy is usually less sensitive to other fundamental constants, unless the hyperfine structure of atomic levels is studied. However, the number of possible dimensionless constants increases when we allow for fast variations of the constants, where "fast" is determined by the time scale of the response of the studied species or experimental apparatus used. In this case, the relevan…

Isotopic variation of parity violation in atomic ytterbium: Description of the measurement method and analysis of systematic effects

We present a detailed description of experimental studies of the parity violation effect in an isotopic chain of atomic ytterbium (Yb), whose results were reported in a recent paper [Antypas et al., Nat. Phys. 15, 120 (2019)]. We discuss the principle of these measurements, made on the Yb $6{s}^{2} {}^{1}{S}_{0}\ensuremath{\rightarrow}5d6s ^{3}D_{1}$ optical transition at 408 nm, describe the experimental apparatus, and give a detailed account of our studies of systematic effects in the experiment. Our results offer a direct observation of the isotopic variation in the atomic parity violation effect, a variation which is in agreement with the prediction of the standard model. These measurem…

Searching for Earth/Solar axion halos

We discuss the sensitivity of the present and near-future axion dark matter experiments to a halo of axions or axion-like particles gravitationally bound to the Earth or the Sun. The existence of such halos, assuming they are formed, renders a significant gain in the sensitivity of axion searches while satisfying all the present experimental bounds. The structure and coherence properties of these halos also imply novel signals, which can depend on the latitude or orientation of the detector. We demonstrate this by analysing the sensitivity of several distinct types of axion dark matter experiments.

Search for axionlike dark matter with a liquid-state nuclear spin comagnetometer

Physical review letters 122(19), 191302 (2019). doi:10.1103/PhysRevLett.122.191302

Absolute optical chiral analysis using cavity-enhanced polarimetry

Chiral analysis is central for scientific advancement in the fields of chemistry, biology, and medicine. It is also indispensable in the development and quality control of chiral compounds in the chemical and pharmaceutical industries. Current methods for chiral analysis, namely optical polarimetry, mass spectrometry and nuclear magnetic resonance, are either insensitive, have low time resolution, or require preparation steps, and so are unsuited for monitoring chiral dynamics within complex environments: the current need of both research and industry. Here we present the concept of absolute optical chiral analysis, as enabled by cavity-enhanced polarimetry, which allows for accurate unambi…

Infrared laser threshold magnetometry with a NV doped diamond intracavity etalon

International audience; We propose a hybrid laser system consisting of a semiconductor external cavity laser associated to an intra-cavity diamond etalon doped with nitrogen-vacancy color centers. We consider laser emission tuned to the infrared absorption line that is enhanced under the magnetic field dependent nitrogen-vacancy electron spin resonance and show that this architecture leads to a compact solid-state magnetometer that can be operated at room-temperature. The sensitivity to the magnetic field limited by the photon shot-noise of the output laser beam is estimated to be less than 1 pT/ √ Hz. Unlike usual NV center infrared magnetometry, this method would not require an external f…

On-Sky Tests of a High-Power Pulsed Laser for Sodium Laser Guide Star Adaptive Optics

We present results of on-sky tests performed in the summer of 2013 to characterize the performance of a prototype high-power pulsed laser for adaptive optics. The laser operates at a pulse repetition rate (PRR) of 600–800[Formula: see text]Hz, with a 6% duty cycle. Its coupling efficiency was found to be, in the best test case (using 18[Formula: see text]W of transmitted power), [Formula: see text] photons s[Formula: see text] sr[Formula: see text] atom[Formula: see text] W[Formula: see text] m2 when circular polarization was employed and [Formula: see text] photons s[Formula: see text] sr[Formula: see text] atom[Formula: see text] W[Formula: see text] m2 with linear polarization. No impro…

Direct limits on the interaction of antiprotons with axion-like dark matter

Astrophysical observations indicate that there is roughly five times more dark matter in the Universe than ordinary baryonic matter, with an even larger amount of the Universe's energy content due to dark energy. So far, the microscopic properties of these dark components have remained shrouded in mystery. In addition, even the five percent of ordinary matter in our Universe has yet to be understood, since the Standard Model of particle physics lacks any consistent explanation for the predominance of matter over antimatter. Inspired by these central problems of modern physics, we present here a direct search for interactions of antimatter with dark matter, and place direct constraints on th…

Application of spin-exchange relaxation-free magnetometry to the Cosmic Axion Spin Precession Experiment

The Cosmic Axion Spin Precession Experiment (CASPEr) seeks to measure oscillating torques on nuclear spins caused by axion or axion-like-particle (ALP) dark matter via nuclear magnetic resonance (NMR) techniques. A sample spin-polarized along a leading magnetic field experiences a resonance when the Larmor frequency matches the axion/ALP Compton frequency, generating precessing transverse nuclear magnetization. Here we demonstrate a Spin-Exchange Relaxation-Free (SERF) magnetometer with sensitivity $\approx 1~{\rm fT/\sqrt{Hz}}$ and an effective sensing volume of 0.1 $\rm{cm^3}$ that may be useful for NMR detection in CASPEr. A potential drawback of SERF-magnetometer-based NMR detection is …

Polarization-driven spin precession of mesospheric sodium atoms

We report experimental results on the first on-sky observation of atomic spin precession of mesospheric sodium driven by polarization modulation of a continuous-wave laser. The magnetic resonance was remotely detected from the ground by observing the enhancement of induced fluorescence when the driving frequency approached the precession frequency of sodium in the mesosphere, between 85 km and 100 km altitude. The experiment was performed at La Palma, and the uncertainty in the measured Larmor frequency ($\approx$260 kHz) corresponded to an error in the geomagnetic field of 0.4 mG. The results are consistent with geomagnetic field models and with the theory of light-atom interaction in the …

Frequency chirped continuous-wave sodium laser guide stars: modeling and optimization

We numerically study a method to increase the photon return flux of continuous-wave laser guide stars using one-dimensional atomic cooling principles. The method relies on chirping the laser towards higher frequencies following the change in velocity of sodium atoms due to recoil, which raises atomic populations available for laser excitation within the Doppler distribution. The efficiency of this effect grows with the average number of atomic excitations between two atomic collisions in the mesosphere. We find the parameters for maximizing the return flux and evaluate the performance of chirping for operation at La Palma. According to our simulations, the optimal chirp rate lies between 0.…

Stochastic fluctuations of bosonic dark matter

Numerous theories extending beyond the standard model of particle physics predict the existence of bosons that could constitute the dark matter (DM) permeating the universe. In the standard halo model (SHM) of galactic dark matter the velocity distribution of the bosonic DM field defines a characteristic coherence time $\tau_c$. Until recently, laboratory experiments searching for bosonic DM fields have been in the regime where the measurement time $T$ significantly exceeds $\tau_c$, so null results have been interpreted as constraints on the coupling of bosonic DM to standard model particles with a bosonic DM field amplitude $\Phi_0$ fixed by the average local DM density. However, motivate…

Production and detection of atomic hexadecapole at Earth's magnetic field

Anisotropy of atomic states is characterized by population differences and coherences between Zeeman sublevels. It can be efficiently created and probed via resonant interactions with light, the technique which is at the heart of modern atomic clocks and magnetometers. Recently, nonlinear magneto-optical techniques have been developed for selective production and detection of higher polarization moments, hexadecapole and hexacontatetrapole, in the ground states of the alkali atoms. Extension of these techniques into the range of geomagnetic fields is important for practical applications. This is because hexadecapole polarization corresponding to the $\Delta M=4$ Zeeman coherence, with maxim…

Roadmap on STIRAP applications

STIRAP (stimulated Raman adiabatic passage) is a powerful laser-based method, usually involving two photons, for efficient and selective transfer of populations between quantum states. A particularly interesting feature is the fact that the coupling between the initial and the final quantum states is via an intermediate state, even though the lifetime of the latter can be much shorter than the interaction time with the laser radiation. Nevertheless, spontaneous emission from the intermediate state is prevented by quantum interference. Maintaining the coherence between the initial and final state throughout the transfer process is crucial. STIRAP was initially developed with applications in …

Overview of the Cosmic Axion Spin Precession Experiment (CASPEr)

An overview of our experimental program to search for axion and axion-like-particle (ALP) dark matter using nuclear magnetic resonance (NMR) techniques is presented. An oscillating axion field can exert a time-varying torque on nuclear spins either directly or via generation of an oscillating nuclear electric dipole moment (EDM). Magnetic resonance techniques can be used to detect such an effect. The first-generation experiments explore many decades of ALP parameter space beyond the current astrophysical and laboratory bounds. It is anticipated that future versions of the experiments will be sensitive to the axions associated with quantum chromodynamics (QCD) having masses \({\lesssim }10^{…

Constraints on Exotic Spin-Dependent Interactions Between Matter and Antimatter from Antiprotonic Helium Spectroscopy.

Heretofore undiscovered spin-0 or spin-1 bosons can mediate exotic spin-dependent interactions between standard-model particles. Here we carry out the first search for semileptonic spin-dependent interactions between matter and antimatter. We compare theoretical calculations and spectroscopic measurements of the hyperfine structure of antiprotonic helium to constrain exotic spin- and velocity-dependent interactions between electrons and antiprotons.

Optically Enhanced Electric Field Sensing Using Nitrogen-Vacancy Ensembles

Nitrogen-vacancy (NV) centers in diamond have shown promise as inherently localized electric-field sensors, capable of detecting individual charges with nanometer resolution. Working with NV ensembles, we demonstrate that a detailed understanding of the internal electric field environment enables enhanced sensitivity in the detection of external electric fields. We follow this logic along two complementary paths. First, using excitation tuned near the NV's zero-phonon line, we perform optically detected magnetic resonance (ODMR) spectroscopy at cryogenic temperatures in order to precisely measure the NV center's excited-state susceptibility to electric fields. In doing so, we demonstrate th…

Trapping and sympathetic cooling of single thorium ions for spectroscopy

Precision optical spectroscopy of exotic ions reveals accurate information about nuclear properties such as charge radii and magnetic and quadrupole moments. Thorium ions exhibit unique nuclear properties with high relevance for testing symmetries of nature. We report loading and trapping of single $^{232}$Th$^+$ ions in a linear Paul trap, embedded into and sympathetically cooled by small crystals of trapped $^{40}$Ca$^+$ ions. Trapped Th ions are identified in a non-destructive manner from the voids in the laser-induced Ca fluorescence pattern emitted by the crystal, and alternatively, by means of a time-of-flight signal when extracting ions from the Paul trap and steering them into an ex…

Limiting P-odd interactions of cosmic fields with electrons, protons and neutrons

We propose methods for extracting limits on the strength of P-odd interactions of pseudoscalar and pseudovector cosmic fields with electrons, protons and neutrons. Candidates for such fields are dark matter (including axions) and dark energy, as well as several more exotic sources described by standard-model extensions. Calculations of parity nonconserving amplitudes and atomic electric dipole moments induced by these fields are performed for H, Li, Na, K, Rb, Cs, Ba+, Tl, Dy, Fr, and Ra+. From these calculations and existing measurements in Dy, Cs and Tl, we constrain the interaction strengths of the parity-violating static pseudovector cosmic field to be 7*10^(-15) GeV with an electron, a…

Intensity interferometry for ultralight bosonic dark matter detection

Ultralight bosonic dark matter (UBDM) can be described by a classical wave-like field oscillating near the Compton frequency of the bosons. If a measurement scheme for the direct detection of UBDM interactions is sensitive to a signature quadratic in the field, then there is a near-zero-frequency (dc) component of the signal. Thus, a detector with a given finite bandwidth can be used to search for bosons with Compton frequencies many orders of magnitude larger than its bandwidth. This opens the possibility of a detection scheme analogous to Hanbury Brown and Twiss intensity interferometry. Assuming that the UBDM is virialized in the galactic gravitational potential, the random velocities pr…

Lower than low: Perspectives on zero- to ultralow-field nuclear magnetic resonance

Abstract The less-traveled low road in nuclear magnetic resonance is discussed, honoring the contributions of Prof. Bernhard Blumich, aspiring towards reaching ‘a new low.’ A history of the subject and its current status are briefly reviewed, followed by an effort to prophesy possible directions for future developments.

A Precise Photometric Ratio via Laser Excitation of the Sodium Layer II: Two-photon Excitation Using Lasers Detuned from 589.16 nm and 819.71 nm Resonances

This article is the second in a pair of articles on the topic of the generation of a two-color artificial star (which we term a "laser photometric ratio star," or LPRS) of de-excitation light from neutral sodium atoms in the mesosphere, for use in precision telescopic measurements in astronomy and atmospheric physics, and more specifically for the calibration of measurements of dark energy using type Ia supernovae. The two techniques respectively described in both this and the previous article would each generate an LPRS with a precisely 1:1 ratio of yellow (589/590 nm) photons to near-infrared (819/820 nm) photons produced in the mesosphere. Both techniques would provide novel mechanisms f…

Analysis method for detecting topological defect dark matter with a global magnetometer network

Abstract The Global Network of Optical Magnetometers for Exotic physics searches (GNOME) is a network of time-synchronized, geographically separated, optically pumped atomic magnetometers that is being used to search for correlated transient signals heralding exotic physics. GNOME is sensitive to exotic couplings of atomic spins to certain classes of dark matter candidates, such as axions. This work presents a data analysis procedure to search for axion dark matter in the form of topological defects: specifically, walls separating domains of discrete degenerate vacua in the axion field. An axion domain wall crossing the Earth creates a distinctive signal pattern in the network that can be d…

Erwin Louis Hahn. 9 June 1921—20 September 2016

Erwin Louis Hahn was one of the most innovative physical scientists in recent history, impacting generations of scientists through his work in nuclear magnetic resonance (NMR), optics, and the intersection of these two fields. Starting with his discovery of the spin echo, a phenomenon of monumental significance and practical importance, Hahn launched a revolution in how we think about spin physics, with numerous implications following in many other areas of science. Current students of NMR and coherent optics quickly discover that many of the key concepts and techniques in these fields derive directly from his work.

Zero- to Ultralow-Field Nuclear Magnetic Resonance Enhanced with Dissolution Dynamic Nuclear Polarization.

Zero- to ultralow-field nuclear magnetic resonance is a modality of magnetic resonance experiment which does not require strong superconducting magnets. Contrary to conventional high-field nuclear magnetic resonance, it has the advantage of allowing high resolution detection of nuclear magnetism through metal as well as within heterogeneous media. To achieve high sensitivity, it is common to couple zero-field nuclear magnetic resonance with hyperpolarization techniques. To date, the most common technique is parahydrogen-induced polarization, which is only compatible with a small number of compounds. In this article, we establish dissolution dynamic nuclear polarization as a versatile method…

Studies towards a directional polychromatic sodium laser guide star

In this work we discuss a mechanism for generation of a coherent source of light from the mesosphere as a new concept of directional laser guide star. In contrast to the near-isotropic spontaneous emission, nonlinear processes in atomic vapors like amplified spontaneous emission can yield highly directional emission in the forward and backward directions. Along with directional emission, excited sodium atoms also radiate at different wavelength creating a polychromatic laser guide star (PLGS). If feasible, a directional PLGS would provide a net gain in the return flux of several orders of magnitude compared to traditional LGS schemes, making possible laser-guided tip/tilt-correction in adap…

Real-Time Nuclear Magnetic Resonance Detection of Fumarase Activity Using Parahydrogen-Hyperpolarized [1- 13 C]Fumarate

Hyperpolarized fumarate can be used as a probe of real-time metabolism in vivo, using carbon-13 magnetic resonance imaging. Dissolution dynamic nuclear polarization is commonly used to produce hyperpolarized fumarate, but a cheaper and faster alternative is to produce hyperpolarized fumarate via PHIP (parahydrogen-induced polarization). In this work, we trans-hydrogenate [1-13C]acetylene dicarboxylate with para-enriched hydrogen using a commercially available Ru catalyst in water to produce hyperpolarized [1-13C]fumarate. We show that fumarate is produced in 89% yield, with succinate as a side product in 11% yield. The proton polarization is converted into 13C magnetization using a constant…

A network of superconducting gravimeters as a detector of matter with feeble nongravitational coupling

Abstract Hidden matter that interacts only gravitationally would oscillate at characteristic frequencies when trapped inside of Earth. For small oscillations near the center of the Earth, these frequencies are around 300 μHz. Additionally, signatures at higher harmonics would appear because of the non-uniformity of Earth’s density. In this work, we use data from a global network of gravimeters of the International Geodynamics and Earth Tide Service (IGETS) to look for these hypothetical trapped objects. We find no evidence for such objects with masses on the order of 1014 kg or greater with an oscillation amplitude of 0.1 re. It may be possible to improve the sensitivity of the search by s…

Action potentials induce biomagnetic fields in Venus flytrap plants

Upon stimulation, plants elicit electrical signals that can travel within a cellular network analogous to the animal nervous system. It is well-known that in the human brain, voltage changes in certain regions result from concerted electrical activity which, in the form of action potentials (APs), travels within nerve-cell arrays. Electrophysiological techniques like electroencephalography, magnetoencephalography, and magnetic resonance imaging are used to record this activity and to diagnose disorders. In the plant kingdom, two types of electrical signals are observed: all-or-nothing APs of similar amplitudes to those seen in humans and animals, and slow-wave potentials of smaller amplitud…

Fiberized diamond-based vector magnetometers

Frontiers 2, 732748 (2021). doi:10.3389/fphot.2021.732748

Gravity Probe Spin: Prospects for measuring general-relativistic precession of intrinsic spin using a ferromagnetic gyroscope

An experimental test at the intersection of quantum physics and general relativity is proposed: measurement of relativistic frame dragging and geodetic precession using intrinsic spin of electrons. The behavior of intrinsic spin in spacetime dragged and warped by a massive rotating body is an experimentally open question, hence the results of such a measurement could have important theoretical consequences. Such a measurement is possible by using mm-scale ferromagnetic gyroscopes in orbit around the Earth. Under conditions where the rotational angular momentum of a ferromagnet is sufficiently small, a ferromagnet's angular momentum is dominated by atomic electron spins and is predicted to e…

Magnetic Gradiometer for Detection of Zero- and Ultralow-Field Nuclear Magnetic Resonance

Magnetic sensors are important for detecting nuclear magnetization signals in nuclear magnetic resonance (NMR). As a complementary analysis tool to conventional high-field NMR, zero- and ultralow-field (ZULF) NMR detects nuclear magnetization signals in the sub-microtesla regime. Current ZULF NMR systems are always equipped with high-quality magnetic shieldings to ensure that ambient magnetic field noise does not dwarf the magnetization signal. An alternative approach is to separate the magnetization signal from the noise based on their differing spatial profiles, as can be achieved using a magnetic gradiometer. Here, we present a gradiometric ZULF NMR spectrometer with a magnetic gradient …

All-Optical Spin Locking in Alkali-Vapor Magnetometers

The nonlinear Zeeman effect can induce splittings and asymmetries of magnetic-resonance lines in the geophysical magnetic-field range. We demonstrate a scheme to suppress the nonlinear Zeeman effect all optically based on spin locking. Spin locking is achieved with an effective oscillating magnetic field provided by the AC Stark-shift of an intensity-modulated and polarization-modulated laser beam. This results in the collapse of the multi-component asymmetric magnetic-resonance line with about 100 Hz width in the Earth-field range into a peak with a central component width of 25Hz. The technique is expected to be broadly applicable in practical magnetometry, potentially boosting the sensit…

Low-energy Tests of Fundamental Physics

This article presents a personal perspective on why it is interesting and important to test all kinds of fundamental laws and search for as-yet-undiscovered particles and interactions using laboratory-based non-accelerator techniques. Such room-scale experiments are already spearheading discovery, and can be expected to become even more important as accelerators reach seemingly inevitable limits.

Battery Diagnostics with Sensitive Magnetometry

The ever-increasing demand for high-capacity rechargeable batteries highlights the need for sensitive and accurate diagnostic technology for determining the state of a cell, for identifying and localizing defects, or for sensing capacity loss mechanisms. Here, we demonstrate the use of atomic magnetometry to map the weak induced magnetic fields around a Li-ion battery cell as a function of state of charge and upon introducing mechanical defects. These measurements provide maps of the magnetic susceptibility of the cell, which follow trends characteristic for the battery materials under study upon discharge. In addition, the measurements reveal hitherto unknown long time-scale transient inte…

Simulations of continuous-wave sodium laser guide stars with polarization modulation at Larmor frequency

The return flux from a sodium laser guide star suffers, at large angles between the geomagnetic field and the laser beam, from the reduction in optical pumping due to spin-precession of sodium atoms. This detrimental effect can be mitigated by modulating the circular polarization of a continuous-wave laser beam in resonance with the Larmor frequency of sodium atoms in the mesosphere. We present an investigation based on numerical modeling to evaluate the brightness enhancement of a laser guide star with polarization modulation of a continuous-wave laser beam at different observatories.

Sodium vapor cell laser guide star experiments for continuous wave model validation

Recent numerical simulations and experiments on sodium Laser Guide Star (LGS) have shown that a continuous wave (CW) laser with circular polarization and re-pumping should maximize the fluorescent photon return flux to the wavefront sensor for adaptive optics applications. The orientation and strength of the geomagnetic field in the sodium layer also play an important role affecting the LGS return ux. Field measurements of the LGS return flux show agreement with the CW LGS model, however, fluctuations in the sodium column abundance and geomagnetic field intensity, as well as atmospheric turbulence, induce experimental uncertainties. We describe a laboratory experiment to measure the photon …

Search for the effect of massive bodies on atomic spectra and constraints on Yukawa-type interactions of scalar particles

We propose a new method to search for hypothetical scalar particles that have feeble interactions with Standard-Model particles. In the presence of massive bodies, these interactions produce a non-zero Yukawa-type scalar-field magnitude. Using radio-frequency spectroscopy data of atomic dysprosium, as well as atomic clock spectroscopy data, we constrain the Yukawa-type interactions of a scalar field with the photon, electron, and nucleons for a range of scalar-particle masses corresponding to length scales $ > 10$ cm. In the limit as the scalar-particle mass $m_\phi \to 0$, our derived limits on the Yukawa-type interaction parameters are: $\Lambda_\gamma \gtrsim 8 \times 10^{19}$ GeV, $\Lam…

Transition-Selective Pulses in Zero-Field Nuclear Magnetic Resonance.

We use low-amplitude, ultralow frequency pulses to drive nuclear spin transitions in zero and ultralow magnetic fields. In analogy to high-field NMR, a range of sophisticated experiments becomes available as these allow narrow-band excitation. As a first demonstration, pulses with excitation bandwidths 0.5–5 Hz are used for population redistribution, selective excitation, and coherence filtration. These methods are helpful when interpreting zero- and ultralow-field NMR spectra that contain a large number of transitions.

Magnetometry with Nitrogen-Vacancy Centers in Diamond

This chapter covers magnetic sensing with nitrogen-vacancy (NV) defect centers in diamond. The NV center fundamentals are introduced and NV optically detected magnetic resonance techniques for dc and ac magnetic sensing are summarized. After reviewing some successful sensing applications, the advantages for using NV magnetometry, as well as some ongoing challenges, are enumerated.

Characterization of the global network of optical magnetometers to search for exotic physics (GNOME)

The Global Network of Optical Magnetometers to search for Exotic physics (GNOME) is a network of geographically separated, time-synchronized, optically pumped atomic magnetometers that is being used to search for correlated transient signals heralding exotic physics. The GNOME is sensitive to nuclear- and electron-spin couplings to exotic fields from astrophysical sources such as compact dark-matter objects (for example, axion stars and domain walls). Properties of the GNOME sensors such as sensitivity, bandwidth, and noise characteristics are studied in the present work, and features of the network's operation (e.g., data acquisition, format, storage, and diagnostics) are described. Charac…

Determination of local defect density in diamond by double electron-electron resonance

Magnetic impurities in diamond influence the relaxation properties and thus limit the sensitivity of magnetic, electric, strain, and temperature sensors based on nitrogen-vacancy color centers. Diamond samples may exhibit significant spatial variations in the impurity concentrations hindering the quantitative analysis of relaxation pathways. Here, we present a local measurement technique which can be used to determine the concentration of various species of defects by utilizing double electron-electron resonance. This method will help to improve the understanding of the physics underlying spin relaxation and guide the development of diamond samples, as well as offering protocols for optimiz…

Singulett‐Kontrast‐Magnetresonanztomographie: Freisetzung der Hyperpolarisation durch den Metabolismus**

A machine learning algorithm for direct detection of axion-like particle domain walls

The Global Network of Optical Magnetometers for Exotic physics searches (GNOME) conducts an experimental search for certain forms of dark matter based on their spatiotemporal signatures imprinted on a global array of synchronized atomic magnetometers. The experiment described here looks for a gradient coupling of axion-like particles (ALPs) with proton spins as a signature of locally dense dark matter objects such as domain walls. In this work, stochastic optimization with machine learning is proposed for use in a search for ALP domain walls based on GNOME data. The validity and reliability of this method were verified using binary classification. The projected sensitivity of this new analy…

Coherent axion-photon transformations in the forward scattering on atoms

In certain laboratory experiments the production and/or detection of axions is due to the photon-axion transformations in a strong magnetic field. This process is coherent, and the rate of the transformation is proportional to the length $l$ and magnitude $B$ of the magnetic field squared, $\sim l^2B^2$. In the present paper, we consider coherent production of axions due to the forward scattering of photons on atoms or molecules. This process may be represented as being due to an effective electromagnetic field which converts photons to axions. We present analytical expressions for such effective magnetic and electric fields induced by resonant atomic M0 and M1 transitions, as well as give …

Resonant detection and production of axions with atoms

The axions and axion-like particles can be detected via a resonant atomic or molecular transition induced by axion absorption. The signal obtained in this process is second order in the axion-electron interaction constant and hence small. In this chapter, it is demonstrated that this signal may become first order in the axion-electron interaction constant if we allow the interference between the axion-induced transition amplitude and the transition amplitude induced by the electromagnetic radiation. Additionally, we show that the conventional scheme of producing axions from photons in a magnetic field may be improved if the field is replaced by an atomic medium in which photons scattering …

Singlet‐Contrast Magnetic Resonance Imaging: Unlocking Hyperpolarization with Metabolism

Abstract Hyperpolarization‐enhanced magnetic resonance imaging can be used to study biomolecular processes in the body, but typically requires nuclei such as 13C, 15N, or 129Xe due to their long spin‐polarization lifetimes and the absence of a proton‐background signal from water and fat in the images. Here we present a novel type of 1H imaging, in which hyperpolarized spin order is locked in a nonmagnetic long‐lived correlated (singlet) state, and is only liberated for imaging by a specific biochemical reaction. In this work we produce hyperpolarized fumarate via chemical reaction of a precursor molecule with para‐enriched hydrogen gas, and the proton singlet order in fumarate is released a…

Local Lorentz invariance tests for photons and hadrons at the Gamma Factory

High-precision tests of local Lorentz invariance, via monitoring of the sidereal time variation of the photon energies emitted by ultrarelativistic heavy-ion beams and of the beam momentum, are proposed. This paper includes descriptions of the physics ideas and the concept for the detector. The experiment results will allow high-precision tests of LLI via anisotropy of the maximum attainable speed of a photon and an ion. The projected accuracy for the asymmetries interpreted in the framework of the anisotropic relativistic mechanics corresponds to the limit on sidereal time variation of the one-way maximum attainable speed at the levels between $10^{-14}$ and $10^{-17}$.

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A Precessing Ferromagnetic Needle Magnetometer

A ferromagnetic needle is predicted to precess about the magnetic field axis at a Larmor frequency $\Omega$ under conditions where its intrinsic spin dominates over its rotational angular momentum, $N\hbar \gg I\Omega$ ($I$ is the moment of inertia of the needle about the precession axis and $N$ is the number of polarized spins in the needle). In this regime the needle behaves as a gyroscope with spin $N\hbar$ maintained along the easy axis of the needle by the crystalline and shape anisotropy. A precessing ferromagnetic needle is a correlated system of $N$ spins which can be used to measure magnetic fields for long times. In principle, by taking advantage of rapid averaging of quantum unce…

Continuous-wave mirrorless lasing at 221  μm in sodium vapors

We demonstrate backward-directed continuous-wave (cw) emission at 2.21 {\mu}m generated on the 4P3/2-4S1/2 population-inverted transition in Na vapors two-photon excited with resonant laser light at 589 and 569 nm. Our study of power and atom-number-density threshold characteristics shows that lasing occurs at sub-10 mW total power of the applied laser light. The observed 6 mrad divergence is defined mainly by the aspect ratio of the gain region. We find that mirrorless lasing at 2.21 {\mu}m is magnetic field and polarization dependent that may be useful for remote magnetometry. The presented results could help determine the requirements for obtaining directional return from sodium atoms in…

Nonlinear magneto-optical rotation in rubidium vapor excited with blue light

We present experimental and numerical studies of nonlinear magneto-optical rotation (NMOR) in rubidium vapor excited with resonant light tuned to the $5^2\!S_{1/2}\rightarrow 6^2\!P_{1/2}$ absorption line (421~nm). Contrary to the experiments performed to date on the strong $D_1$ or $D_2$ lines, in this case, the spontaneous decay of the excited state $6^2\!P_{1/2}$ may occur via multiple intermediate states, affecting the dynamics, magnitude and other characteristics of NMOR. Comparing the experimental results with the results of modelling based on Auzinsh et al., Phys. Rev. A 80, 1 (2009), we demonstrate that despite the complexity of the structure, NMOR can be adequately described with a…

The cosmic axion spin precession experiment (CASPEr): a dark-matter search with nuclear magnetic resonance

The Cosmic Axion Spin Precession Experiment (CASPEr) is a nuclear magnetic resonance experiment (NMR) seeking to detect axion and axion-like particles which could make up the dark matter present in the universe. We review the predicted couplings of axions and axion-like particles with baryonic matter that enable their detection via NMR. We then describe two measurement schemes being implemented in CASPEr. The first method, presented in the original CASPEr proposal, consists of a resonant search via continuous-wave NMR spectroscopy. This method offers the highest sensitivity for frequencies ranging from a few Hz to hundreds of MHz, corresponding to masses $ m_{\rm a} \sim 10^{-14}$--$10^{-6}…

Search for Ultralight Scalar Dark Matter with Atomic Spectroscopy

We report new limits on ultralight scalar dark matter (DM) with dilaton-like couplings to photons that can induce oscillations in the fine-structure constant alpha. Atomic dysprosium exhibits an electronic structure with two nearly degenerate levels whose energy splitting is sensitive to changes in alpha. Spectroscopy data for two isotopes of dysprosium over a two-year span is analyzed for coherent oscillations with angular frequencies below 1 rad/s. No signal consistent with a DM coupling is identified, leading to new constraints on dilaton-like photon couplings over a wide mass range. Under the assumption that the scalar field comprises all of the DM, our limits on the coupling exceed tho…

Improving the coherence properties of solid-state spin ensembles via optimized dynamical decoupling

In this work, we optimize a dynamical decoupling (DD) protocol to improve the spin coherence properties of a dense ensemble of nitrogen-vacancy (NV) centers in diamond. Using liquid nitrogen-based cooling and DD microwave pulses, we increase the transverse coherence time T2 from ∼ 0.7 ms up to ∼ 30 ms. We extend previous work of single-axis (Carr-Purcell-Meiboom-Gill) DD towards the preservation of arbitrary spin states. After performing a detailed analysis of pulse and detuning errors, we compare the performance of various DD protocols. We identify that the concatenated XY8 pulse sequences serves as the optimal control scheme for preserving an arbitrary spin state. Finally, we use the conc…

Longitudinal spin-relaxation in nitrogen-vacancy centers in electron irradiated diamond

We present systematic measurements of longitudinal relaxation rates ($1/T_1$) of spin polarization in the ground state of the nitrogen-vacancy (NV$^-$) color center in synthetic diamond as a function of NV$^-$ concentration and magnetic field $B$. NV$^-$ centers were created by irradiating a Type 1b single-crystal diamond along the [100] axis with 200 keV electrons from a transmission electron microscope with varying doses to achieve spots of different NV$^-$ center concentrations. Values of ($1/T_1$) were measured for each spot as a function of $B$.

Production and detection of atomic hexadecapole at Earth’s magnetic field

We report a novel method that allows selective creation and detection of a macroscopic long lived hexadecapole polarization in the F = 2 ground state of 87Rb atoms at Earth's magnetic field (510 mG).

Spin Hyperpolarization in Modern Magnetic Resonance.

Magnetic resonance techniques are successfully utilized in a broad range of scientific disciplines and in a number of practical applications, with medical MRI being the most widely-known example. Currently, both fundamental and applied magnetic resonance are enjoying a major boost owing to the dramatic signal enhancement provided by the rapidly-developing field of spin hyperpolarization. Such techniques are able to enhance signal intensities in magnetic resonance by several orders of magnitude, and thus to largely overcome its major disadvantage of relatively low sensitivity compared to other analytical techniques. This provides new impetus for existing applications, and, even more importan…

Measuring molecular parity nonconservation using nuclear-magnetic-resonance spectroscopy

The weak interaction does not conserve parity and therefore induces energy shifts in chiral enantiomers that should in principle be detectable in molecular spectra. Unfortunately, the magnitude of the expected shifts are small and in spectra of a mixture of enantiomers, the energy shifts are not resolvable. We propose a nuclear magnetic resonance (NMR) experiment in which we titrate the chirality (enantiomeric excess) of a solvent and measure the diasteriomeric splitting in the spectra of a chiral solute in order to search for an anomalous offset due to parity nonconservation (PNC). We present a proof-of-principle experiment in which we search for PNC in the \textsuperscript{13}C resonances…

Detection of missing low-lying atomic states in actinium

Two lowest-energy odd-parity atomic levels of actinium, 7s^27p 2P^o_1/2, 7s^27p 2P^o_3/2, were observed via two-step resonant laser-ionization spectroscopy and their respective energies were measured to be 7477.36(4) cm^-1 and 12 276.59(2) cm^-1. The lifetimes of these states were determined as 668(11) ns and 255(7) ns, respectively. In addition, these properties were calculated using a hybrid approach that combines configuration interaction and coupled-cluster methods in good agreement. The data are of relevance for understanding the complex atomic spectra of actinides and for developing efficient laser-cooling and ionization schemes for actinium, with possible applications for high-purity…

Search for New Physics with Atoms and Molecules

This article reviews recent developments in tests of fundamental physics using atoms and molecules, including the subjects of parity violation, searches for permanent electric dipole moments, tests of the CPT theorem and Lorentz symmetry, searches for spatiotemporal variation of fundamental constants, tests of quantum electrodynamics, tests of general relativity and the equivalence principle, searches for dark matter, dark energy and extra forces, and tests of the spin-statistics theorem. Key results are presented in the context of potential new physics and in the broader context of similar investigations in other fields. Ongoing and future experiments of the next decade are discussed.

Suppression of nonlinear Zeeman effect and heading error in earth-field-range alkali-vapor magnetometers

The nonlinear Zeeman effect can induce splitting and asymmetries of magnetic-resonance lines in the geophysical magnetic field range. This is a major source of "heading error" for scalar atomic magnetometers. We demonstrate a method to suppress the nonlinear Zeeman effect and heading error based on spin locking. In an all-optical synchronously pumped magnetometer with separate pump and probe beams, we apply a radio-frequency field which is in-phase with the precessing magnetization. In an earth-range field, a multi-component asymmetric magnetic-resonance line with ? 60 Hz width collapses into a single peak with a width of 22 Hz, whose position is largely independent of the orientation of th…

Infrasonic, Acoustic and Seismic Waves Produced by the Axion Quark Nuggets

We advocate an idea that the Axion Quark Nuggets (AQN) hitting the Earth can be detected by analysing the infrasound, acoustic and seismic waves which always accompany the AQN's passage in the atmosphere and underground. Our estimates for the infrasonic frequency $\nu\simeq 5$ ~Hz and overpressure $\delta p\sim 0.3 ~$Pa for relatively large size dark matter (DM) nuggets suggest that sensitivity of presently available instruments is already sufficient to detect very intense (but very rare) events today with existing technology. A study of much more frequent but less intense events requires a new type of instruments. We propose a detection strategy for a systematic study to search for such re…

Dependence of atomic parity-violation effects on neutron skins and new physics

We estimate the relative contribution of nuclear structure and new physics couplings to the parity non-conserving spin-independent effects in atomic systems, for both single isotopes and isotopic ratios. General expressions are presented to assess the sensitivity of isotopic ratios to neutron skins and to couplings beyond standard model at tree level. The specific coefficients for these contributions are calculated assuming Fermi distribution for proton and neutron nuclear densities for isotopes of Cs, Ba, Sm, Dy, Yb, Pb, Fr, and Ra. The present work aims to provide a guide to the choice of the best isotopes and pairs of isotopes for conducting atomic PNC measurements.

Quantum technologies and the elephants

Extraordinary progress in quantum sensors and technologies opens new avenues for exploring the Universe and testing the assumptions forming the basis of modern physics. This QST focus issue: focus on quantum sensors for new-physics discoveries is a next-decade roadmap on developing a wide range of quantum sensors and new technologies towards discoveries of new physics. It covers the next generation of various technologies, including atomic and nuclear clocks, atomic and diamond-based magnetometers, atom and laser interferometers, control of trapped atoms, ions, and molecules, optomechanical systems, and many others. In this editorial, we outline major problems of fundamental physics we aim …

Detection of the Lowest-Lying Odd-Parity Atomic Levels in Actinium

Two lowest-energy odd-parity atomic levels of actinium, 7s27pP21/2o, 7s27pP23/2o, were observed via two-step resonant laser-ionization spectroscopy and their respective energies were measured to be 7477.36(4) and 12 276.59(2) cm-1. The lifetimes of these states were determined as 668(11) and 255(7) ns, respectively. In addition, we observed the effect of the hyperfine structure on the line for the transition to P23/2o. These properties were calculated using a hybrid approach that combines configuration interaction and coupled-cluster methods, in good agreement with the experiment. The data are of relevance for understanding the complex atomic spectra of actinides and for developing efficien…

13C-Decoupled J-Coupling Spectroscopy Using Two-Dimensional Nuclear Magnetic Resonance at Zero-Field

We present a two-dimensional method for obtaining 13C-decoupled, 1H-coupled nuclear magnetic resonance (NMR) spectra in zero magnetic field using coherent spin-decoupling. The result is a spectrum determined only by the proton–proton J-coupling network. Detection of NMR signals in zero magnetic field requires at least two different nuclear spin species, but the proton J-spectrum is independent of isotopomer, thus potentially simplifying spectra and thereby improving the analytical capabilities of zero-field NMR. The protocol does not rely on a difference in Larmor frequency between the coupled nuclei, allowing for the direct determination of J-coupling constants between chemically equivalen…

Four-wave mixing in a ring cavity

We investigate a four-wave mixing process in an N interaction scheme in Rb vapor placed inside a low-finesse ring cavity. We observe strong amplification and generation of a probe signal, circulating in the cavity, in the presence of two strong optical pump fields. We study the variations in probe field gain and dispersion as functions of experimental parameters with an eye on potential application of such a system for enhanced rotation measurements. A density-matrix calculation is performed to model the system, and the theoretical results are compared to those of the experiment.

Photoelectrical detection of electron spin resonance of nitrogen-vacancy centres in diamond

The protocols for the control and readout of Nitrogen Vacancy (NV) centres electron spins in diamond offer an advanced platform for quantum computation, metrology and sensing. These protocols are based on the optical readout of photons emitted from NV centres, which process is limited by the yield of photons collection. Here we report on a novel principle for the detection of NV centres magnetic resonance in diamond by directly monitoring spin-preserving electron transitions through measurement of NV centre related photocurrent. The demonstrated direct detection technique offers a sensitive way for the readout of diamond NV sensors and diamond quantum devices on diamond chips. The Photocurr…

Resonance photoproduction of pionic atoms at the proposed Gamma Factory

We present a possibility of direct resonance production of pionic atoms (Coulomb bound states of a negative pion and a nucleus) with a rate of up to $\ensuremath{\approx}{10}^{10}$ per second using the gamma-ray beams from the Gamma Factory.

A precise photometric ratio via laser excitation of the sodium layer - I. One-photon excitation using 342.78 nm light

The largest uncertainty on measurements of dark energy using type Ia supernovae is presently due to systematics from photometry; specifically to the relative uncertainty on photometry as a function of wavelength in the optical spectrum. We show that a precise constraint on relative photometry between the visible and near-infrared can be achieved in upcoming surveys (such as in LSST at the Vera C. Rubin Observatory) via a mountaintop-located laser source tuned to the 342.78 nm vacuum excitation wavelength of neutral sodium atoms. Using a high-power (500 W) laser modified from laser guide star studies, this excitation will produce an artificial star (which we term a "laser photometric ratio s…

Revisiting spin-dependent forces mediated by new bosons : potentials in the coordinate-space representation for macroscopic- and atomic-scale experiments

The exchange of spin-0 or spin-1 bosons between fermions or spin-polarised macroscopic objects gives rise to various spin-dependent potentials. We derive the coordinate-space non-relativistic potentials induced by the exchange of such bosons, including contact terms that can play an important role in atomic-scale phenomena, and correct for errors and omissions in the literature. We summarise the properties of the potentials and their relevance for various types of experiments. These potentials underpin the interpretation of experiments that search for new bosons, including spectroscopy, torsion-pendulum measurements, magnetometry, parity nonconservation and electric dipole moment experiment…

Interference-assisted resonant detection of axions

Detection schemes for the quantum chromodynamics axions and other axion-like particles in light-shining-through-a-wall (LSW) experiments are based on the conversion of these particles into photons in a magnetic field. An alternative scheme may involve the detection via a resonant atomic or molecular transition induced by resonant axion absorption. The signal obtained in this process is second order in the axion-electron interaction constant but may become first order if we allow interference between the axion-induced transition amplitude and the transition amplitude induced by the electromagnetic radiation that produces the axions.

Hyperfine level structure in nitrogen-vacancy centers near the ground-state level anticrossing

Energy levels of nitrogen-vacancy centers in diamond were investigated using optically detected magnetic-resonance spectroscopy near the electronic ground-state level anticrossing (GSLAC) at an axial magnetic field around 102.4~mT in diamond samples with a nitrogen concentration of 1~ppm and 200~ppm. By applying radiowaves in the frequency ranges from 0 to 40 MHz and from 5.6 to 5.9 GHz, we observed transitions that involve energy levels mixed by the hyperfine interaction. We developed a theoretical model that describes the level mixing, transition energies, and transition strengths between the ground-state sublevels, including the coupling to the nuclear spin of the NV center\textquotesing…

Polychromatic, continuous-wave mirrorless lasing from monochromatic pumping of cesium vapor

We report on studies of simultaneous continuous-wave mirrorless lasing on multiple optical transitions, realized by pumping hot cesium vapor with laser light resonant with the 6$S_{1/2}\rightarrow 8$P$_{3/2}$ transition. The multiplicity of decay paths for the excited atoms to their ground state is responsible for the emergence of lasing in a number of transitions, observed here in at least seven wavelengths in the infrared (IR), and at two wavelengths in the blue. We study the properties of the fields generated in the cesium vapor, such as optical power, directionality and optical linewidth.

Polarization transfer via field sweeping in parahydrogen-enhanced nuclear magnetic resonance.

&lt;div&gt;&lt;br&gt;&lt;/div&gt;&lt;div&gt;&lt;table&gt;&lt;tr&gt;&lt;td&gt;We show that in a spin system of two magnetically inequivalent protons coupled to a heteronucleus such as 13C, an adiabatic magnetic field sweep, passing through zero field, transfers proton singlet order into magnetization of the coupled heteronucleus. This effect is potentially useful in parahydrogen-enhanced nuclear magnetic resonance, and is demonstrated on singlet-hyperpolarized [1-13C]maleic acid, which is prepared via the reaction between [1-13C]acetylene dicarboxylic acid and para-enriched hydrogen gas. The magnetic field sweeps are of microtesla amplitudes, and have durations on the order of seconds. We sh…

Opportunities for Fundamental Physics Research with Radioactive Molecules

Molecules containing short-lived, radioactive nuclei are uniquely positioned to enable a wide range of scientific discoveries in the areas of fundamental symmetries, astrophysics, nuclear structure, and chemistry. Recent advances in the ability to create, cool, and control complex molecules down to the quantum level, along with recent and upcoming advances in radioactive species production at several facilities around the world, create a compelling opportunity to coordinate and combine these efforts to bring precision measurement and control to molecules containing extreme nuclei. In this manuscript, we review the scientific case for studying radioactive molecules, discuss recent atomic, mo…

Imaging the local charge environment of nitrogen-vacancy centers in diamond

Characterizing the local internal environment surrounding solid-state spin defects is crucial to harnessing them as nanoscale sensors of external fields. This is especially germane to the case of defect ensembles which can exhibit a complex interplay between interactions, internal fields and lattice strain. Working with the nitrogen-vacancy (NV) center in diamond, we demonstrate that local electric fields dominate the magnetic resonance behavior of NV ensembles at low magnetic field. We introduce a simple microscopic model that quantitatively captures the observed spectra for samples with NV concentrations spanning over two orders of magnitude. Motivated by this understanding, we propose an…

Atomic and molecular transitions induced by axions via oscillating nuclear moments

The interaction of standard model's particles with the axionic Dark Matter field may generate oscillating nuclear electric dipole moments (EDMs), oscillating nuclear Schiff moments and oscillating nuclear magnetic quadrupole moments (MQMs) with a frequency corresponding to the axion's Compton frequency. Within an atom or a molecule an oscillating EDM, Schiff moment or MQM can drive transitions between atomic or molecular states. The excitation events can be detected, for example, via subsequent fluorescence or photoionization. Here we calculate the rates of such transitions. If the nucleus has octupole deformation or quadrupole deformation then the transition rate due to Schiff moment and M…

Parity-violating interactions of cosmic fields with atoms, molecules, and nuclei: Concepts and calculations for laboratory searches and extracting limits

We propose methods and present calculations that can be used to search for evidence of cosmic fields by investigating the parity-violating effects, including parity nonconservation amplitudes and electric dipole moments, that they induce in atoms. The results are used to constrain important fundamental parameters describing the strength of the interaction of various cosmic fields with electrons, protons, and neutrons. Candidates for such fields are dark matter (including axions) and dark energy, as well as several more exotic sources described by standard-model extensions. Existing parity nonconservation experiments in Cs, Dy, Yb, and Tl are combined with our calculations to directly place …

Photochemically induced dynamic nuclear polarization of heteronuclear singlet order

Photochemically induced dynamic nuclear polarization (photo-CIDNP) is a method to hyperpolarize nuclear spins using light. In most cases, CIDNP experiments are performed in high magnetic fields and the sample is irradiated by light inside a nuclear magnetic resonance (NMR) spectrometer. Here we demonstrate photo-CIDNP hyperpolarization generated in the Earth's magnetic field and under zero- to ultralow-field (ZULF) conditions. Irradiating a sample containing tetraphenylporphyrin and para-benzoquinone for several seconds with light-emitting diodes produces strong hyperpolarization of 1H and 13C nuclear spins, enhancing the NMR signals more than 200 times. The hyperpolarized spin states at th…

Sidebands in Optically Detected Magnetic Resonance Signals of Nitrogen Vacancy Centers in Diamond

We study features in the optically detected magnetic resonance (ODMR) signals associated with negatively charged nitrogen-vacancy (NV) centers coupled to other paramagnetic impurities in diamond. Our results are important for understanding ODMR line shapes and for optimization of devices based on NV centers. We determine the origins of several side features to the unperturbed NV magnetic resonance by studying their magnetic field and microwave power dependences. Side resonances separated by around 130 MHz are due to hyperfine coupling between NV centers and nearest-neighbor C-13 nuclear spins. Side resonances separated by approximately {40, 260, 300} MHz are found to originate from simultan…

Optically detected magnetic resonances of nitrogen-vacancy ensembles inC13-enriched diamond

We present an experimental and theoretical study of the optically detected magnetic resonance signals for ensembles of negatively charged nitrogen-vacancy (NV) centers in a $^{13}\mathrm{C}$ isotopically enriched single-crystal diamond. We observe four broad transition peaks with superimposed sharp features at zero magnetic field and study their dependence on an applied magnetic field. A theoretical model that reproduces all qualitative features of these spectra is developed. Understanding the magnetic-resonance spectra of NV centers in an isotopically enriched diamond is important for emerging applications in nuclear magnetic resonance.

Chapter 23. Singlet Order in Heteronuclear Spin Systems

The concept of heteronuclear Long-Lived spin States (LLSs) is introduced. In the simplest case of a pair of heteronuclei, such states are given by the singlet order of the spin pair, which can be efficiently sustained under Zero or Ultra-Low Field (ZULF) conditions. Here we describe two possible ways of detecting long-lived singlet order of heteronuclei: detection at ZULF conditions and NMR (Nuclear Magnetic Resonance) detection at high field utilising fast field-cycling. A theoretical description of the underlying spin dynamics is presented for both cases; the discussion is supported by experimental examples of LLSs in 13CH groups. The generality of these phenomena is discussed, as well as…

Fundaments of photoelectric readout of spin states in diamond

Abstract The chapter “Fundaments of photoelectric readout of spin states in diamond” deals with the detection of NV centre spins in diamond using the photoelectric detection of magnetic resonances (PDMR) method, introduced in a series of recent publications. It provides in particular insights into the physics of electronic transitions of the NV center, leading to the free carrier generation, and discusses methodologies how to implement the photocurrent detection principles in the dynamically evolving field of quantum technologies. Recent results on the single electron and the single nuclear spin qubits photoelectric readout are presented, along with a microwave-free NV magnetometry techniqu…

Zero-field magnetometry based on nitrogen-vacancy ensembles in diamond

Ensembles of nitrogen-vacancy (NV) centers in diamonds are widely utilized for magnetometry, magnetic-field imaging and magnetic-resonance detection. They have not been used for magnetometry at zero ambient field because Zeeman sublevels lose first-order sensitivity to magnetic fields as they are mixed due to crystal strain or electric fields. In this work, we realize a zero-field (ZF) magnetometer using polarization-selective microwave excitation in a 12C-enriched HPHT crystal sample. We employ circularly polarized microwaves to address specific transitions in the optically detected magnetic resonance and perform magnetometry with a noise floor of 250 pT/Hz^(1/2). This technique opens the …

Eddy current imaging with an atomic radio-frequency magnetometer

We use a radio-frequency $^{85}$Rb alkali-vapor cell magnetometer based on a paraffin-coated cell with long spin-coherence time and a small, low-inductance driving coil to create highly resolved conductivity maps of different objects. We resolve sub-mm features in conductive objects, we characterize the frequency response of our technique, and by operating at frequencies up to 250 kHz we are able to discriminate between differently conductive materials based on the induced response. The method is suited to cover a wide range of driving frequencies and can potentially be used for detecting non-metallic objects with low DC conductivity.

Proposal for a Cosmic Axion Spin Precession Experiment (CASPEr)

We propose an experiment to search for QCD axion and axionlike-particle dark matter. Nuclei that are interacting with the background axion dark matter acquire time-varying CP-odd nuclear moments such as an electric dipole moment. In analogy with nuclear magnetic resonance, these moments cause precession of nuclear spins in a material sample in the presence of an electric field. Precision magnetometry can be used to search for such precession. An initial phase of this experiment could cover many orders of magnitude in axionlike-particle parameter space beyond the current astrophysical and laboratory limits. And with established techniques, the proposed experimental scheme has sensitivity to …

Towards Large-Scale Steady-State Enhanced Nuclear Magnetization with In Situ Detection

Signal Amplification By Reversible Exchange (SABRE) boosts NMR signals of various nuclei enabling new applications spanning from magnetic resonance imaging to analytical chemistry and fundamental physics. SABRE is especially well positioned for continuous generation of enhanced magnetization on a large scale, however, several challenges need to be addressed for accomplishing this goal. Specifically, SABRE requires (i) a specialized catalyst capable of reversible H2 activation and (ii) physical transfer of the sample from the point of magnetization generation to the point of detection (e.g., a high-field or a benchtop NMR spectrometer). Moreover, (iii) continuous parahydrogen bubbling accele…

Search for Axionlike Dark Matter Using Solid-State Nuclear Magnetic Resonance.

Physical review letters 126(14), 141802 (2021). doi:10.1103/PhysRevLett.126.141802

Molecular parity nonconservation in nuclear spin couplings

The weak interaction does not conserve parity, which is apparent in many nuclear and atomic phenomena. However, thus far, parity nonconservation has not been observed in molecules. Here we consider nuclear-spin-dependent parity nonconserving contributions to the molecular Hamiltonian. These contributions give rise to a parity nonconserving indirect nuclear spin-spin coupling which can be distinguished from parity conserving interactions in molecules of appropriate symmetry, including diatomic molecules. We estimate the magnitude of the coupling, taking into account relativistic corrections. Finally, we propose and simulate an experiment to detect the parity nonconserving coupling using liqu…

Axion quark nuggets and how a global network can discover them

We advocate an idea that the presence of the daily and annual modulations of the axion flux on the Earth surface may dramatically change the strategy of the axion searches. Our computations are based on the so-called Axion Quark Nugget (AQN) dark matter model which was originally put forward to explain the similarity of the dark and visible cosmological matter densities $\Omega_{\rm dark}\sim \Omega_{\rm visible}$. In our framework, the population of galactic axions with mass $ 10^{-6} {\rm eV}\lesssim m_a\lesssim 10^{-3}{\rm eV}$ and velocity $\sim 10^{-3} c$ will be always accompanied by the axions with typical velocities $\sim 0.6 c$ emitted by AQNs. We formulate the broadband detection …

High magnetic fields for fundamental physics

Various fundamental-physics experiments such as measurement of the birefringence of the vacuum, searches for ultralight dark matter (e.g., axions), and precision spectroscopy of complex systems (including exotic atoms containing antimatter constituents) are enabled by high-field magnets. We give an overview of current and future experiments and discuss the state-of-the-art DC- and pulsed-magnet technologies and prospects for future developments.

Ferromagnetic gyroscopes for tests of fundamental physics

A ferromagnetic gyroscope (FG) is a ferromagnet whose angular momentum is dominated by electron spin polarization and that will precess under the action of an external torque, such as that due to a magnetic field. Here we model and analyze FG dynamics and sensitivity, focusing on practical schemes for experimental realization. In the case of a freely floating FG, we model the transition from dynamics dominated by libration in relatively high externally applied magnetic fields, to those dominated by precession at relatively low applied fields. Measurement of the libration frequency enables in situ measurement of the magnetic field and a technique to reduce the field below the threshold for w…

Quantum sensitivity limits of nuclear magnetic resonance experiments searching for new fundamental physics

Nuclear magnetic resonance is a promising experimental approach to search for ultra-light axion-like dark matter. Searches such as the cosmic axion spin-precession experiments (CASPEr) are ultimately limited by quantum-mechanical noise sources, in particular, spin-projection noise. We discuss how such fundamental limits can potentially be reached. We consider a circuit model of a magnetic resonance experiment and quantify three noise sources: spin-projection noise, thermal noise, and amplifier noise. Calculation of the total noise spectrum takes into account the modification of the circuit impedance by the presence of nuclear spins, as well as the circuit back-action on the spin ensemble. S…

Light-induced polarization effects in atoms with partially resolved hyperfine structure and applications to absorption, fluorescence, and nonlinear magneto-optical rotation

The creation and detection of atomic polarization is examined theoretically, through the study of basic optical-pumping mechanisms and absorption and fluorescence measurements, and the dependence of these processes on the size of ground- and excited-state hyperfine splittings is determined. The consequences of this dependence are studied in more detail for the case of nonlinear magneto-optical rotation in the Faraday geometry (an effect requiring the creation and detection of rank-two polarization in the ground state) with alkali atoms. Analytic formulas for the optical rotation signal under various experimental conditions are presented.

Real Time Nuclear Magnetic Resonance Detection of Fumarase Activity using Parahydrogen-Hyperpolarized [1-13C]fumarate

Hyperpolarized fumarate can be used as a probe of real-time metabolism in vivo, using carbon-13 magnetic resonance imaging. Dissolution dynamic nuclear polarization is commonly used to produce hyperpolarized fumarate, but a cheaper and faster alternative is to produce hyperpolarized fumarate via PHIP (parahydrogen induced polarization). In this work we trans-hydrogenate [1-13C]acetylene dicarboxylate with para-enriched hydrogen using a commercially available Ru catalyst in water to produce hyperpolarized [1-13C]fumarate. We show that fumarate is produced in 89% yield, with succinate as a side product in 11% yield. The proton polarization is converted into 13C magnetization using a constant …

Optimizing a Dynamical Decoupling Protocol for Solid-State Electronic Spin Ensembles in Diamond

We demonstrate significant improvements of the spin coherence time of a dense ensemble of nitrogen-vacancy (NV) centers in diamond through optimized dynamical decoupling (DD). Cooling the sample down to 77 K suppresses longitudinal spin relaxation ${T}_{1}$ effects and DD microwave pulses are used to increase the transverse coherence time ${T}_{2}$ from $\ensuremath{\sim}0.7\phantom{\rule{0.28em}{0ex}}\mathrm{ms}$ up to $\ensuremath{\sim}30\phantom{\rule{0.28em}{0ex}}\mathrm{ms}$. We extend previous work of single-axis (Carr-Purcell-Meiboom-Gill) DD towards the preservation of arbitrary spin states. Following a theoretical and experimental characterization of pulse and detuning errors, we c…

Constraints on bosonic dark matter from ultralow-field nuclear magnetic resonance

The nature of dark matter, the invisible substance making up over $80\%$ of the matter in the Universe, is one of the most fundamental mysteries of modern physics. Ultralight bosons such as axions, axion-like particles or dark photons could make up most of the dark matter. Couplings between such bosons and nuclear spins may enable their direct detection via nuclear magnetic resonance (NMR) spectroscopy: as nuclear spins move through the galactic dark-matter halo, they couple to dark-matter and behave as if they were in an oscillating magnetic field, generating a dark-matter-driven NMR signal. As part of the Cosmic Axion Spin Precession Experiment (CASPEr), an NMR-based dark-matter search, w…

Eddy-Current Imaging with Nitrogen-Vacancy Centers in Diamond

We demonstrate microwave-free eddy-current imaging using nitrogen-vacancy centers in diamond. By detecting the eddy-current induced magnetic field of conductive samples, we can distinguish between different materials and shapes and identify structural defects. Our technique allows for the discrimination of different materials according to their conductivity. The sensitivity of the measurements is calculated as 8$\times 10 ^{5}$\,S/m\,$\sqrt[]{\textrm{Hz}}$ at 3.5\,MHz, for a cylindrical sample with radius $r_0$\,=\,1\,mm and height $h$\,=\,0.1\,mm (volume $\sim$\,0.3\,mm$^3$), at a distance of 0.5\,mm. In comparison with existing technologies, the diamond-based device exhibits a superior ba…

Sensitive magnetometry in challenging environments

State-of-the-art magnetic field measurements performed in shielded environments under carefully controlled conditions rarely reflect the realities of those applications envisioned in the introductions of peer-reviewed publications. Nevertheless, significant advances in magnetometer sensitivity have been accompanied by serious attempts to bring these magnetometers into the challenging working environments in which they are often required. This review discusses the ways in which various (predominantly optically pumped) magnetometer technologies have been adapted for use in a wide range of noisy and physically demanding environments.

The Revised SI: Fundamental Constants, Basic Physics and Units

Comparison between observation and simulation of sodium LGS return flux with a 20W CW laser on Tenerife

We report on the comparison between observations and simulations of a completed 12-month field observation campaign at Observatorio del Teide, Tenerife, using ESO's transportable 20 watt CW Wendelstein laser guide star system. This mission has provided sodium photon return flux measurements of unprecedented detail regarding variation of laser power, polarization and sodium D2b repumping. The Raman fiber laser and projector technology are very similar to that employed in the 4LGSF/AOF laser facility, recently installed and commissioned at the VLT in Paranal. The simulations are based on the open source LGSBloch density matrix simulation package and we find good overall agreement with experim…

New Atomic Methods for Dark Matter Detection

We calculate the parity and time-reversal violating effects that are induced in atoms, nuclei, and molecules by their interaction with various background cosmic fields, such as axion dark matter or dark energy.

Optical polarization of nuclear ensembles in diamond

We report polarization of a dense nuclear-spin ensemble in diamond and its dependence on magnetic field and temperature. The polarization method is based on the transfer of electron spin polarization of negatively charged nitrogen vacancy color centers to the nuclear spins via the excited-state level anti-crossing of the center. We polarize 90% of the 14N nuclear spins within the NV centers, and 70% of the proximal 13C nuclear spins with hyperfine interaction strength of 13-14 MHz. Magnetic-field dependence of the polarization reveals sharp decrease in polarization at specific field values corresponding to cross-relaxation with substitutional nitrogen centers, while temperature dependence o…

Zero-Field J-spectroscopy of Quadrupolar Nuclei

Zero- to ultralow-field (ZULF) nuclear magnetic resonance (NMR) is a version of NMR that allows studying molecules and their transformations in the regime dominated by intrinsic spin-spin interactions. While spin dynamics at zero magnetic field can be probed indirectly, J-spectra can also be measured at zero field by using non-inductive sensors, for example, optically-pumped magnetometers (OPMs). A J-spectrum can be detected when a molecule contains at least two different types of magnetic nuclei (i.e., nuclei with different gyromagnetic ratios) that are coupled via J-coupling. Up to date, no pure J-spectra of molecules featuring the coupling to quadrupolar nuclei were reported. Here we sho…

Dark matter searches using accelerometer-based networks

Quantum science and technology 6(3), 034004 (2021). doi:10.1088/2058-9565/abef4f

Dynamics of a Ferromagnetic Particle Levitated Over a Superconductor

Under conditions where the angular momentum of a ferromagnetic particle is dominated by intrinsic spin, applied torque is predicted to cause gyroscopic precession of the particle. If the particle is sufficiently isolated from the environment, a measurement of spin precession can potentially yield sensitivity to torque beyond the standard quantum limit. Levitation of a micron-scale ferromagnetic particle above a superconductor is a possible method of near frictionless suspension enabling observation of ferromagnetic particle precession and ultrasensitive torque measurements. We experimentally investigate the dynamics of a micron-scale ferromagnetic particle levitated above a superconducting …

Coherent population oscillations with nitrogen-vacancy color centers in diamond

We present results of our research on two-field (two-frequency) microwave spectroscopy in nitrogen-vacancy (NV-) color centers in a diamond. Both fields are tuned to transitions between the spin sublevels of the NV- ensemble in the 3A2 ground state (one field has a fixed frequency while the second one is scanned). Particular attention is focused on the case where two microwaves fields drive the same transition between two NV- ground state sublevels (ms=0 -&gt; ms=+1). In this case, the observed spectra exhibit a complex narrow structure composed of three Lorentzian resonances positioned at the pump-field frequency. The resonance widths and amplitudes depend on the lifetimes of the levels in…

Lineshape-asymmetry elimination in weak atomic transitions driven by an intense standing wave field

Owing to the ac-Stark effect, the lineshape of a weak optical transition in an atomic beam can become significantly distorted, when driven by an intense standing wave field. We use an Yb atomic beam to study the lineshape of the 6s2 1S0 -&gt; 5d6s 3D1 transition, which is excited with light circulating in a Fabry-Perot resonator. We demonstrate two methods to avoid the distortion of the transition profile. Of these, one relies on the operation of the resonator in multiple longitudinal modes, and the other in multiple transverse modes.

Temperature- and Magnetic-Field-Dependent Longitudinal Spin Relaxation in Nitrogen-Vacancy Ensembles in Diamond

We present an experimental study of the longitudinal electron-spin relaxation time (T1) of negatively charged nitrogen-vacancy (NV) ensembles in diamond. T1 was studied as a function of temperature from 5 to 475 K and magnetic field from 0 to 630 G for several samples with various NV and nitrogen concentrations. Our studies reveal three processes responsible for T1 relaxation. Above room temperature, a two-phonon Raman process dominates, and below, we observe an Orbach-type process with an activation energy, 73(4) meV, which closely matches the local vibrational modes of the NV center. At yet lower temperatures, sample dependent cross relaxation processes dominate, resulting in temperature …

Microwave-free magnetometry with nitrogen-vacancy centers in diamond

We use magnetic-field-dependent features in the photoluminescence of negatively charged nitrogen-vacancy centers to measure magnetic fields without the use of microwaves. In particular, we present a magnetometer based on the level anti-crossing in the triplet ground state at 102.4 mT with a demonstrated noise floor of 6 nT/$\sqrt{\text{Hz}}$, limited by the intensity noise of the laser and the performance of the background-field power supply. The technique presented here can be useful in applications where the sensor is placed closed to conductive materials, e.g. magnetic induction tomography or magnetic field mapping, and in remote-sensing applications since principally no electrical acces…

Battery characterization via eddy-current imaging with nitrogen-vacancy centers in diamond

Sensitive and accurate diagnostic technologies with magnetic sensors are of great importance for identifying and localizing defects of rechargeable solid batteries in a noninvasive detection. We demonstrate a microwave-free AC magnetometry method with negatively charged NV centers in diamond based on a cross-relaxation feature between NV centers and individual substitutional nitrogen (P1) centers occurring at 51.2 mT. We apply the technique to non-destructive solid-state battery imaging. By detecting the eddy-current-induced magnetic field of the battery, we distinguish a defect on the external electrode and identify structural anomalies within the battery body. The achieved spatial resolut…

Prospects of SPIN Gyroscopes Based on Nitrogen-Vacancy Centers in Diamond

This project aims to develop solid-state gyroscopes based on ensembles of negatively charged nitrogen-vacancy (NV) centers in diamond [1], [2]. The NV center is a defect formed in diamond by one substitutional nitrogen atom and an adjacent vacancy. The NV- center features a ground state with electronic spin $\mathrm{S}=1$ , which can be initialized, manipulated, and detected via convenient optical, microwave and radiofrequency transitions (Fig. 1). Nuclear spins are appealing in the context of gyroscopes because they have much smaller gyromagnetic ratios than that of the electron (by a factor of about 1000), reducing the requirements on static magnetic-field stability and homogeneity. The l…

Solution nuclear magnetic resonance spectroscopy on a nanostructured diamond chip

We demonstrate nuclear magnetic resonance (NMR) spectroscopy of picoliter-volume solutions with a nanostructured diamond chip. Using optical interferometric lithography, diamond surfaces were nanostructured with dense, high-aspect-ratio nanogratings, enhancing the surface area by more than a factor of 15 over mm^2 regions of the chip. The nanograting sidewalls were doped with nitrogen-vacancy (NV) centers so that more than 10 million NV centers in a (25 micrometer)^2 laser spot are located close enough to the diamond surface (5 nm) to detect the NMR spectrum of 1 pL of fluid lying within adjacent nanograting grooves. The platform was used to perform 1H and 19F NMR spectroscopy at room tempe…

Dichroic atomic vapor laser lock with multi-gigahertz stabilization range

A dichroic atomic vapor laser lock (DAVLL) system exploiting buffer-gas-filled millimeter-scale vapor cells is presented. This system offers similar stability as achievable with conventional DAVLL system using bulk vapor cells, but has several important advantages. In addition to its compactness, it may provide continuous stabilization in a multi-gigahertz range around the optical transition. This range may be controlled either by changing the temperature of the vapor or by application of a buffer gas under an appropriate pressure. In particular, we experimentally demonstrate the ability of the system to lock the laser frequency between two hyperfine components of the $^{85}$Rb ground state…

A Hypothetical Effect of the Maxwell–Proca Electromagnetic Stresses on Galaxy Rotation Curves

Maxwell–Proca electrodynamics corresponding to finite photon mass causes a substantial change in the Maxwell stress tensor, and under certain circumstances, may cause electromagnetic stresses to act effectively as "negative pressure." This paper describes a model where this negative pressure imitates gravitational pull and may produce forces comparable to gravity and may even become dominant. The effect is associated with random magnetic fields with correlation lengths exceeding the photon Compton wavelength. The stresses act predominantly on the interstellar gas and cause an additional force pulling the gas toward the center and toward the galactic plane. Stars do not experience any signif…

Correlation of high-field and zero- to ultralow-field NMR properties using 2D spectroscopy

The field of zero- to ultralow-field (ZULF) nuclear magnetic resonance (NMR) is currently experiencing a rapid growth, owing to the progress in optical magnetometry, and also attractive features of ZULF NMR, such as low hardware cost and excellent spectral resolution achieved under ZULF conditions. In this work, an approach is proposed and demonstrated for simultaneous acquisition of ZULF-NMR spectra of individual 13C-containing isotopomers of chemical compounds in a complex mixture. The method makes use of fast field cycling, so that the spin evolution takes place at ZULF conditions, whereas signal detection is performed in a high-field NMR spectrometer. This method has excellent sensitivi…

Characterization of high-temperature performance of cesium vapor cells with anti-relaxation coating

© 2017 Author(s). Vapor cells with antirelaxation coating are widely used in modern atomic physics experiments due to the coating's ability to maintain the atoms' spin polarization during wall collisions. We characterize the performance of vapor cells with different coating materials by measuring longitudinal spin relaxation and vapor density at temperatures up to 95 °C. We infer that the spin-projection-noise-limited sensitivity for atomic magnetometers with such cells improves with temperature, which demonstrates the potential of antirelaxation coated cells in applications of future high-sensitivity magnetometers.

Polarization-driven spin precession of mesospheric sodium atoms: publisher's note.

This publisher's note corrects an error in the author listing of Opt. Lett.43, 5825 (2018)OPLEDP0146-959210.1364/OL.43.005825.

Nuclear-spin comagnetometer based on a liquid of identical molecules

Atomic comagnetometers are used in searches for anomalous spin-dependent interactions. Magnetic field gradients are one of the major sources of systematic errors in such experiments. Here we describe a comagnetometer based on the nuclear spins within an ensemble of identical molecules. The dependence of the measured spin-precession frequency ratio on the first-order magnetic field gradient is suppressed by over an order of magnitude compared to a comagnetometer based on overlapping ensembles of different molecules. Our single-species comagnetometer is shown to be capable of measuring the hypothetical spin-dependent gravitational energy of nuclei at the $10^{-17}$ eV level, comparable to the…

Spectral signatures of axionlike dark matter

We derive spectral line shapes of the expected signal for a haloscope experiment searching for axionlike dark matter. The knowledge of these line shapes is needed to optimize an experimental design and data analysis procedure. We extend the previously known results for the axion-photon and axion-gluon couplings to the case of gradient (axion-fermion) coupling. A unique feature of the gradient interaction is its dependence not only on magnitudes but also on directions of velocities of galactic halo particles, which leads to the directional sensitivity of the corresponding haloscope. We also discuss the daily and annual modulations of the gradient signal caused by the Earth's rotational and o…

Rubidium dimers in paraffin-coated cells

Measurements were made to determine the density of rubidium dimer vapor in paraffin-coated cells. The number density of dimers and atoms in similar paraffin-coated and uncoated cells was measured by optical spectroscopy. Due to the relatively low melting point of paraffin, a limited temperature range of 43-80 deg C was explored, with the lower end corresponding to a dimer density of less than 10^7 cm^(-3). With one-minute integration time, a sensitivity to dimer number density of better than 10^6 cm^(-3) was achieved. No significant difference in dimer density was observed between the cells.

Can a quantum nondemolition measurement improve the sensitivity of an atomic magnetometer?

Noise properties of an idealized atomic magnetometer that utilizes spin squeezing induced by a continuous quantum nondemolition measurement are considered. Such a magnetometer measures spin precession of $N$ atomic spins by detecting optical rotation of far-detuned light. Fundamental noise sources include the quantum projection noise and the photon shot-noise. For measurement times much shorter than the spin-relaxation time observed in the absence of light ($\tau_{\rm rel}$) divided by $\sqrt{N}$, the optimal sensitivity of the magnetometer scales as $N^{-3/4}$, so an advantage over the usual sensitivity scaling as $N^{-1/2}$ can be achieved. However, at longer measurement times, the optimi…

Miniature Cavity-Enhanced Diamond Magnetometer

We present a highly sensitive miniaturized cavity-enhanced room-temperature magnetic-field sensor based on nitrogen-vacancy (NV) centers in diamond. The magnetic resonance signal is detected by probing absorption on the 1042\,nm spin-singlet transition. To improve the absorptive signal the diamond is placed in an optical resonator. The device has a magnetic-field sensitivity of 28 pT/$\sqrt{\rm{Hz}}$, a projected photon shot-noise-limited sensitivity of 22 pT/$\sqrt{\rm{Hz}}$ and an estimated quantum projection-noise-limited sensitivity of 0.43 pT/$\sqrt{\rm{Hz}}$ with the sensing volume of $\sim$ 390 $\mu$m $\times$ 4500 $\mu$m$^{2}$. The presented miniaturized device is the basis for an e…

Probing fast oscillating scalar dark matter with atoms and molecules

Light scalar Dark Matter with scalar couplings to matter is expected within several scenarios to induce variations in the fundamental constants of nature. Such variations can be searched for, among other ways, via atomic spectroscopy. Sensitive atomic observables arise primarily due to possible changes in the fine-structure constant or the electron mass. Most of the searches to date have focused on slow variations of the constants (i.e. modulation frequencies $<$ 1 Hz). In a recent experiment \mbox{[Phys. Rev. Lett. 123, 141102 (2019)]} called WReSL (Weekend Relaxion-Search Laboratory), we reported on a direct search for rapid variations in the radio-frequency band. Such a search is particu…

Continuous-wave cavity ring-down polarimetry

We present a new cavity-based polarimetric scheme for highly sensitive and time-resolved measurements of birefringence and dichroism, linear and circular, that employs rapidly pulsed single-frequency continuous wave (CW) laser sources and extends current cavity-based spectropolarimetric techniques. We demonstrate how the use of a CW laser source allows for gains in spectral resolution, signal intensity, and data acquisition rate compared to traditional pulsed-based cavity ring-down polarimetry (CRDP). We discuss a particular CW-CRDP modality that is different from intensity-based cavity-enhanced polarimetric schemes as it relies on the determination of the polarization rotation frequency du…

Constant-adiabaticity ultralow magnetic field manipulations of parahydrogen-induced polarization: application to an AA'X spin system

The field of magnetic resonance imaging with hyperpolarized contrast agents is rapidly expanding, and parahydrogen-induced polarization (PHIP) is emerging as an inexpensive and easy-to-implement method for generating the required hyperpolarized biomolecules. Hydrogenative PHIP delivers hyperpolarized proton spin order to a substrate via chemical addition of H2 in the spin-singlet state, but it is typically necessary to transfer the proton polarization to a heteronucleus (usually 13C) which has a longer spin lifetime. Adiabatic ultralow magnetic field manipulations can be used to induce the polarization transfer, but this is necessarily a slow process, which is undesirable since the spins co…

Zero- to Ultralow-Field Nuclear Magnetic Resonance $J$-Spectroscopy with Commercial Atomic Magnetometers

Zero- to ultralow-field nuclear magnetic resonance (ZULF NMR) is an alternative spectroscopic method to high-field NMR, in which samples are studied in the absence of a large magnetic field. Unfortunately, there is a large barrier to entry for many groups, because operating the optical magnetometers needed for signal detection requires some expertise in atomic physics and optics. Commercially available magnetometers offer a solution to this problem. Here we describe a simple ZULF NMR configuration employing commercial magnetometers, and demonstrate sufficient functionality to measure samples with nuclear spins prepolarized in a permanent magnet or initialized using parahydrogen. This opens …

Stand-Off Magnetometry with Directional Emission from Sodium Vapors

International audience; Stand-off magnetometry allows measuring magnetic field at a distance, and can be employed in geophysical research, hazardous environment monitoring, and security applications. Stand-off magnetometry based on resonant scattering from atoms or molecules is often limited by the scarce amounts of detected light. The situation would be dramatically improved if the light emitted by excited atoms were to propagate towards the excitation light source in a directional manner. Here, we demonstrate that this is possible by means of mirrorless lasing. In a tabletop experiment, we detect free-precession signals of ground-state sodium spins under the influence of an external magne…

Optical quenching and recovery of photoconductivity in single-crystal diamond

We study the photocurrent induced by pulsed-light illumination (pulse duration is several nanoseconds) of single-crystal diamond containing nitrogen impurities. Application of additional continuous-wave light of the same wavelength quenches pulsed photocurrent. Characterization of the optically quenched photocurrent and its recovery is important for the development of diamond based electronics and sensing. (C) 2017 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license. This work was supported by AFOSR and the DARPA QuASAR program, by NSF Grant No. ECCS-1202258, and by DFG through the DIP program (FO 703/2-1).

Level anti-crossing magnetometry with color centers in diamond

Recent developments in magnetic field sensing with negatively charged nitrogen-vacancy centers (NV) in diamond employ magnetic-field (MF) dependent features in the photoluminescence (PL) and eliminate the need for microwaves (MW). Here, we study two approaches towards improving the magnetometric sensitivity using the ground-state level anti-crossing (GSLAC) feature of the NV center at a background MF of 102.4\,mT. Following the first approach, we investigate the feature parameters for precise alignment in a dilute diamond sample; the second approach extends the sensing protocol into absorption via detection of the GSLAC in the diamond transmission of a 1042\,nm laser beam. This leads to an …

Efficient polarization of high-angular-momentum systems

We propose methods of optical pumping that are applicable to open, high-angular-momentum transitions in atoms and molecules, for which conventional optical pumping would lead to significant population loss. Instead of applying circularly polarized cw light, as in conventional optical pumping, we propose to use techniques for coherent population transfer (e.g., adiabatic fast passage) to arrange the atoms so as to increase the entropy removed from the system with each spontaneous decay from the upper state. This minimizes the number of spontaneous-emission events required to produce a stretched state, thus reducing the population loss due to decay to other states. To produce a stretched stat…

Investigation of antirelaxation wall coatings beyond melting temperatures

We investigate vapor cells with antirelaxation wall coatings by measuring their relaxation properties beyond the melting temperatures and compare with the melting behavior of the coating material as observed with differential scanning calorimetry.

Measurement of untruncated nuclear spin interactions via zero- to ultralow-field nuclear magnetic resonance

Zero- to ultra-low-field nuclear magnetic resonance (ZULF NMR) provides a new regime for the measurement of nuclear spin-spin interactions free from effects of large magnetic fields, such as truncation of terms that do not commute with the Zeeman Hamiltonian. One such interaction, the magnetic dipole-dipole coupling, is a valuable source of spatial information in NMR, though many terms are unobservable in high-field NMR, and the coupling averages to zero under isotropic molecular tumbling. Under partial alignment, this information is retained in the form of so-called residual dipolar couplings. We report zero- to ultra-low-field NMR measurements of residual dipolar couplings in acetonitrile…

Color centers in diamond as novel probes of superconductivity

Magnetic imaging using color centers in diamond through both scanning and wide-field methods offers a combination of unique capabilities for studying superconductivity, for example, enabling accurate vector magnetometry at high temperature or high pressure, with spatial resolution down to the nanometer scale. The paper briefly reviews various experimental modalities in this rapidly developing nascent field and provides an outlook towards possible future directions.

Surpassing the Energy Resolution Limit with Ferromagnetic Torque Sensors

We discuss the fundamental noise limitations of a ferromagnetic torque sensor based on a levitated magnet in the tipping regime. We evaluate the optimal magnetic field resolution taking into account the thermomechanical noise and the mechanical detection noise at the standard quantum limit (SQL). We find that the Energy Resolution Limit (ERL), pointed out in recent literature as a relevant benchmark for most classes of magnetometers, can be surpassed by many orders of magnitude. Moreover, similarly to the case of a ferromagnetic gyroscope, it is also possible to surpass the standard quantum limit for magnetometry with independent spins, arising from spin-projection noise. Our finding indica…

Heading-Error-Free Optical Atomic Magnetometry in the Earth-Field Range

Alkali-metal atomic magnetometry is widely used due to its high sensitivity and cryogen-free operation. However, when operating in geomagnetic field, it suffers from heading errors originating from nonlinear Zeeman (NLZ) splittings and magnetic resonance asymmetries, which lead to difficulties in mobile-platform measurements. We demonstrate an alignment based $^{87}$Rb magnetometer, which, with only a single magnetic resonance peak and well-separated hyperfine transition frequencies, is insensitive or even immune to NLZ-related heading errors. It is shown that the magnetometer can be implemented for practical measurements in the geomagnetic environments and the photon-shot-noise-limited sen…

Sensitive magnetometry reveals inhomogeneities in charge storage and weak transient internal currents in Li-ion cells

The ever-increasing demand for high-capacity rechargeable batteries highlights the need for sensitive and accurate diagnostic technology for determining the state of a cell, for identifying and localizing defects, and for sensing capacity loss mechanisms. Here, we leverage atomic magnetometry to map the weak induced magnetic fields around Li-ion battery cells in a magnetically shielded environment. The ability to rapidly measure cells nondestructively allows testing even commercial cells in their actual operating conditions, as a function of state of charge. These measurements provide maps of the magnetic susceptibility of the cell, which follow trends characteristic for the battery materia…

Nondestructive in-line sub-picomolar detection of magnetic nanoparticles in flowing complex fluids

AbstractOver the last decades, the use of magnetic nanoparticles in research and commercial applications has increased dramatically. However, direct detection of trace quantities remains a challenge in terms of equipment cost, operating conditions and data acquisition times, especially in flowing conditions within complex media. Here we present the in-line, non-destructive detection of magnetic nanoparticles using high performance atomic magnetometers at ambient conditions in flowing media. We achieve sub-picomolar sensitivities measuring ~30 nm ferromagnetic iron and cobalt nanoparticles that are suitable for biomedical and industrial applications, under flowing conditions in water and who…

Is light narrowing possible with dense-vapor paraffin coated cells for atomic magnetometers?

We investigated the operation of an all-optical rubidium-87 atomic magnetometer with amplitude-modulated light. To study the suppression of spin-exchange relaxation, three schemes of pumping were implemented with room-temperature and heated paraffin coated vacuum cells. Efficient pumping and accumulation of atoms in the F=2 ground state were obtained. However, the sought-for narrowing of the resonance lines has not been achieved. A theoretical analysis of the polarization degree is presented to illustrate the absence of light narrowing due to radiation trapping at high temperature.

Rapid hyperpolarization and purification of the metabolite fumarate in aqueous solution

Significance Magnetic resonance imaging is hindered by inherently low sensitivity, which limits the method for the most part to observing water molecules in the body. Hyperpolarized molecules exhibit strongly enhanced MRI signals which opens the door for imaging low-concentration species in vivo. Biomolecules can be hyperpolarized and injected into a patient allowing for metabolism to be tracked in real time, greatly expanding the information available to the radiologist. Parahydrogen-induced polarization (PHIP) is a hyperpolarization method renowned for its low cost and accessibility, but is generally limited by low polarization levels, modest molecular concentrations, and contamination by…

Zero- to Ultralow-Field NMR Spectroscopy of Small Biomolecules.

Nuclear magnetic resonance (NMR) spectroscopy is a well-established analytical technique used to study chemicals and their transformations. However, high-field NMR spectroscopy necessitates advanced infrastructure, and even cryogen-free benchtop NMR spectrometers cannot be readily assembled from commercially available components. We demonstrate construction of a portable zero-field NMR spectrometer employing a commercially available magnetometer and investigate its applications in analytical chemistry. In particular, J-spectra of small representative biomolecules [13C]-formic acid, [1-13C]-glycine, [2,3-13C]-fumarate, and [1-13C]-d-glucose were acquired, and an approach relying on the prese…

Rapid online solid-state battery diagnostics with optically pumped magnetometers

Applied Sciences 10(21), 7864 (2020). doi:10.3390/app10217864

System for control of polarization state of light and generation of light with continuously rotating linear polarization

We present a technique for generating light in an arbitrary polarization state. The technique is based on interference of two orthogonally polarized light beams, whose amplitudes and phases are controlled with a Mach-Zehnder inteferometer with acousto-optic modulators (AOMs) placed in each arm. We demonstrate that via control over amplitudes, phases, and frequencies of acoustic waves driving the AOMs, any polarization state can be synthesized. In particular, we demonstrate generation of linearly polarized light, whose polarization plane continuously rotates at a rate from 1 kHz to 1 MHz. Such light finds applications in science (e.g., investigations of Bloch-Siegert effect) and technology (…

Oscillating nuclear electric dipole moments inside atoms

Interaction with the axion dark matter (DM) field generates an oscillating nuclear electric dipole moment (EDM) with a frequency corresponding to the axion's Compton frequency. Within an atom, an oscillating EDM can drive electric dipole transitions in the electronic shell. In the absence of radiation, and if the axion frequency matches a dipole transition, it can promote the electron into the excited state. The excitation events can be detected, for example, via subsequent uorescence or photoionization. Here we calculate the rates of such transitions. For a single light atom and an axion Compton frequency resonant with a transition energy corresponding to 1 eV, the rate is on the order of …

Relaxion Stars and their detection via Atomic Physics

The cosmological relaxion can address the hierarchy problem, while its coherent oscillations can constitute dark matter in the present universe. We consider the possibility that the relaxion forms gravitationally bound objects that we denote as relaxion stars. The density of these stars would be higher than that of the local dark matter density, resulting in enhanced signals in table-top detectors, among others. Furthermore, we raise the possibility that these objects may be trapped by an external gravitational potential, such as that of the Earth or the Sun. This leads to formation of relaxion halos of even greater density. We discuss several interesting implications of relaxion halos, as …

Probing New Long-Range Interactions by Isotope Shift Spectroscopy

We explore a method to probe new long- and intermediate-range interactions using precision atomic isotope shift spectroscopy. We develop a formalism to interpret linear King plots as bounds on new physics with minimal theory inputs. We focus only on bounding the new physics contributions that can be calculated independently of the standard model nuclear effects. We apply our method to existing Ca[superscript +] data and project its sensitivity to conjectured new bosons with spin-independent couplings to the electron and the neutron using narrow transitions in other atoms and ions, specifically, Sr and Yb. Future measurements are expected to improve the relative precision by 5 orders of magn…

Constraining exotic interactions

Beyond-the-standard-model interactions mediated by an exchange of virtual "new" bosons result in a finite set of possible effective interaction potentials between standard-model particles such as electrons and nucleons. We discuss the classification of such potentials and briefly review recent experiments searching for such exotic interactions at spatial scales from sub-nanometers to tens of thousand kilometers.

A network of precision gravimeters as a detector of matter with feeble nongravitational coupling

Hidden matter that interacts only gravitationally would oscillate at characteristic frequencies when trapped inside of Earth. For small oscillations near the center of the Earth, these frequencies are around 300 $\mu$Hz. Additionally, signatures at higher harmonics would appear because of the non-uniformity of Earth's density. In this work, we use data from a global network of gravimeters of the International Geodynamics and Earth Tide Service (IGETS) to look for these hypothetical trapped objects. We find no evidence for such objects with masses on the order of 10$^{14}$ kg or greater with an oscillation amplitude of 0.1 $r_e$. It may be possible to improve the sensitivity of the search by…

Microwave-free vector magnetometry with nitrogen-vacancy centers along a single axis in diamond

Sensing vector magnetic fields is critical to many applications in fundamental physics, bioimaging, and material science. Magnetic-field sensors exploiting nitrogen-vacancy (NV) centers are particularly compelling as they offer high sensitivity and spatial resolution even at nanoscale. Achieving vector magnetometry has, however, often required applying microwaves sequentially or simultaneously, limiting the sensors' applications under cryogenic temperature. Here we propose and demonstrate a microwave-free vector magnetometer that simultaneously measures all Cartesian components of a magnetic field using NV ensembles in diamond. In particular, the present magnetometer leverages the level ant…

Noncovalent force spectroscopy using wide-field optical and diamond-based magnetic imaging

A realization of the force-induced remnant magnetization spectroscopy (FIRMS) technique of specific biomolecular binding is presented where detection is accomplished with wide-field optical and diamond-based magnetometry using an ensemble of nitrogen-vacancy (NV) color centers. The technique may be adapted for massively parallel screening of arrays of nanoscale samples.

Rapid parameter estimation of discrete decaying signals using autoencoder networks

Machine learning: science and technology 2(4), 045024 (2021). doi:10.1088/2632-2153/ac1eea

Extreme nuclear magnetic resonance: Zero field, single spins, dark matter….

An unusual regime for liquid-state nuclear magnetic resonance (NMR) where the magnetic field strength is so low that the $J$-coupling (intramolecular spin-spin) interactions dominate the spin Hamiltonian opens a new paradigm with applications in spectroscopy, quantum control, and in fundamental-physics experiments, including searches for well-motivated dark-matter candidates. An interesting possibility is to bring this kind of "extreme NMR" together with another one---single nuclear spin detected with a single-spin quantum sensor. This would enable single-molecule $J$-spectroscopy.

Nuclear magnetic resonance at millitesla fields using a zero-field spectrometer

We describe new analytical capabilities for nuclear magnetic resonance (NMR) experiments in which signal detection is performed with chemical resolution (via spin-spin J couplings) in the zero to ultra-low magnetic field region, below 1μT. Using magnetic fields in the 100μT to 1mT range, we demonstrate the implementation of conventional NMR pulse sequences with spin-species selectivity.

Towards large‐scale steady‐state enhanced nuclear magnetization with in situ detection

Magnetic resonance in chemistry 59(12), 1208 - 1215 (2021). doi:10.1002/mrc.5161

Experimental benchmarking of quantum control in zero-field nuclear magnetic resonance

Zero-field nuclear magnetic resonance (NMR) provides complementary analysis modalities to those of high-field NMR and allows for ultra-high-resolution spectroscopy and measurement of untruncated spin-spin interactions. Unlike for the high-field case, however, universal quantum control -- the ability to perform arbitrary unitary operations -- has not been experimentally demonstrated in zero-field NMR. This is because the Larmor frequency for all spins is identically zero at zero field, making it challenging to individually address different spin species. We realize a composite-pulse technique for arbitrary independent rotations of $^1$H and $^{13}$C spins in a two-spin system. Quantum-inform…

Evidence for degenerate mirrorless lasing in alkali metal vapor: forward beam magneto-optical experiment

We report an experimental observation of degenerate mirrorless lasing in forward direction under excitation of a dilute atomic Rb vapor with a single linearly polarized cw laser light resonant with cycling Fe &gt; Fg atomic D2 transitions. Light polarized orthogonally to the laser light is generated for the input light intensity exceeding a threshold value of about 3 mW/cm^2. Application of a transverse magnetic field directed along the input light polarization reveals a sharp about 20 mG wide magnetic resonance centered at B = 0. Increasing the incident light intensity from 3 to 300 mW/cm^2, the generated light undergoes rapid amplitude increase followed by a decline and resonance broadeni…

Search for axion-like dark matter with spin-based amplifiers

Ultralight axion-like particles (ALPs) are well-motivated dark matter candidates introduced by theories beyond the standard model. However, the constraints on the existence of ALPs through existing laboratory experiments are hindered by their current sensitivities, which are usually weaker than astrophysical limits. Here, we demonstrate a new quantum sensor to search for ALPs in the mass range that spans about two decades from 8.3 feV to 744 feV. Our sensor makes use of hyperpolarized long-lived nuclear spins as a pre-amplifier that effectively enhances coherently oscillating axion-like dark-matter field by a factor of &gt;100. Using spin-based amplifiers, we achieve an ultrahigh magnetic s…

Spiking dynamics of frequency up-converted field generated in continuous-wave excited rubidium vapours

We report on spiking dynamics of frequency up-converted emission at 420 nm generated on the 6P3/2-5S1/2 transition in Rb vapour two-photon excited to the 5D5/2 level with laser light at 780 and 776 nm. The spike duration is less than the natural lifetime of any excited level involved in the interaction with both continuous and pulsed pump radiation. The spikes at 420 nm are attributed to temporal properties of the directional emission at 5.23 {\mu}m generated on the population inverted 5D5/2-6P3/2 transition. A link between the spiking regime and cooperative effects is discussed. We suggest that the observed stochastic behaviour is due to the quantum-mechanical nature of the cooperative eff…

Atomic physics studies at the gamma factory at CERN

The Gamma Factory initiative proposes to develop novel research tools at CERN by producing, accelerating and storing highly relativistic, partially stripped ion beams in the SPS and LHC storage rings. By exciting the electronic degrees of freedom of the stored ions with lasers, high-energy narrow-band photon beams will be produced by properly collimating the secondary radiation that is peaked in the direction of ions' propagation. Their intensities, up to $10^{17}$ photons per second, will be several orders of magnitude higher than those of the presently operating light sources in the particularly interesting $\gamma$--ray energy domain reaching up to 400 MeV. This article reviews opportuni…

Electrical readout microwave-free sensing with diamond

While nitrogen-vacancy (NV-) centers have been extensively investigated in the context of spin-based quantum technologies, the spin-state readout is conventionally performed optically, which may limit miniaturization and scalability. Here, we report photoelectric readout of ground-state cross-relaxation features, which serves as a method for measuring electron spin resonance spectra of nanoscale electronic environments and also for microwave-free sensing. As a proof of concept, by systematically tuning NV centers into resonance with the target electronic system, we extracted the spectra for the P1 electronic spin bath in diamond. Such detection may enable probing optically inactive defects …

Cross-relaxation studies with optically detected magnetic resonances in nitrogen-vacancy centers in diamond in an external magnetic field

In this paper cross-relaxation between nitrogen-vacancy (NV) centers and substitutional nitrogen in a diamond crystal was studied. It was demonstrated that optically detected magnetic resonance signals (ODMR) can be used to measure these signals successfully. The ODMR were detected at axial magnetic field values around 51.2~mT in a diamond sample with a relatively high (200~ppm) nitrogen concentration. We observed transitions that involve magnetic sublevels that are split by the hyperfine interaction. Microwaves in the frequency ranges from 1.3 GHz to 1.6 GHz ($m_S=0\longrightarrow m_S=-1$ NV transitions) and from 4.1 to 4.6 GHz ($m_S=0\longrightarrow m_S=+1$ NV transitions) were used. To u…

Spin-lattice relaxation of individual solid-state spins

Understanding the effect of vibrations on the relaxation process of individual spins is crucial for implementing nanosystems for quantum information and quantum metrology applications. In this work, we present a theoretical microscopic model to describe the spin-lattice relaxation of individual electronic spins associated to negatively charged nitrogen-vacancy centers in diamond, although our results can be extended to other spin-boson systems. Starting from a general spin-lattice interaction Hamiltonian, we provide a detailed description and solution of the quantum master equation of an electronic spin-one system coupled to a phononic bath in thermal equilibrium. Special attention is given…

Sawtooth-wave adiabatic-passage slowing of dysprosium

We report on sawtooth wave adiabatic passage (SWAP) slowing of bosonic and fermionic dysprosium isotopes by using a 136 kHz wide transition at 626 nm. A beam of precooled atoms is further decelerated in one dimension by the SWAP force and the amount of atoms at near zero velocity is measured. We demonstrate that the SWAP slowing can be twice as fast as in a conventional optical molasses operated on the same transition. In addition, we investigate the parameter range for which the SWAP force is efficiently usable in our set-up, and relate the results to the adiabaticity condition. Furthermore, we add losses to the hyperfine ground-state population of fermionic dysprosium during deceleration …

Search for exotic spin-dependent interactions with a spin-based amplifier

Description

Searching for axion stars and $Q$-balls with a terrestrial magnetometer network

Light (pseudo-)scalar fields are promising candidates to be the dark matter in the Universe. Under certain initial conditions in the early Universe and/or with certain types of self-interactions, they can form compact dark-matter objects such as axion stars or Q-balls. Direct encounters with such objects can be searched for by using a global network of atomic magnetometers. It is shown that for a range of masses and radii not ruled out by existing observations, the terrestrial encounter rate with axion stars or Q-balls can be sufficiently high (at least once per year) for a detection. Furthermore, it is shown that a global network of atomic magnetometers is sufficiently sensitive to pseudos…

Zero-field nuclear magnetic resonance spectroscopy of viscous liquids

Abstract We report zero-field NMR measurements of a viscous organic liquid, ethylene glycol. Zero-field spectra were taken showing resolved scalar spin–spin coupling (J-coupling) for ethylene glycol at different temperatures and water contents. Molecular dynamics strongly affects the resonance linewidth, which closely follows viscosity. Quantum chemical calculations have been used to obtain the relative stability and coupling constants of all ethylene glycol conformers. The results show the potential of zero-field NMR as a probe of molecular structure and dynamics in a wide range of environments, including viscous fluids.

Millicharged dark matter detection with ion traps

We propose the use of trapped ions for detection of millicharged dark matter. Millicharged particles will scatter off the ions, giving a signal either in individual events or in the overall heating rate of the ions. Ion traps have several properties which make them ideal detectors for such a signal. First, ion traps have demonstrated significant isolation of the ions from the environment, greatly reducing the background heating and event rates. Second, ion traps can have low thresholds for detection of energy deposition, down to $\sim \text{neV}$. Third, since the ions are charged, they naturally have large cross sections for scattering with the millicharged particles, further enhanced by t…

Zero-field nuclear magnetic resonance of chemically exchanging systems.

Zero- to ultralow-field (ZULF) nuclear magnetic resonance (NMR) is an emerging tool for precision chemical analysis. In this work, we study dynamic processes and investigate the influence of chemical exchange on ZULF NMR J-spectra. We develop a computational approach that allows quantitative calculation of J-spectra in the presence of chemical exchange and apply it to study aqueous solutions of [15N]ammonium (15N\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${\mathrm{H}}_4^ +$$\end{document}H4+) as a model syst…

Deep neural networks to recover unknown physical parameters from oscillating time series.

PLOS ONE 17(5), e0268439 (2022). doi:10.1371/journal.pone.0268439

Demonstration of diamond nuclear spin gyroscope

Description

Raman and nuclear magnetic resonance investigation of alkali metal vapor interaction with alkene-based anti-relaxation coating.

The use of anti-relaxation coatings in alkali vapor cells yields substantial performance improvements by reducing the probability of spin relaxation in wall collisions by several orders of magnitude. Some of the most effective anti-relaxation coating materials are alpha-olefins, which (as in the case of more traditional paraffin coatings) must undergo a curing period after cell manufacturing in order to achieve the desired behavior. Until now, however, it has been unclear what physicochemical processes occur during cell curing, and how they may affect relevant cell properties. We present the results of nondestructive Raman-spectroscopy and magnetic-resonance investigations of the influence …

On the Possibility of Miniature Diamond-Based Magnetometers Using Waveguide Geometries

Micromachines 9(6), 276 (2018). doi:10.3390/mi9060276

Scalar Dark Matter in the Radio-Frequency Band: Atomic-Spectroscopy Search Results

Among the prominent candidates for dark matter are bosonic fields with small scalar couplings to the Standard-Model particles. Several techniques are employed to search for such couplings and the current best constraints are derived from tests of gravity or atomic probes. In experiments employing atoms, observables would arise from expected dark-matter-induced oscillations in the fundamental constants of nature. These studies are primarily sensitive to underlying particle masses below $10^{-14}$ eV. We present a method to search for fast oscillations of fundamental constants using atomic spectroscopy in cesium vapor. We demonstrate sensitivity to scalar interactions of dark matter associate…

Infrared laser magnetometry with a NV doped diamond intracavity etalon

We propose an hybrid laser system consisting of a semiconductor external cavity laser associated to an intra-cavity diamond etalon doped with nitrogen-vacancy color centers. We consider laser emission tuned to the infrared absorption line that is enhanced under the magnetic field dependent nitrogen-vacancy electron spin resonance and show that this architecture leads to a compact solid-state magnetometer that can be operated at room-temperature. The sensitivity to the magnetic field limited by the photon shot-noise of the output laser beam is estimated to be around $250~\mathrm{fT/\sqrt{Hz}}$. Unlike usual NV center infrared magnetometry, this method would not require an external frequency …

Emergent hydrodynamics in a strongly interacting dipolar spin ensemble.

Conventional wisdom holds that macroscopic classical phenomena naturally emerge from microscopic quantum laws. However, despite this mantra, building direct connections between these two descriptions has remained an enduring scientific challenge. In particular, it is difficult to quantitatively predict the emergent "classical" properties of a system (e.g. diffusivity, viscosity, compressibility) from a generic microscopic quantum Hamiltonian. Here, we introduce a hybrid solid-state spin platform, where the underlying disordered, dipolar quantum Hamiltonian gives rise to the emergence of unconventional spin diffusion at nanometer length scales. In particular, the combination of positional di…

Search for topological defect dark matter with a global network of optical magnetometers

Ultralight bosons such as axion-like particles are viable candidates for dark matter. They can form stable, macroscopic field configurations in the form of topological defects that could concentrate the dark matter density into many distinct, compact spatial regions that are small compared with the Galaxy but much larger than the Earth. Here we report the results of the search for transient signals from the domain walls of axion-like particles by using the global network of optical magnetometers for exotic (GNOME) physics searches. We search the data, consisting of correlated measurements from optical atomic magnetometers located in laboratories all over the world, for patterns of signals p…

Wide-Field Imaging of Superconductor Vortices with Electron Spins in Diamond

Understanding the mechanisms behind high-$T_{c}$ Type-II superconductors (SC) is still an open task in condensed matter physics. One way to gain further insight into the microscopic mechanisms leading to superconductivity is to study the magnetic properties of the SC in detail, for example by studying the properties of vortices and their dynamics. In this work we describe a new method of wide-field imaging magnetometry using nitrogen-vacancy (NV) centers in diamond to image vortices in an yttrium barium copper oxide (YBCO) thin film. We demonstrate quantitative determination of the magnetic field strength of the vortex stray field, the observation of vortex patterns for different cooling fi…

Alkali-vapor magnetic resonance driven by fictitious radiofrequency fields

We demonstrate an all-optical 133Cs scalar magnetometer, operating in nonzero magnetic field, in which the magnetic resonance is driven by an effective oscillating magnetic field provided by the AC Stark shift of an intensity-modulated laser beam. We achieve a projected shot-noise-limited sensitivity of 1.7fT/Hz and measure a technical noise floor of 40fT/Hz. These results are essentially identical to a coil-driven scalar magnetometer using the same setup. This all-optical scheme offers advantages over traditional coil-driven magnetometers for use in arrays and in magnetically sensitive fundamental physics experiments, e.g., searches for a permanent electric dipole moment of the neutron.

Imaging Topological Spin Structures Using Light-Polarization and Magnetic Microscopy

We present an imaging modality that enables detection of magnetic moments and their resulting stray magnetic fields. We use wide-field magnetic imaging that employs a diamond-based magnetometer and has combined magneto-optic detection (e.g. magneto-optic Kerr effect) capabilities. We employ such an instrument to image magnetic (stripe) domains in multilayered ferromagnetic structures.

A method for measurement of spin-spin couplings with sub-mHz precision using zero- to ultralow-field nuclear magnetic resonance.

We present a method which allows for the extraction of physical quantities directly from zero- to ultralow-field nuclear magnetic resonance (ZULF NMR) data. A numerical density matrix evolution is used to simulate ZULF NMR spectra of several molecules in order to fit experimental data. The method is utilized to determine the indirect spin-spin couplings ($J$-couplings) in these, which is achieved with precision of $10^{-2}$--$10^{-4}$ Hz. The simulated and measured spectra are compared to earlier research. Agreement and precision improvement for most of the $J$-coupling estimates are achieved. The availability of an efficient, flexible fitting method for ZULF NMR enables a new generation of…

Pseudovector and pseudoscalar spin-dependent interactions in atoms

Hitherto unknown elementary particles can be searched for with atomic spectroscopy. We conduct such a search using a potential that results from the longitudinal polarization of a pseudovector particle. We show that such a potential, inversely proportional to the boson's mass squared, $V \propto 1/M^2$, can stay finite at $M \to 0$ if the theory is renormalizable. We also look for a pseudoscalar boson, which induces a contact spin-dependent potential that does not contribute to new forces searched for in experiments with macroscopic objects, but may be seen in atomic spectroscopy. We extract limits on the interaction constants of these potentials from the experimental spectra of antiprotoni…

Constraints on exotic spin-dependent interactions between electrons from helium fine-structure spectroscopy

Agreement between theoretical calculations of atomic structure and spectroscopic measurements is used to constrain possible contribution of exotic spin-dependent interactions between electrons to the energy differences between states in helium-4. In particular, constraints on dipole-dipole interactions associated with the exchange of pseudoscalar bosons (such as axions or axion-like particles) with masses ${10}^{\ensuremath{-}2}\ensuremath{\lesssim}m\ensuremath{\lesssim}{10}^{4}\mathrm{eV}$ are improved by a factor of $\ensuremath{\sim}100$. The first atomic-scale constraints on several exotic velocity-dependent dipole-dipole interactions are established as well.

Chemical Reaction Monitoring Using Zero-Field Nuclear Magnetic Resonance Enables Study of Heterogeneous Samples in Metal Containers

Abstract We demonstrate that heterogeneous/biphasic chemical reactions can be monitored with high spectroscopic resolution using zero‐field nuclear magnetic resonance spectroscopy. This is possible because magnetic susceptibility broadening is negligible at ultralow magnetic fields. We show the two‐step hydrogenation of dimethyl acetylenedicarboxylate with para‐enriched hydrogen gas in conventional glass NMR tubes, as well as in a titanium tube. The low frequency zero‐field NMR signals ensure that there is no significant signal attenuation arising from shielding by the electrically conductive sample container. This method paves the way for in situ monitoring of reactions in complex heteroge…

Intensity-correlated spiking of infrared and ultraviolet emission from sodium vapors

The directional spiking infrared and ultraviolet emission from sodium vapors excited to the 4D5/2 level by a continuous-wave resonant laser pump, that constitute a novel feature of the cooperative effects, has been analyzed. Cascade mirrorless lasing at 2207 and 2338 nm on population-inverted transitions and ultraviolet radiation at 330 nm that is generated due to four-wave mixing process demonstrate a high degree of intensity correlation.

Photoluminescence at the ground state level anticrossing of the nitrogen-vacancy center in diamond

The nitrogen-vacancy center (NV center) in diamond at magnetic fields corresponding to the ground state level anticrossing (GSLAC) region gives rise to rich photoluminescence (PL) signals due to the vanishing energy gap between the electron spin states, which enables to have an effect on the NV center's luminescence for a broad variety of environmental couplings. In this article we report on the GSLAC photoluminescence signature of NV ensembles in different spin environments at various external fields. We investigate the effects of transverse electric and magnetic fields, P1 centers, NV centers, and the $^{13}$C nuclear spins, each of which gives rise to a unique PL signature at the GSLAC. …

Dynamic effects in nonlinear magneto-optics of atoms and molecules: review

A brief review is given of topics relating to dynamical processes arising in nonlinear interactions between light and resonant systems (atoms or molecules) in the presence of a magnetic field.

Improved Bounds on Ultralight Scalar Dark Matter in the Radio-Frequency Range

We present a search for fundamental constant oscillations in the range $20$~kHz-$100$ MHz, that may arise within models for ultralight dark matter (UDM). Using two independent, significantly upgraded optical-spectroscopy apparatus, we achieve up to $\times$1000 greater sensitivity in the search relative to previous work. We report no observation of UDM and thus constrain respective couplings to electrons and photons within the investigated UDM particle mass range $8\cdot 10^{-11}-4\cdot 10^{-7}$ eV. The constraints significantly exceed previously set bounds, and as we show, may surpass in future experiments those provided by equivalence-principle experiments in a specific case regarding the…

Data File 1.csv

This table contains information regarding maximal observed power, divergence and linewidth for the observed mirrorless lasing components