0000000000115521
AUTHOR
Andrey Jarmola
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…
Diamond magnetometer enhanced by ferrite flux concentrators
Magnetometers based on nitrogen-vacancy (NV) centers in diamond are promising room-temperature, solid-state sensors. However, their reported sensitivity to magnetic fields at low frequencies (<1 kHz) is presently >10 pT s^{1/2}, precluding potential applications in medical imaging, geoscience, and navigation. Here we show that high-permeability magnetic flux concentrators, which collect magnetic flux from a larger area and concentrate it into the diamond sensor, can be used to improve the sensitivity of diamond magnetometers. By inserting an NV-doped diamond membrane between two ferrite cones in a bowtie configuration, we realize a ~250-fold increase of the magnetic field amplitude wi…
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…
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…
Diamond Magnetic Microscopy of Malarial Hemozoin Nanocrystals.
Magnetic microscopy of malarial hemozoin nanocrystals was performed using optically detected magnetic resonance imaging of near-surface diamond nitrogen-vacancy centers. Hemozoin crystals were extracted from $Plasmodium$-$falciparum$-infected human blood cells and studied alongside synthetic hemozoin crystals. The stray magnetic fields produced by individual crystals were imaged at room temperature as a function of applied field up to 350 mT. More than 100 nanocrystals were analyzed, revealing the distribution of their magnetic properties. Most crystals ($96\%$) exhibit a linear dependence of stray field magnitude on applied field, confirming hemozoin's paramagnetic nature. A volume magneti…
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 $B$.
Electric-Field-Induced Symmetry Breaking of Angular Momentum Distribution in Atoms
We report the experimental observation of alignment to orientation conversion in the 7D_3/2 and 9D_3/2 states of Cs in the presence of an external dc electric field, and without the influence of magnetic fields or atomic collisions. Initial alignment of angular momentum states was created by two-step excitation with linearly polarized laser radiation. The appearance of transverse orientation of angular momentum was confirmed by the observation of circularly polarized light. We present experimentally measured signals and compare them with the results of a detailed theoretical model based on the optical Bloch equations.
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…
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…
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.
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…
Nuclear quadrupole resonance spectroscopy with a femtotesla diamond magnetometer
Sensitive Radio-Frequency (RF) magnetometers that can detect oscillating magnetic fields at the femtotesla level are needed for demanding applications such as Nuclear Quadrupole Resonance (NQR) spectroscopy. RF magnetometers based on Nitrogen-Vacancy (NV) centers in diamond have been predicted to offer femtotesla sensitivity, but published experiments have largely been limited to the picotesla level. Here, we demonstrate a femtotesla RF magnetometer based on an NV-doped diamond membrane inserted between two ferrite flux concentrators. The device operates in bias magnetic fields of 2-10 microtesla and provides a ~300-fold amplitude enhancement within the diamond for RF magnetic fields in the…
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…
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…
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…
Two-dimensional nuclear magnetic resonance spectroscopy with a microfluidic diamond quantum sensor
Quantum sensors based on nitrogen-vacancy centers in diamond have emerged as a promising detection modality for nuclear magnetic resonance (NMR) spectroscopy owing to their micron-scale detection volume and non-inductive based detection. A remaining challenge is to realize sufficiently high spectral resolution and concentration sensitivity for multidimensional NMR analysis of picoliter sample volumes. Here, we address this challenge by spatially separating the polarization and detection phases of the experiment in a microfluidic platform. We realize a spectral resolution of 0.65 +/- 0.05 Hz, an order-of-magnitude improvement over previous diamond NMR studies. We use the platform to perform …
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…
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.
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…
Demonstration of diamond nuclear spin gyroscope
Description
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…