Energy dependence of the electron-boson coupling strength in the electron-doped cuprate superconductor Pr1.85Ce0.15CuO4−δ

In the conventional theory of superconductivity the critical temperature Tc is determined by the electron-phonon coupling constant and the phonon cut-off frequency. The hallmark experiments of McMillan and Rowell demonstrated that bosons (phonons) responsible for pairing can be observed through the frequency dependence of the gap parameter. Determination of the electron-boson coupling strength in high-${T}_{c}$ cuprates is, however, not an easy task. One of the promising ways is to measure the energy relaxation rate of photoexcited carriers by using femtosecond real-time techniques. Here, considering the electron relaxation process within the conduction band, it is commonly assumed that the…

Band-selective third-harmonic generation in superconducting MgB$_2$: Possible evidence for Higgs amplitude mode in the dirty limit

We report on time-resolved linear and nonlinear terahertz spectroscopy of the two-band superconductor MgB$_2$ with the superconducting transition temperature $T_c \approx 36$ K. Third-harmonic generation (THG) is observed below $T_c$ by driving the system with intense narrowband THz pulses. For the pump-pulse frequencies $f=$ 0.3, 0.4, and 0.5 THz, temperature-dependent evolution of the THG signals exhibits a resonance maximum at the temperatures with the resonance conditions $2f=2\Delta_\pi(T)$ fulfilled, for the dirty-limit superconducting gap $2\Delta_\pi$. In contrast, for $f=$ 0.6 and 0.7 THz with $2f>2\Delta_\pi(T\rightarrow0)=1.03$ THz, the THG intensity increases monotonically with …

Static and dynamic properties of low-temperature order in the one-dimensional semiconductor(NbSe4)3I

We investigated static and dynamic lattice properties in a quasi-one-dimensional charge-ordered semiconductor ${({\mathrm{NbSe}}_{4})}_{3}\mathrm{I}$ by using Raman, femtosecond pump-probe spectroscopy and x-ray diffraction. In addition to a well-documented pseudo-Jahn-Teller ferrodistortive structural transition at ${T}_{C}=274$ K, where the displacements of Nb ions lead to ferroelectric (FE) in-chain polarization with opposite direction in adjacent chains, all methods suggest an additional lowering of symmetry at ${T}^{*}\ensuremath{\approx}160$ K. Although antiferroelectric (AFE) phase is partially formed at ${T}_{C}$, our results consistently point to an enhancement of the interchain or…

Optical read-out of the N\'eel vector in metallic antiferromagnet Mn$_{2}$Au

Metallic antiferromagnets with broken inversion symmetry on the two sublattices, strong spin-orbit coupling and high N\'{e}el temperatures offer new opportunities for applications in spintronics. Especially Mn$_{2}$Au, with high N\'{e}el temperature and conductivity, is particularly interesting for real-world applications. Here, manipulation of the orientation of the staggered magnetization,\textit{\ i.e.} the N\'{e}el vector, by current pulses has been recently demonstrated, with the read-out limited to studies of anisotropic magnetoresistance or X-ray magnetic linear dichroism. Here, we report on the in-plane reflectivity anisotropy of Mn$_{2}$Au (001) films, which were N\'{e}el vector al…

Tracking the time-evolution of the electron distribution function in Copper by femtosecond broadband optical spectroscopy

Multitemperature models are nowadays often used to quantify the ultrafast electron-phonon (boson) relaxations and coupling strengths in advanced quantum solids. To test their applicability and limitations, we perform systematic studies of carrier relaxation dynamics in copper, a prototype system for which the two-temperature model (TTM) was initially considered. Using broadband time-resolved optical spectroscopy, we study the time evolution of the electron distribution function, $f(E)$, over a large range of excitation densities. Following intraband optical excitation, $f(E)$ is found to be athermal over several 100 fs, with a substantial part of the absorbed energy already being transferre…

Cooperative atomic motion probed by ultrafast transmission electron diffraction

In numerous solids exhibiting broken symmetry ground states, changes in electronic (spin) structure are accompanied by structural changes. Femtosecond time-resolved techniques recently contributed many important insights into the origin of their ground states by tracking dynamics of the electronic subsystem with femtosecond light pulses. Moreover, several studies of structural dynamics in systems with periodic lattice modulation (PLD) were performed. Since intensities of the super-lattice diffraction peaks are in the first approximation proportional to the square of the PLD amplitude, their temporal dynamics provides access to cooperative atomic motion. This process takes place on a fractio…

Optical control of vibrational coherence triggered by an ultrafast phase transition

Femtosecond time-resolved x-ray diffraction is employed to study the dynamics of the periodic lattice distortion (PLD) associated with the charge-density-wave (CDW) in K0.3MoO3. Using a multi-pulse scheme we show the ability to extend the lifetime of coherent oscillations of the PLD about the undistorted structure through re-excitation of the electronic states. This suggests that it is possible to enter a regime where the symmetry of the potential energy landscape corresponds to the high symmetry phase but the scattering pathways that lead to the damping of coherent dynamics are still controllable by altering the electronic state population. The demonstrated control over the coherence time …

Band-selective third-harmonic generation in superconducting MgB2 : Possible evidence for the Higgs amplitude mode in the dirty limit

Dynamics of Collective Modes in an unconventional Charge Density Wave system BaNi$_{2}$As$_{2}$

AbstractBaNi2As2 is a non-magnetic analogue of BaFe2As2, the parent compound of a prototype pnictide high-temperature superconductor, displaying superconductivity already at ambient pressure. Recent diffraction studies demonstrated the existence of two types of periodic lattice distortions above and below the triclinic phase transition, suggesting the existence of an unconventional charge-density-wave (CDW) order. The suppression of CDW order upon doping results in a sixfold increase in the superconducting transition temperature and enhanced nematic fluctuations, suggesting CDW is competing with superconductivity. Here, we apply time-resolved optical spectroscopy to investigate collective d…

Manipulation of charge transfer and transport in plasmonic-ferroelectric hybrids for photoelectrochemical applications

Utilizing plasmonic nanostructures for efficient and flexible conversion of solar energy into electricity or fuel presents a new paradigm in photovoltaics and photoelectrochemistry research. In a conventional photoelectrochemical cell, consisting of a plasmonic structure in contact with a semiconductor, the type of photoelectrochemical reaction is determined by the band bending at the semiconductor/electrolyte interface. The nature of the reaction is thus hard to tune. Here instead of using a semiconductor, we employed a ferroelectric material, Pb(Zr,Ti)O3 (PZT). By depositing gold nanoparticle arrays and PZT films on ITO substrates, and studying the photocurrent as well as the femtosecond …

Combined investigation of collective amplitude and phase modes in a quasi-one-dimensional charge-density-wave system over a wide spectral range

We investigate experimentally both the amplitude and phase channels of the collective modes in the quasi-1D charge-density-wave (CDW) system, K0.3MoO3, by combining (i) optical impulsive-Raman pump-probe and (ii) terahertz time-domain spectroscopy (THz-TDS), with high resolution and a detailed analysis of the full complex-valued spectra in both cases. This allows an unequivocal assignment of the observed bands to CDW modes across the THz range up to 9 THz. We revise and extend a time-dependent Ginzburg-Landau model to account for the observed temperature dependence of the modes, where the combination of both amplitude and phase modes allows one to robustly determine the bare-phonon and elec…

Temperature-Dependent Change of the Electronic Structure in the Kondo Lattice System $YbRh_{2}Si_{2}$

Seminar, Deutschland; Journal of physics / Condensed matter 00(00), 1-20 (2021). doi:10.1088/1361-648X/abe479

Ultrafast Metamorphosis of a Complex Charge Density Wave in Tantalumdiselenite

Using ultrafast electron diffraction, we record the transformation between a nearly-commensurate and an incommensurate charge-density-wave in 1T-TaS2, which takes place orders of magnitude faster than previously observed for commensurate-to-incommensurate transitions.

Néel Spin-Orbit Torque Driven Antiferromagnetic Resonance in Mn2Au Probed by Time-Domain THz Spectroscopy

We observe the excitation of collective modes in the terahertz (THz) range driven by the recently discovered Neel spin-orbit torques (NSOTs) in the metallic antiferromagnet Mn_{2}Au. Temperature-dependent THz spectroscopy reveals a strong absorption mode centered near 1 THz, which upon heating from 4 to 450 K softens and loses intensity. A comparison with the estimated eigenmode frequencies implies that the observed mode is an in-plane antiferromagnetic resonance (AFMR). The AFMR absorption strength exceeds those found in antiferromagnetic insulators, driven by the magnetic field of the THz radiation, by 3 orders of magnitude. Based on this and the agreement with our theory modeling, we inf…

Energy scales and dynamics of electronic excitations in functionalized gold nanoparticles measured at the single particle level.

The knowledge of the electronic structure and dynamics of nanoparticles is a prerequisite to develop miniaturized single-electron devices based on nanoparticles. Low-temperature transport measurements of individual stable metallic nanoparticles enable unravelling the system specific electronic structure while ultrafast optical spectroscopy gives access to the electron dynamics. In this work, we investigate bare and thiol-functionalized gold nanoparticles. For the latter, we employ a fast and low-cost fabrication technique which yields nanoparticles with narrow size distribution. Using relatively long thiol-ended alkane chains for the functionalization modifies the electronic density of stat…

Single crystal-like thin films of blue bronze

Abstract Pulsed laser deposition technique was employed to grow thin films of K 0.3 M o O 3 on A l 2 O 3 (1-102) and S r T i O 3 (510) substrates. Structural and imaging characterization revealed good quality films with well oriented grains of few microns in length. Both non-selective (transport) and order-selective (femtosecond pump-probe spectroscopy) probes revealed charge density wave properties that are very close to those of the single crystals. The films exhibit metal-semiconductor phase transition in resistivity, pump-probe data show phase transition at the same temperature as the single crystal and the threshold for the photo-induced phase transition is approximately the same as in…

Robust hybridization gap in the Kondo insulator YbB12 probed by femtosecond optical spectroscopy

In heavy fermions the relaxation dynamics of photoexcited carriers has been found to be governed by the low energy indirect gap ${\mathrm{E}}_{g}$ resulting from hybridization between localized moments and conduction band electrons. Here, carrier relaxation dynamics in a prototype Kondo insulator $\mathrm{Yb}{\mathrm{B}}_{12}$ is studied over a large range of temperatures and over three orders of magnitude. We utilize the intrinsic nonlinearity of dynamics to quantitatively determine microscopic parameters, such as electron-hole recombination rate. The extracted value reveals that hybridization is accompanied by a strong charge transfer from localized $4f$ levels. The results imply the pres…

Collective Modes and Structural Modulation in Ni-Mn-Ga(Co) Martensite Thin Films Probed by Femtosecond Spectroscopy and Scanning Tunneling Microscopy.

International audience; The origin of the martensitic transition in the magnetic shape memory alloy Ni-Mn-Ga has been widely discussed. While several studies suggest it is electronically driven, the adaptive martensite model reproduced the peculiar nonharmonic lattice modulation. We used femtosecond spectroscopy to probe the temperature and doping dependence of collective modes, and scanning tunneling microscopy revealed the corresponding static modulations. We show that the martensitic phase can be described by a complex charge-density wave tuned by magnetic ordering and strong electron-lattice coupling.

Ultrafast Metamorphosis of a Complex Charge-Density Wave

Modulated phases, commensurate or incommensurate with the host crystal lattice, are ubiquitous in solids. The transition between such phases involves formation and rearrangement of domain walls and is generally slow. Using ultrafast electron diffraction, we directly record the photoinduced transformation between a nearly commensurate and an incommensurate charge-density-wave phase in 1T-TaS(2). The transformation takes place on the picosecond time scale, orders of magnitude faster than previously observed for commensurate-to-incommensurate transitions. The transition speed and mechanism can be linked to the peculiar nanoscale structure of the photoexcited nearly commensurate phase.

Light-induced superconductivity

Intense light pulses irradiating a sample of K3C60 result in dramatic changes of its high-frequency (terahertz) conductivity. Could these be signatures of fleeting superconductivity at 100 K and beyond?