arXiv subjects

Jure Demsar

Publications and source records attributed to Jure Demsar.

At least 19 recordsLinked to original sources

arXiv2026

Pressure-tuning of electronic structure of CeTe3 probed by femtosecond collective mode spectroscopy

We use femtosecond optical spectroscopy to study the evolution of coherent order-parameter dynamics in the prototypical charge-density-wave (CDW) system CeTe3 under hydrostatic pressure. The CDW transition temperature decreases from approximately 570 K at ambient pressure to near room temperature at approximately 6 GPa. The pressure dependence of the order-parameter recovery dynamics indicates enhanced electron-phonon coupling with increasing pressure, implying that CDW suppression is driven predominantly by the reduction in Fermi-surface nesting. Above 7 GPa, no evidence of CDW order is observed down to cryogenic temperatures. Concurrently, the relaxation dynamics exhibit significant slowing down at low-temperatures, consistent with emerging heavy-electron behaviour due to pressure-enhanced hybridization between localized Ce 4f levels and itinerant carriers.

cond-mat.str-el↗

arXiv2026

Ultrafast decoupling of quasiparticles and spin fluctuations in superconducting cuprates

Understanding how quasiparticles are generated following a rapid quench of superconductivity in high-Tc cuprates is a key unresolved problem in nonequilibrium superconductivity. Here we resolve these processes in optimally doped YBCO [YBa2Cu3Oy(y=6.94, Tc=92 K)] using broadband (0.16 -4.1 eV, ca. 100 fs) and nearly single-cycle (6 fs) transient reflectivity spectroscopy. We show that within a few femtosecond, enhanced electron-electron Umklapp scattering dominates, signaling a transient modulation of long-range Coulomb interactions on the eV scale. This regime is followed by a rapid suppression of the scattering rate of the mid-infrared absorption associated with carriers dressed by spin fluctuations. We attribute this observation to an ultrafast decoupling of quasiparticles from the spin-fluctuation background, occurring on a 90 fs timescale set by the inverse optical gap. These findings reveal the correlated many-body dynamics underlying quasiparticle generation in cuprates and provide further clues for unconventional pairing mechanism.

cond-mat.str-el↗

arXiv2026

Ultrafast Decoherence of Charge Density Waves in K$_{0.3}$MoO$_{3}$

Recent works have suggested that transient suppression of a charge density wave (CDW) by an ultra-short excitation can lead to an inversion of the CDW phase. We experimentally investigate the dynamics of the CDW in K$_{0.3}$MoO$_{3}$ by time resolved x-ray diffraction after excitation with optical pulses. Our results indicate a transient inversion of the CDW phase close to the surface that evolves into a highly disordered state in less than one picosecond. Numerical simulations solving the Ginzburg-Landau equation including disorder from strong pinning defects reproduce our main observations. Our findings highlight the critical role of disorder in schemes for coherent control in condensed matter systems.

cond-mat.str-el↗

arXiv2023

Possible Eliashberg-type superconductivity enhancement effects in a two-band superconductor MgB2 driven by narrow-band THz pulses

We study THz-driven condensate dynamics in epitaxial thin films of MgB$_{2}$, a prototype two-band superconductor (SC) with weak interband coupling. The temperature and excitation density dependent dynamics follow the behavior predicted by the phenomenological bottleneck model for the single-gap SC, implying adiabatic coupling between the two condensates on the ps timescale. The amplitude of the THz-driven suppression of condensate density reveals an unexpected decrease in pair-breaking efficiency with increasing temperature - unlike in the case of optical excitation. The reduced pair-breaking efficiency of narrow-band THz pulses, displaying minimum near $\approx0.7$ T$_{c}$, is attributed to THz-driven, long-lived, non-thermal quasiparticle distribution, resulting in Eliashberg-type enhancement of superconductivity, competing with pair-breaking.

cond-mat.supr-con↗

arXiv2023

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 electron-phonon coupling parameters. While the coupling is indeed strongest for the lowest-energy phonon, dropping sharply for the immediately subsequent phonons, it grows back significantly for the higher-energy phonons, demonstrating their important role in driving the CDW formation. We also include a reassessment of our previous analysis of the lowest-lying phase modes, whereby assuming weaker electronic damping for the phase channel results in a qualitative picture more consistent with quantum-mechanical treatments of the collective modes, with a strongly coupled amplitudon and phason as the lowest modes.

cond-mat.str-el↗

arXiv2023

Collective modes in the charge-density wave state of K$_{0.3}$MoO$_3$: The role of long-range Coulomb interactions revisited

We re-examine the effect of long-range Coulomb interactions on the collective amplitude and phase modes in the incommensurate charge-density-wave ground state of quasi-one-dimensional conductors. Using an effective action approach we show that the longitudinal acoustic phonon protects the gapless linear dispersion of the lowest phase mode in the presence of long-range Coulomb interactions. Moreover, in Gaussian approximation, amplitude fluctuations are not affected by long-range Coulomb interactions. We also calculate the collective mode dispersions at finite temperatures and compare our results with the measured energies of amplitude and phase modes in K$_{0.3}$MoO$_3$. With the exception of the lowest phase mode, the temperature dependence of the measured mode energies can be quantitatively described within a multi-phonon Fr\"{o}hlich model for generic electron-phonon interactions neglecting long-range Coulomb interactions.

cond-mat.str-el↗

arXiv2022

Highly anisotropic transient optical response of charge density wave order in ZrTe$_3$

Low dimensionality in CDW systems leads to anisotropic optical properties, in both equilibrium and non-equilibrium conditions. Here we perform polarized two-color pump probe measurements on a quasi-1D material ZrTe$_3$, in order to study the anisotropic transient optical response in the CDW state. Profound in-plane anisotropy is observed with respect to polarization of probe photons. Below $T_\mathrm{CDW}$ both the quasi-particle relaxation signal and amplitude mode (AM) oscillation signal are much larger with $\mathbf{E}_\mathrm{pr}$ nearly parallel to $a$ axis ($\mathbf{E}_\mathrm{pr} \parallel a$) than for $\mathbf{E}_\mathrm{pr}$ parallel to $b$ axis ($\mathbf{E}_\mathrm{pr} \parallel b$). This reveals that $\mathbf{E}_\mathrm{pr} \parallel a$ signal is much more sensitive to the variation of the CDW gap. Interestingly, the lifetime of the AM oscillations observed with $\mathbf{E}_\mathrm{pr} \parallel b$ is longer than $\mathbf{E}_\mathrm{pr} \parallel a$. Moreover, at high pump fluence where the electronic order melts and the AM oscillations vanish for $\mathbf{E}_\mathrm{pr} \parallel a$ , the AM oscillatory response still persists for $\mathbf{E}_\mathrm{pr} \parallel b$. We discuss possible origins that lead to such unusual discrepancy between the two polarizations.

cond-mat.str-el↗

arXiv2022

Selective coupling of coherent optical phonons in YBa$_2$Cu$_3$O$_{7-\delta}$ with electronic transitions

We investigate coherent lattice dynamics in optimally doped YBa$_2$Cu$_3$O$_{7-\delta}$ driven by ultrashort ($\sim$ 12 fs) near infrared (NIR) and near ultraviolet (NUV) pulses. Transient reflectivity experiments, performed at room temperature and under moderate ($<$0.1 mJ/cm$^2$) excitation fluence, reveal $A_g$-symmetry phonon modes related to the O(2,3) bending in the CuO$_2$ planes and to the apical O(4) stretching at frequencies between 10 and 15 THz, in addition to the previously reported Ba and Cu(2) vibrations at 3.5 and 4.5 THz. The relative coherent phonon amplitudes are in stark contrast to the relative phonon intensities in the spontaneous Raman scattering spectrum excited at the same wavelength. This contrast indicates mode-dependent contributions of the Raman and non-Raman mechanisms to the coherent phonon generation. We show that the particularly intense coherent Cu(2) phonon, together with its initial phase, supports its generation predominately via a displacive mechanism, possibly involving the charge transfer within the CuO$_2$ planes. The small amplitude of the coherent out-of-phase O(2,3) bending mode at 10 THz also suggests the involvement of non-Raman generation mechanism. The generation of the other coherent phonons can in principle be explained within the framework of Raman mechanism. When the pump light has the polarization component perpendicular to the CuO$_2$ plane, the coherent O(4) mode at 15 THz is strongly enhanced compared to the in-plane excitation, corresponding to the large polarizability component associated with the hopping between the apical and the chain oxygens, O(4) and O(1).

cond-mat.mtrl-sci↗

arXiv2022

Tracking the surface atomic motion in a coherent phonon oscillation

X-ray photoelectron diffraction is a powerful tool for determining the structure of clean and adsorbate-covered surfaces. Extending the technique into the ultrafast time domain will open the door to studies as diverse as the direct determination of the electron-phonon coupling strength in solids and the mapping of atomic motion in surface chemical reactions. Here we demonstrate time-resolved photoelectron diffraction using ultrashort soft X-ray pulses from the free electron laser FLASH. We collect Se 3d photoelectron diffraction patterns over a wide angular range from optically excited Bi$_2$Se$_3$ with a time resolution of 140 fs. Combining these with multiple scattering simulations allows us to track the motion of near-surface atoms within the first 3 ps after triggering a coherent vibration of the A$_{1g}$ optical phonons. Using a fluence of 4.2 mJ/cm$^2$ from a 1.55 eV pump laser, we find the resulting coherent vibrational amplitude in the first two interlayer spacings to be on the order of 1 pm.

cond-mat.mtrl-sci↗

arXiv2022

Optically-triggered strain-driven Néel vector manipulation in a metallic antiferromagnet

The absence of stray fields, their insensitivity to external magnetic fields, and ultrafast dynamics make antiferromagnets promising candidates for active elements in spintronic devices. Here, we demonstrate manipulation of the Néel vector in the metallic collinear antiferromagnet Mn$_2$Au by combining strain and femtosecond laser excitation. Applying tensile strain along either of the two in-plane easy axes and locally exciting the sample by a train of femtosecond pulses, we align the Néel vector along the direction controlled by the applied strain. The dependence on the laser fluence and strain suggests the alignment is a result of optically-triggered depinning of 90$^{\mathrm{o}}$ domain walls and their sliding in the direction of the free energy gradient, governed by the magneto-elastic coupling. The resulting, switchable, state is stable at room temperature and insensitive to magnetic fields. Such an approach may provide ways to realize robust high-density memory device with switching timescales in the picosecond range.

cond-mat.mtrl-sci↗

arXiv2022

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

BaNi$_{2}$As$_{2}$ is a non-magnetic analogue of BaFe$_{2}$As$_{2}$, 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 dynamics in BaNi$_{2}$As$_{2}$. We demonstrate the existence of several CDW amplitude modes. Their smooth evolution through the structural phase transition implies the commensurate CDW order in the triclinic phase evolves from the high-temperature unidirectional incommensurate CDW, and may indeed trigger the structural phase transition. Excitation density dependence reveals exceptional resilience of CDW against perturbation, implying an unconventional origin of the underlying electronic instability.

cond-mat.supr-con↗

arXiv2021

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 $2f=2Δ_π(T)$ fulfilled, for the dirty-limit superconducting gap $2Δ_π$. In contrast, for $f=$ 0.6 and 0.7 THz with $2f>2Δ_π(T\rightarrow0)=1.03$ THz, the THG intensity increases monotonically with decreasing temperature. Moreover, for $2f<2Δ_π(T\rightarrow0)$ the THG is found nearly isotropic with respect to the pump-pulse polarization. These results suggest a predominant contribution of the driven Higgs amplitude mode of the dirty-limit $π$-band superconducting gap, pointing to the importance of scattering for observation of the Higgs mode in superconductors.

cond-mat.supr-con↗

arXiv2021

Direct Observation of Antiferromagnetic Parity Violation in the Electronic Structure of Mn$_2$Au

Parity symmetric photoemission spectra are ubiquitous in solid state research, being prevalent in many highly active areas, such as unconventional superconductors, nonmagnetic and antiferromagnetic topological insulators, and weakly relativistic collinear magnets, among others. The direct observation of parity-violating metallic Kramers degenerate bands has remained hitherto experimentally elusive. Here we observe the antiferromagnetic parity violation (APV) in the bandstructure of Mn$_2$Au thin films by using momentum microscopy with sub-$mu$m spatial resolution, allowing momentum resolved photoemission on single antiferromagnetic domains. The APV arises from breaking the P symmetry of the underlying crystal structure by the collinear antiferromagnetism, while preserving the joint space-time inverison PT -symmetry and in combination with large spin-orbit coupling. In addition, our work also demonstrates a novel tool to directly image the Neel vector direction by combining spatially resolved momentum microscopy with ab-initio calculations.

cond-mat.mtrl-sci↗

arXiv2021

Optical read-out of the Néel vector in metallic antiferromagnet Mn$_{2}$Au

Metallic antiferromagnets with broken inversion symmetry on the two sublattices, strong spin-orbit coupling and high Néel temperatures offer new opportunities for applications in spintronics. Especially Mn$_{2}$Au, with high Néel temperature and conductivity, is particularly interesting for real-world applications. Here, manipulation of the orientation of the staggered magnetization,\textit{\ i.e.} the Néel 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 Néel vector aligned in pulsed magnetic fields. In the near-infrared, the anisotropy is $\approx$ 0.6\%, with higher reflectivity for the light polarized along the Néel vector. The observed magnetic linear dichroism is about four times larger than the anisotropic magnetoresistance. This suggests the dichroism in Mn$_{2}$Au is a result of the strong spin-orbit interactions giving rise to anisotropy of interband optical transitions, in-line with recent studies of electronic band-structure. The considerable magnetic linear dichroism in the near-infrared could be used for ultrafast optical read-out of the Néel vector in Mn$_{2}$Au.

cond-mat.mtrl-sci↗

arXiv2021

Ultrafast electronic line width broadening in the C 1s core level of graphene

Core level binding energies and absorption edges are at the heart of many experimental techniques concerned with element-specific structure, electronic structure, chemical reactivity, elementary excitations and magnetism. X-ray photoemission spectroscopy (XPS) in particular, can provide information about the electronic and vibrational many-body interactions in a solid as these are reflected in the detailed energy distribution of the photoelectrons. Ultrafast pump-probe techniques add a new dimension to such studies, introducing the ability to probe a transient state of the many-body system. Here we use a free electron laser to investigate the effect of a transiently excited electron gas on the core level spectrum of graphene, showing that it leads to a large broadening of the C 1s peak. Confirming a decade-old prediction, the broadening is found to be caused by an exchange of energy and momentum between the photoemitted core electron and the hot electron system, rather than by vibrational excitations. This interpretation is supported by a line shape analysis that accounts for the presence of the excited electrons. Fitting the spectra to this model directly yields the electronic temperature of the system, in agreement with electronic temperature values obtained from valence band data. Furthermore, making use of time- and momentum-resolved C 1s spectra, we illustrate how the momentum change of the outgoing core electrons leads to a small but detectable change in the time-resolved photoelectron diffraction pattern and to a nearly complete elimination of the core level binding energy variation associated with the narrow $σ$-band in the C 1s state. The results demonstrate that the XPS line shape can be used as an element-specific and local probe of the excited electron system and that X-ray photoelectron diffraction investigations remain feasible at very high electronic temperatures.

cond-mat.str-el↗

arXiv2021

Subpicosecond metamagnetic phase transition driven by non-equilibrium electron dynamics

Femtosecond light-induced phase transitions between different macroscopic orders provide the possibility to tune the functional properties of condensed matter on ultrafast timescales. In first-order phase transitions, transient non-equilibrium phases and inherent phase coexistence often preclude non-ambiguous detection of transition precursors and their temporal onset. Here, we present a study combining time-resolved photoelectron spectroscopy and ab-initio electron dynamics calculations elucidating the transient subpicosecond processes governing the photoinduced generation of ferromagnetic order in antiferromagnetic FeRh. The transient photoemission spectra are accounted for by assuming that not only the occupation of electronic states is modified during the photoexcitation process. Instead, the photo-generated non-thermal distribution of electrons modifies the electronic band structure. The ferromagnetic phase of FeRh, characterized by a minority band near the Fermi energy, is established 350+- 30 fs after the laser excitation. Ab-initio calculations indicate that the phase transition is initiated by a photoinduced Rh-to-Fe charge transfer.

cond-mat.str-el↗

arXiv2020

An open-source, end-to-end workflow for multidimensional photoemission spectroscopy

Characterization of the electronic band structure of solid state materials is routinely performed using photoemission spectroscopy. Recent advancements in short-wavelength light sources and electron detectors give rise to multidimensional photoemission spectroscopy, allowing parallel measurements of the electron spectral function simultaneously in energy, two momentum components and additional physical parameters with single-event detection capability. Efficient processing of the photoelectron event streams at a rate of up to tens of megabytes per second will enable rapid band mapping for materials characterization. We describe an open-source workflow that allows user interaction with billion-count single-electron events in photoemission band mapping experiments, compatible with beamlines at $3^{\text{rd}}$ and $4^{\text{th}}$ generation light sources and table-top laser-based setups. The workflow offers an end-to-end recipe from distributed operations on single-event data to structured formats for downstream scientific tasks and storage to materials science database integration. Both the workflow and processed data can be archived for reuse, providing the infrastructure for documenting the provenance and lineage of photoemission data for future high-throughput experiments.

physics.data-an↗

arXiv2020

Non-equilibrium phenomena in superconductors probed by femtosecond time-domain spectroscopy

Development of ultrafast lasers and non-linear optical techniques over the last two decades provides tools to access real-time dynamics of low energy excitations in superconductors. For example, time-resolved THz spectroscopy and time- and angular-resolved photoemission spectroscopy provide access to the real-time dynamics of the superconducting gap amplitude. Such studies enable determination of microscopic parameters like quasi-particle recombination rates, pair-breaking rates and electron-boson coupling constants. Recently, intense THz pulses have been used to probe the non-linear dynamics, including observation of collective modes. Moreover, using low frequency electromagnetic pulses, there are several reports of amplification of superconductivity in both conventional and unconventional superconductors. Starting with a brief historical overview of the pioneering work, where non-equilibrium phenomena in superconductors were investigated using quasi-continuous excitation, we review some of the insights that are provided by using real-time approaches. We focus on conventional BCS superconductors, whose ground state is reasonably well understood, and address similarities and open questions related to the corresponding studies in high-T$_{c}$ superconductors.

cond-mat.supr-con↗