arXiv subjects

J. Demsar

Publications and source records attributed to J. Demsar.

At least 19 recordsLinked to original sources

arXiv2025

Orbital magnetization in the Nb-substituted Kagome metal CsV$_3$Sb$_5$

This study uses angle-resolved photoemission spectroscopy to examine the low-temperature electronic structure of Cs(V$_{0.95}$Nb$_{0.05}$)$_3$Sb$_5$, demonstrating that partially substituting V atoms with isoelectronic Nb atoms results in \blue{an increase of the band width} and enhanced gap opening at the Dirac-like crossings due to the resulting chemical pressure. This increases the magnetic circular dichroism signal in the angular distribution (MCDAD) compared to CsV$_3$Sb$_5$, enabling detailed analysis of magnetic circular dichroism in several bands near the Fermi level. These results \blue{substantiate} the predicted coupling of orbital magnetic moments to three van Hove singularities near the Fermi level at M points. Previous studies have observed that Nb doping \blue{lowers the charge density transition temperature} and increases the critical temperature for superconductivity. This article demonstrates that Nb doping concomitantly increases the magnetic circular dichroism signal attributed to orbital moments.

cond-mat.mtrl-sci↗

arXiv2024

Chirality in the Kagome Metal CsV$_3$Sb$_5$

Using x-ray photoelectron diffraction (XPD) and angle-resolved photoemission spectroscopy, we study photoemission intensity changes related to changes in the geometric and electronic structure in the kagome metal CsV$_3$Sb$_5$ upon transition to an unconventional charge density wave (CDW) state. The XPD patterns reveal the presence of a chiral atomic structure in the CDW phase. Furthermore, using circularly polarized x-rays, we have found a pronounced non-trivial circular dichroism in the angular distribution of the valence band photoemission in the CDW phase, indicating a chirality of the electronic structure. This observation is consistent with the proposed orbital loop current order. In view of a negligible spontaneous Kerr signal in recent magneto-optical studies, the results suggest an antiferromagnetic coupling of the orbital magnetic moments along the $c$-axis. While the inherent structural chirality may also induce circular dichroism, the observed asymmetry values seem to be too large in the case of the weak structural distortions caused by the CDW.

cond-mat.str-el↗

arXiv2023

Control of the asymmetric band structure in Mn2Au by a ferromagnetic driver layer

Hard X-ray angle-resolved photoemission spectroscopy reveals the momentum-resolved band structure in an epitaxial Mn2Au(001) film capped by a 2 nm thick ferromagnetic Permalloy layer. By magnetizing the Permalloy capping layer, the exceptionally strong exchange bias aligns the Neel vector in the Mn2Au(001) film accordingly. Uncompensated interface Mn magnetic moments in Mn2Au were identified as the origin of the exchange bias using X-ray magnetic circular dichroism in combination with photoelectron emission microscopy. Using time-of-flight momentum microscopy, we measure the asymmetry of the band structure in Mn2Au resulting from the homogeneous orientation of the Neel vector. Comparison with theory shows that the Neel vector, determined by the magnetic moment of the top Mn layer, is antiparallel to the Permalloy magnetization. The experimental results demonstrate that hard X-ray photoemission spectroscopy can measure the band structure of epitaxial layers beneath a metallic capping layer and corroborate the asymmetric band structure in Mn2Au that was previously inferred only indirectly.

cond-mat.mtrl-sci↗

arXiv2021

Robust hybridization gap in a Kondo Insulator YbB${}_{12}$ 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, E$_{g}$, resulting from hybridization between localized moments and conduction band electrons. Here, carrier relaxation dynamics in a prototype Kondo insulator YbB${}_{12}$ is studied over large range of temperatures and over three orders of magnitude. We utilize the intrinsic non-linearity 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 presence of a hybridization gap up to temperatures of the order of E$_{g}$/k$_{B}\approx200$ K, which is extremely robust against electronic excitation. Finally, below 20 K the data reveal changes in the low energy electronic structure, attributed to short-range antiferromagnetic correlations between the localized levels.

cond-mat.str-el↗

arXiv2019

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 offers new routes for manipulation of coherent lattice states.

cond-mat.str-el↗

arXiv2018

N\'{e}el Spin Orbit Torque driven antiferromagnetic resonance in Mn$_{2}$Au probed by time-domain THz spectroscopy

We observe the excitation of collective modes in the THz range driven by the recently discovered N\'{e}el spin-orbit torques (NSOT) 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 K to 450 K softens and looses intensity. Comparison with the estimated eigenmode frequencies implies that the observed mode is an in-plane antiferromagnetic resonance (AFMR) mode. The AFMR absorption strength exceeds those found in antiferromagnetic insulators, driven by the magnetic field of the THz radiation, by three orders of magnitude. Based on this and the agreement with our theory modelling, we infer that the driving mechanism for the observed mode is the current induced NSOT. This electric manipulation of the Ne\'{e}l order parameter at high frequencies makes Mn$_{2}$Au a prime candidate for AFM ultrafast memory applications.

cond-mat.str-el↗

arXiv2016

Ultrafast Polaron Dynamics in Layered and Perovskite Manganites: 2D and 3D Polarons

We have studied the sub-picosecond quasiparticle dynamics in the perovskite manganite La0.7Ca0.3MnO3 and the layered manganite La1.4Sr1.6Mn2O7 using ultrafast optical spectroscopy. We found that for T > TC, initial relaxation proceeds on the time scale of several hundred femtoseconds and corresponds to the redressing of a photoexcited electron to its polaronic ground state. The temperature and dimensionality dependence of this polaron redressing time provides insight into the relationship between polaronic motion and spin dynamics on a sub-picosecond time scale. We also observe a crossover to a more conventional electron-phonon relaxation in the ferromagnetic metallic phase below Tc.

cond-mat.str-el↗

arXiv2016

Non-thermal separation of electronic and structural orders in a persisting charge density wave

The simultaneous ordering of different degrees of freedom in complex materials undergoing spontaneous symmetry-breaking transitions often involves intricate couplings that have remained elusive in phenomena as wide ranging as stripe formation, unconventional superconductivity or colossal magnetoresistance. Ultrafast optical, x-ray and electron pulses can elucidate the microscopic interplay between these orders by probing the electronic and lattice dynamics separately, but a simultaneous direct observation of multiple orders on the femtosecond scale has been challenging. Here we show that ultrabroadband terahertz pulses can simultaneously trace the ultrafast evolution of coexisting lattice and electronic orders. For the example of a charge-density-wave (CDW) in 1T-TiSe2, we demonstrate that two components of the CDW order parameter - excitonic correlations and a periodic lattice distortion (PLD) - respond very differently to 12-fs optical excitation. Even when the excitonic order of the CDW is quenched, the PLD can persist in a coherently excited state. This observation proves that excitonic correlations are not the sole driving force of the CDW transition in 1T-TiSe2, and exemplifies the sort of profound insight that disentangling strongly coupled components of order parameters in the time domain may provide for the understanding of a broad class of phase transitions.

physics.optics↗

arXiv2016

Melting the Superconducting State in the Electron Doped Cuprate Pr$_{1.85}% $Ce$_{0.15}$CuO$_{4-\delta}$ with Intense near-infrared and Terahertz Pulses

We studied the superconducting (SC) state depletion process in an electron doped cuprate Pr$_{1.85}$Ce$_{0.15}$CuO$_{4-\delta}$ by pumping with near-infrared (NIR) and narrow-band THz pulses. When pumping with THz pulses tuned just above the SC gap, we find the absorbed energy density required to deplete superconductivity, $A_{dep}$, matches the thermodynamic condensation energy. Contrary, by NIR pumping $A_{dep}$ is an order of magnitude higher, despite the fact that the SC gap is much smaller than the energy of relevant bosonic excitations. The result implies that only a small subset of bosons contribute to pairing.

cond-mat.supr-con↗

arXiv2012

Ultrafast dynamics of charge density waves in 4Hb-TaSe2 probed by femtosecond electron diffraction

The dynamics of the photoinduced commensurate to incommensurate charge density wave (CDW) phase transition in 4Hb-TaSe2 are investigated by femtosecond electron diffraction. In the perturbative regime the CDW reforms on a 150 ps timescale, which is two orders of magnitude slower than in other transition-metal dichalcogenides. We attribute this to a weak coupling between the CDW carrying T-layers and thus demonstrate the importance of three-dimensionality for the existence of CDWs. With increasing optical excitation the phase transition is achieved showing a second order character in contrast to the first order behavior in thermal equilibrium.

cond-mat.str-el↗

arXiv2012

Ultrafast transient generation of spin-densitywave order in the normal state of BaFe2As2 driven by coherent lattice vibrations

The interplay among charge, spin and lattice degrees of freedom in solids gives rise to intriguing macroscopic quantum phenomena such as colossal magnetoresistance, multiferroicity and high-temperature superconductivity. Strong coupling or competition between various orders in these systems presents the key to manipulate their functional properties by means of external perturbations such as electric and magnetic fields or pressure. Ultrashort and intense optical pulses have emerged as an interesting tool to investigate elementary dynamics and control material properties by melting an existing order. Here, we employ few-cycle multi-terahertz pulses to resonantly probe the evolution of the spin-density-wave (SDW) gap of the pnictide compound BaFe2As2 following excitation with a femtosecond optical pulse. When starting in the low-temperature ground state, optical excitation results in a melting of the SDW order, followed by ultrafast recovery. In contrast, the SDW gap is induced when we excite the normal state above the transition temperature. Very surprisingly, the transient ordering quasi-adiabatically follows a coherent lattice oscillation at a frequency as high as 5.5 THz. Our results attest to a pronounced spin-phonon coupling in pnictides that supports rapid development of a macroscopic order on small vibrational displacement even without breaking the symmetry of the crystal.

cond-mat.supr-con↗

arXiv2011

Energy-gap dynamics of superconducting NbN thin films studied by time-resolved terahertz spectroscopy

Using time-domain Terahertz spectroscopy we performed direct studies of the photoinduced suppression and recovery of the superconducting gap in a conventional BCS superconductor NbN. Both processes are found to be strongly temperature and excitation density dependent. The analysis of the data with the established phenomenological Rothwarf-Taylor model enabled us to determine the bare quasiparticle recombination rate, the Cooper pair-breaking rate and the electron-phonon coupling constant, λ= 1.1 +/- 0.1, which is in excellent agreement with theoretical estimates.

cond-mat.supr-con↗

arXiv2011

Photoinduced melting of superconductivity in the high-Tc superconductor La2-xSrxCuO4 probed by time-resolved optical and THz techniques

Dynamics of depletion and recovery of superconducting state in La2-xSrxCuO_4 thin films is investigated utilizing optical pump-probe and optical pump - THz probe techniques as a function of temperature and excitation fluence. The absorbed energy density required to suppress superconductivity is found to be about 8 times higher than the thermodynamically determined condensation energy density and nearly temperature independent between 4 and 25 K. These findings indicate that during the time when superconducting state suppression takes place (~0.7 ps), a large part (nearly 90%) of the energy is transferred to the phonons with energy lower than twice the maximum value of of the SC gap and only 10% is spent on Cooper pair breaking.

cond-mat.supr-con↗

arXiv2010

Disentanglement of the electronic and lattice parts of the order parameter in a 1D Charge Density Wave system probed by femtosecond spectroscopy

We report on the high resolution studies of the temperature (T) dependence of the q=0 phonon spectrum in the quasi one-dimensional charge density wave (CDW) compound K0.3MoO3 utilizing time-resolved optical spectroscopy. Numerous modes that appear below Tc show pronounced T-dependences of their amplitudes, frequencies and dampings. Utilizing the time-dependent Ginzburg-Landau theory we show that these modes result from linear coupling of the electronic part of the order parameter to the 2kF phonons, while the (electronic) CDW amplitude mode is overdamped.

cond-mat.str-el↗

arXiv2010

Femtosecond Quasiparticle and Phonon Dynamics in Superconducting YBa2Cu3O7 Studied by Wideband Terahertz Spectroscopy

We measure the anisotropic mid-infrared response of electrons and phonons in bulk YBa2Cu3O7 after femtosecond photoexcitation. A line shape analysis of specific lattice modes reveals their transient occupation and coupling to the superconducting condensate. The apex oxygen vibration is strongly excited within 150 fs demonstrating that the lattice absorbs a major portion of the pump energy before the quasiparticles are thermalized. Our results attest to substantial electron-phonon scattering and introduce a powerful concept probing electron-lattice interactions in a variety of complex materials.

cond-mat.supr-con↗

arXiv2009

Hot electron relaxation in a heavy fermion system with tuned doping

Femtosecond time-resolved optical spectroscopy was used to systematically study photoexcited carrier relaxation dynamics in the intermediate-valence heavy fermion system Yb1-xLuxAl3 (0 < x < 1). Given the demonstrated sensitivity of this experimental technique to the presence of the low energy gaps in the charge excitation spectrum, the aim of this work was to study the effect of dilution of the Kondo lattice on its low energy electronic structure. The results imply that in Yb1-xLuxAl3 the hybridization gap, resulting from hybridization of local moments and conduction electrons, persists up to 30% doping. Interestingly, below some characteristic, doping dependent temperature T*(x) the relaxation time divergence, governed by the relaxation bottleneck due to the presence of the indirect hybridization gap, is truncated. This observation is attributed to the competing ballistic transport of hot electrons out of the probed volume at low temperatures. The derived theoretical model accounts for both the functional form of relaxation dynamics below T*(x), as well as the doping dependence of the low temperature relaxation rate in Yb1-xLuxAl3.

cond-mat.str-el↗

arXiv2009

Morphology Effectively Controls Singlet-Triplet Exciton Relaxation and Charge Transport in Organic Semiconductors

We present a comparative study of ultrafast photo-conversion dynamics in tetracene (Tc) and pentacene (Pc) single crystals and Pc films using optical pump-probe spectroscopy. Photo-induced absorption in Tc and Pc crystals is activated and temperature-independent respectively, demonstrating dominant singlet-triplet exciton fission. In Pc films (as well as C$_{60}$-doped films) this decay channel is suppressed by electron trapping. These results demonstrate the central role of crystallinity and purity in photogeneration processes and will constrain the design of future photovoltaic devices.

cond-mat.other↗

arXiv2009

Dynamics of photoinduced Charge Density Wave-metal phase transition in K0.3MoO3

We present first systematic studies of the photoinduced phase transition from the ground charge density wave (CDW) state to the normal metallic (M) state in the prototype quasi-1D CDW system K0.3MoO3. Ultrafast non-thermal CDW melting is achieved at the absorbed energy density that corresponds to the electronic energy difference between the metallic and CDW states. The results imply that on the sub-picosecond timescale when melting and subsequent initial recovery of the electronic order takes place the lattice remains unperturbed.

cond-mat.str-el↗