arXiv subjects

Stefan Kaiser

Publications and source records attributed to Stefan Kaiser.

At least 19 recordsLinked to original sources

arXiv2026

Dynamics of Charge-Density-Wave puddles in 2$H$-NbSe$_2$

Electronic phases in quantum materials are often governed by nanoscale inhomogeneity, where local order develops within spatially confined regions or puddles. A prominent example is an incommensurate charge-density-wave (I-CDW) that comprises locally commensurate domains. In 2$H$-NbSe$_2$, such an I-CDW state persists alongside lattice anharmonicity and superconductivity, raising fundamental questions about the dynamical stabilization of CDW order in puddles. Here, we probe the puddle-dynamics in 2$H$-NbSe$_2$. Raman scattering reveals a strong Fano-coupling between the interlayer shear vibration and the CDW amplitude mode. Time-resolved reflectivity measurement shows a low-frequency ~0.15 THz coherent overdamped oscillation onsetting within the CDW regime at ~17 K, pointing towards a so far unexplored transition. This we identify as a Fano-coupled phonon-CDW hybrid emerging from the collective dynamics of CDW puddles. We establish a framework for capturing intertwinned glassy dynamics with an overdamped oscillatory model. Such dynamics in 2H-NbSe2 highlight how lattice pinning and electronic correlations in layered materials affect the CDW order, which is crucial for the design of novel Van der Waals devices.

cond-mat.str-el↗

arXiv2025

Dissecting coupled orders in a terahertz-driven electron-doped cuprate

The interplay between superconductivity and charge density wave has often been studied from an equilibrium point of view. For example, using static tuning knobs such as doping, magnetic field and pressure, superconductivity can be enhanced or suppressed. The resulting effect on the co-existing charge density wave order, if any, is judged by variations in its ground state properties such as the ordering temperature or the spatial correlation. Such an approach can be understood as coordinated static displacements of two coupled order parameters within a Ginzburg-Landau description, evincing their interplay as either co-operative or competing but does not provide further microscopic information about the interaction. In order to assess such information, we dynamically perturb both orders from equilibrium and observe their coupling directly in the time-domain. We show that high-field multicycle terahertz pulses drive both the Higgs amplitude fluctuations of the superconducting order as well as collective fluctuations of the charge order in an electron-doped cuprate, resulting in characteristic third harmonic generation. A notable time delay is manifested between their respective driven dynamics. We propose that this may signify the important energy scale describing their coupling or imply a terahertz field-depinned charge density wave that destroys macroscopic superconductivity. Our work demonstrates a holistic approach for investigating coupled superconducting and charge density wave orders, which may shed novel light on their intertwined presence and widespread fluctuations in many classes of unconventional superconductors.

cond-mat.supr-con↗

arXiv2024

Direct observation of the Higgs particle in a superconductor by non-equilibrium Raman scattering

Even before its role in electroweak symmetry breaking, the Anderson-Higgs mechanism was introduced to explain the Meissner effect in superconductors. Spontaneous symmetry-breaking yields massless phase modes representing the low-energy excitations of the Mexican-Hat potential. Only in superconductors the phase mode is shifted towards higher energies owing to the gauge field of the charged condensate. This results in a low-energy excitation spectrum governed by the Higgs mode. Consequently, the Meissner effect signifies a macroscopic quantum condensate in which a photon acquires mass, representing a one-to-one analogy to high-energy physics. We report on the direct observation of the Higgs particle in the high-temperature superconductor Bi-2212 by developing an innovative technique to study its symmetries and energies after a "soft quench" of the Mexican-Hat potential. Population inversion of the metastable Higgs particle induced by an initial laser pulse allows identifying the polarization-dependent Higgs modes as an additional anti-Stokes Raman-scattering signal. Within Ginzburg-Landau theory, the Higgs-mode energy is connected to the Cooper-pair coherence length. Within a BCS weak-coupling model we develop a quantitative and coherent description of single-particle and two-particle channels. This opens the avenue for Higgs Spectroscopy in quantum condensates and provides a unique pathway to control and explore Higgs physics.

cond-mat.supr-con↗

arXiv2024

Noncollinear electric dipoles in a polar, chiral phase of CsSnBr$_3$ perovskite

Polar and chiral crystal symmetries confer a variety of potentially useful functionalities upon solids by coupling otherwise noninteracting mechanical, electronic, optical, and magnetic degrees of freedom. We describe two unstudied phases of the 3D perovskite, CsSnBr$_3$, which emerge below 85 K due to the formation of Sn(II) lone pairs and their interaction with extant octahedral tilts. Phase II (77 K<$T$<85 K, space group $P2_1/m$) exhibits ferroaxial order driven by a noncollinear pattern of lone pair-driven distortions within the plane normal to the unique octahedral tilt axis, preserving the inversion symmetry observed at higher temperatures. Phase I ($T$<77 K, space group $P2_1$) additionally exhibits ferroelectric order due to distortions along the unique tilt axis, breaking both inversion and mirror symmetries. This polar and chiral phase exhibits second harmonic generation from the bulk and a large, intrinsic polarization$-$electrostriction coefficient along the polar axis ($Q_{22}\approx$1.1 m$^4$ C$^{-2}$), resulting in acute negative thermal expansion ($\alpha_V=-9\times10^{-5}$ K$^{-1}$) through the onset of spontaneous polarization. The unprecedented structures of phases I and II were predicted by recursively following harmonic phonon instabilities to generate a tree of candidate structures and subsequently corroborated by synchrotron X-ray powder diffraction and polarized Raman and $^{81}$Br nuclear quadrupole resonance spectroscopies. Relativistic electronic structure scenarios compatible with reported photoluminescence measurements are discussed. Together, the polar symmetry, small bandgap, large spin-orbit splitting of Sn 5$p$ orbitals, and predicted strain sensitivity of the symmetry-breaking distortions suggest bulk samples and epitaxial films of CsSnBr$_3$ or its neighboring solid solutions as strong candidates for bulk Rashba effects.

cond-mat.mtrl-sci↗

arXiv2023

Near-infrared light-induced superconducting-like state in underdoped YBa$_2$Cu$_3$O$_y$ studied by $c$-axis terahertz third-harmonic generation

Recent observation of the light-induced superconducting (SC)-like transient response in the $c$-axis optical conductivity far above the SC transition temperature $T_{\mathrm{c}}$ in underdoped YBa$_2$Cu$_3$O$_y$ (YBCO) has attracted great attention in the field of high-$T_{\mathrm{c}}$ superconductors. Since then, various theoretical and experimental studies have been devoted to elucidating its microscopic origin. One prominent fingerprint of the light-induced superconductivity is the emergence of $1/ω$-like spectral behavior in the imaginary part of the optical conductivity in the terahertz (THz) frequency range. However, the spectral profile can also be described by the Drude response of the quasiparticles (QPs) with a substantially low scattering rate. To circumvent this critical ambiguity, we investigated the light-induced nonequilibrium state in an underdoped YBCO sample with $T_{\mathrm{c}}$ of 61 K using the nonlinear THz optical response originating from the SC collective excitation of the ac-driven Josephson current. Upon the near-infrared (NIR) photoexcitation above $T_{\mathrm{c}}$ in the YBCO sample, the $1/ω$-like spectral behavior in the imaginary part of the optical conductivity emerges, consistent with the previous studies. However, the THz third-harmonic generation arising from the ac-driven Josephson current along the $c$-axis was absent in the NIR photoexcited state. These results indicate that the NIR-pump induced state exhibiting the $1/ω$-like response above $T_{\mathrm{c}}$ is distinct from the long-range ordered SC state in equilibrium. Based on these observations, the possible origins of the irregularly coherent charge carrier response along the $c$-axis induced by the photoexcitation are discussed.

cond-mat.supr-con↗

arXiv2023

Tracing the dynamics of superconducting order via transient third harmonic generation

Ultrafast optical control of quantum systems is an emerging field of physics. In particular, the possibility of light-driven superconductivity with ultrashort laser pulses has attracted much of attention. To identify non-equilibrium superconductivity, it is necessary to measure fingerprints of superconductivity on ultrafast timescales. Recently non-linear THz third harmonic generation (THG) was shown to directly probe the collective degrees of freedoms of the superconducting condensate including particularly the Higgs mode. Here we extend this idea to light-driven non-equilibrium states in superconducting La2-xSrxCuO4 establishing a protocol to access the transient superconducting (SC) order-parameter fluctuations. We perform an optical pump-THz-THG drive experiment and use a two-dimensional spectroscopy approach to disentangle the driven third-harmonic response of optically excited quasiparticles and the pure condensate response. In this way, 2D spectroscopy separately probes both the ultrafast pair breaking dynamics and transient pairing amplitude of the condensate.

cond-mat.supr-con↗

arXiv2022

Dynamical interplay between superconductivity and charge-density-wave: a nonlinear terahertz study of coherently-driven 2H-NbSe2 and La2-xSrxCuO4

2H-NbSe2 is an archetypal system in which superconductivity and charge-density-wave (CDW) coexist and compete macroscopically with each other. In particular, this interplay also manifests in their dynamical fluctuations. As a result, the superconducting amplitude fluctuations (i.e. Higgs mode) is pushed below the quasiparticle continuum, allowing it to become a coherent excitation observable by Raman scattering. In the present study, we coherently drive the collective oscillations of the two orders and visualize their interplay in the driven states in the time domain. We find that both collective modes contribute to terahertz third harmonic generation (THG) and the THG signals interfere below Tc, leading to an anti-resonance of the integrated THG signal. The dynamical Ginzburg-Landau model suggests that around the anti-resonance a periodic energy transfer between the driven Higgs oscillations and the driven CDW oscillations is possible. In addition to 2H-NbSe2, we also studied an underdoped La2-xSrxCuO4 (x ~ 0.12) driven beyond the perturbative regime of THG. A similar interference between two sources of THG is observed below Tc. While there might be additional sources of THG in these experiments, our results illustrate the roles of coupled modes in the terahertz THG process and the tantalizing possibility of coherent control via such couplings.

cond-mat.supr-con↗

arXiv2022

Intense terahertz radiation via the transverse thermoelectric effect

Terahertz (THz) radiation is a powerful tool with widespread applications ranging from imaging, sensing, and broadband communications to spectroscopy and nonlinear control of materials. Future progress in THz technology depends on the development of efficient, structurally simple THz emitters that can be implemented in advanced miniaturized devices. Here we show how the natural electronic anisotropy of layered conducting transition metal oxides enables the generation of intense terahertz radiation via the transverse thermoelectric effect. In thin films grown on offcut substrates, femtosecond laser pulses generate ultrafast out-of-plane temperature gradients, which in turn launch in-plane thermoelectric currents, thus allowing efficient emission of the resulting THz field out of the film structure. We demonstrate this scheme in experiments on thin films of the layered metals PdCoO2 and La1.84Sr0.16CuO4, and present model calculations that elucidate the influence of the material parameters on the intensity and spectral characteristics of the emitted THz field. Due to its simplicity, the method opens up a promising avenue for the development of highly versatile THz sources and integrable emitter elements.

cond-mat.mtrl-sci↗

arXiv2021

Unveiling the underlying interactions in Ta2NiSe5 from photo-induced lifetime change

We present a generic procedure for quantifying the interplay of electronic and lattice degrees of freedom in photo-doped insulators through a comparative analysis of theoretical many-body simulations and time- and angle-resolved photoemission spectroscopy (TR-ARPES) of the transient response of the candidate excitonic insulator Ta2NiSe5. Our analysis demonstrates that the electron-electron interactions dominate the electron-phonon ones. In particular, a detailed analysis of the TRARPES spectrum enables a clear separation of the dominant broadening (electronic lifetime) effects from the much smaller bandgap renormalization. Theoretical calculations show that the observed strong spectral broadening arises from the electronic scattering of the photo-excited particle-hole pairs and cannot be accounted for in a model in which electron-phonon interactions are dominant. We demonstrate that the magnitude of the weaker subdominant bandgap renormalization sensitively depends on the distance from the semiconductor/semimetal transition in the high-temperature state, which could explain apparent contradictions between various TR-ARPES experiments. The analysis presented here indicates that electron-electron interactions play a vital role (although not necessarily the sole one) in stabilizing the insulating state.

cond-mat.str-el↗

arXiv2021

Fano interference of the Higgs mode in cuprate high-Tc superconductors

Despite decades of search for the pairing boson in cuprate high-Tc superconductors, its identity still remains debated to date. For this reason, spectroscopic signatures of electron-boson interactions in cuprates have always been a center of attention. For example, the kinks in the quasiparticle dispersion observed by angle-resolved photoemission spectroscopy (ARPES) studies have motivated a decade-long investigation of electron-phonon as well as electron-paramagnon interactions in cuprates. On the other hand, the overlap between the charge-order correlations and the pseudogap in the cuprate phase diagram has also generated discussions about the potential link between them. In the present study, we provide a fresh perspective on these intertwined interactions using the novel approach of Higgs spectroscopy, i.e. an investigation of the amplitude oscillations of the superconducting order parameter driven by a terahertz radiation. Uniquely for cuprates, we observe a Fano interference of its dynamically driven Higgs mode with another collective mode, which we reveal to be charge density wave fluctuations from an extensive doping- and magnetic field-dependent study. This finding is further corroborated by a mean field model in which we describe the microscopic mechanism underlying the interaction between the two orders. Our work demonstrates Higgs spectroscopy as a novel and powerful technique for investigating intertwined orders and microscopic processes in unconventional superconductors.

cond-mat.supr-con↗

arXiv2021

Phononic soft mode and strong electronic background behavior across the structural phase transition in the excitonic insulator Ta$_2$NiSe$_5$ (with Erratum)

Ta$_2$NiSe$_5$ became one of the most investigated candidate materials for hosting an excitonic insulator ground state. Many studies describe the corresponding phase transition as a condensation of excitons breaking a continuous symmetry. This view got challenged recently pointing out the importance of the loss of two mirror symmetries at a structural phase transition that occurs together with the semiconductor-excitonic insulator transition. For such a scenario an unstable optical zone-center phonon at low energy is proposed to drive the transition. Here we report on the experimental observation of such a soft mode behavior using Raman spectroscopy. In addition we find a novel spectral feature, likely of electronic or joint electronic and phononic origin, that is clearly distinct from the lattice dynamics and that becomes dominant at Tc. This suggests a picture of joint structural and electronic order driving the phase transition.

cond-mat.str-el↗

arXiv2020

Current-assisted Raman activation of the Higgs mode in superconductors

The Higgs mode in superconductors is a scalar mode without electric or magnetic dipole moment. Thus, it is commonly believed that its excitation is restricted to a nonlinear two-photon Raman process. However, recent efforts have shown that a linear excitation in the presence of a supercurrent is possible, resulting in a new resonant enhancement at $Ω=2Δ$ with the driving light frequency $Ω$ and the energy of the Higgs mode $2Δ$. This is in contrast to the usual $2Ω= 2Δ$ resonance condition found in nonlinear third-harmonic generation experiments. In this communication, we show that such a linear excitation can still be described as an effective Raman two-photon process, with one photon at $ω=2Δ$ and one virtual photon at $ω=0$ which represents the dc supercurrent. At the same time we demonstrate that a straightforward infrared activation with a single photon excitation is negligible. Moreover, we give a general context to our theory, providing an explanation for how the excitation of the Higgs mode in both THz quench and drive experiments can be understood within a conventional difference-frequency generation or sum-frequency generation process, respectively. In such a picture, the observed new resonance condition $Ω= 2Δ$ is just a special case. With the same approach, we further discuss another recent experiment, where we find a suppression of odd order higher harmonics in the presence of a dc supercurrent.

cond-mat.supr-con↗

arXiv2020

Phase-resolved Higgs response in superconducting cuprates

In high energy physics, the Higgs field couples to gauge bosons and fermions and gives mass to their elementary excitations. Experimentally, such couplings can be inferred from the decay product of the Higgs boson, i.e. the scalar (amplitude) excitation of the Higgs field. In superconductors, Cooper pairs bear a close analogy to the Higgs field. Interaction between the Cooper pairs and other degrees of freedom provides dissipation channel for the amplitude mode, which may reveal important information about the microscopic pairing mechanism. To this end, we investigate the Higgs (amplitude) mode of several cuprate thin films using phase-resolved terahertz third harmonic generation (THG). In addition to the heavily damped Higgs mode itself, we observe a universal jump in the phase of the driven Higgs oscillation as well as a non-vanishing THG above Tc. These findings indicate coupling of the Higgs mode to other collective modes and potentially a nonzero pairing amplitude above Tc.

cond-mat.supr-con↗

arXiv2019

Possible light-induced superconductivity in a strongly correlated electron system

Using a nonequilibrium implementation of the Lanczos-based exact diagonalisation technique we study the possibility of the light-induced superconducting phase coherence in a solid state system after an ultrafast optical excitation. In particular, we investigate the buildup of superconducting correlations by calculating an exact time-dependent wave function reflecting the properties of the system in non-equilibrium and the corresponding transient response functions. Within our picture we identify a possible transient Meissner effect after dynamical quenching of the non-superconducting wavefunction and extract a characteristic superfluid density that we compare to experimental data. Finally, we find that the stability of the induced superconducting state depends crucially on the nature of the excitation quench: namely, a pure interaction quench induces a long-lived superconducting state, whereas a phase quench leads to a short-lived transient superconductor.

cond-mat.supr-con↗

arXiv2018

Photo-excited Dynamics in the Excitonic Insulator Ta2NiSe5

The excitonic insulator is an intriguing correlated electron phase formed of condensed excitons. A promising candidate is the small band gap semiconductor Ta2NiSe5. Here we investigate the quasiparticle and coherent phonon dynamics in Ta2NiSe5 in a time resolved pump probe experiment. Using the models originally developed by Kabanov et al. for superconductors, we show that the material's intrinsic gap can be described as almost temperature independent for temperatures up to about 250 K to 275 K. This behavior supports the existence of the excitonic insulator state in Ta2NiSe5. The onset of an additional temperature dependent component to the gap above these temperatures suggests that the material is located in the BEC-BCS crossover regime. Furthermore, we show that this state is very stable against strong photoexcitation, which reveals that the free charge carriers are unable to effectively screen the attractive Coulomb interaction between electrons and holes, likely due to the quasi one-dimensional structure of Ta2NiSe5.

cond-mat.str-el↗

arXiv2016

Coherent Order Parameter Oscillations in the Ground State of the Excitonic Insulator Ta2NiSe5

The excitonic insulator is an intriguing electronic phase of quasi-condensed excitons. A prominent candidate is the small bandgap semiconductor Ta2NiSe5, in which excitons are believed to undergo a BEC-like transition. But experimental evidence for the existence of a coherent condensate in this material is still missing. A direct fingerprint of such a state would be the observation of its collective modes, which are equivalent to the Higgs- and Goldstone-modes in superconductors. Here we report evidence for the existence of a coherent amplitude response in the excitonic insulator phase of Ta2NiSe5. Using non-linear excitations with short laser pulses we identify a phonon-coupled state of the condensate that can be understood as a coupling of its electronic Higgs-mode to a low frequency phonon. The Higgs-mode contribution substantiates the picture of an electronically driven phase transition and characterizes the transient order parameter of the excitonic insulator as a function of temperature and excitation density.

cond-mat.str-el↗

arXiv2014

Charge-order fluctuations and superconductivity in two-dimensional organic metals

We report comprehensive Raman and infrared investigations of charge-order (CO) fluctuations in the organic metal $β^{\prime\prime}$-(BEDT-TTF)$_2$SF$_5$CHFSO$_3$ and superconductor $β^{\prime\prime}$-(BEDT-TTF)$_2$SF$_5$CH$_2$CF$_2$SO$_3$. The charge-sensitive vibrational bands have been analyzed through an extension of the well-known Kubo model for the spectral signatures of an equilibrium between two states. At room temperature, both salts exhibit charge fluctuations between two differently charged molecular states with an exchange frequency of about $6\times10^{11} {\rm s}^{-1}$. The exchange rate of the metallic salt remains roughly constant down to 10 K, while in the superconductor the exchange velocity starts to decrease below 200 K, and a "frozen" charge-ordered state emerges, and coexists with the charge-order fluctuation state down to the superconducting temperature. These findings are confronted with other existing spectroscopic experiments, and a tentative phase diagram is proposed for the $β^{\prime\prime}$ BEDT-TTF quarter-filled salts.

cond-mat.supr-con↗

arXiv2011

Nonlinear phononics: A new ultrafast route to lattice control

To date, two types of coupling between electromagnetic radiation and a crystal lattice have been identified experimentally. One is direct, for infrared (IR)-active vibrations that carry an electric dipole. The second is indirect, it occurs through intermediate excitation of the electronic system via electron-phonon coupling, as in stimulated Raman scattering. Nearly 40 years ago, proposals were made of a third path, referred to as ionic Raman scattering (IRS). It was posited that excitation of an IR-active phonon could serve as the intermediate state for a Raman scattering process relying on lattice anharmonicity as opposed to electron phonon interaction. In this paper, we report an experimental demonstration of ionic Raman scattering and show that this mechanism is relevant to optical control in solids. The key insight is that a rectified phonon field can exert a directional force onto the crystal, inducing an abrupt displacement of the atoms from the equilibrium positions that could not be achieved through excitation of an IR-active vibration alone, for which the force is oscillatory. IRS opens up a new direction for the coherent control of solids in their electronic ground state, different from approaches that rely on electronic excitations.

cond-mat.other↗