arXiv subjects

R. Hackl

Publications and source records attributed to R. Hackl.

At least 19 recordsLinked to original sources

arXiv2024

Chiral electronic excitations and strong electron-phonon coupling to Weyl fermions in the Kagome semimetal Co$_3$Sn$_2$S$_2$

We present results of a Raman scattering study of the Kagome ferromagnet Co$_3$Sn$_2$S$_2$, with a focus on electronic and phononic excitations and their interplay. We provide a theoretical analysis of the electronic band structure, enabling a semi-quantitative explanation of the spectra. A prominent feature in the electronic spectra is a redistribution of spectral weight from low to high energies in all polarization configurations starting at the Curie temperature T$_C$. In the symmetry-resolved spectra, the suppression of the A$_{1g}$ continuum in the ferromagnetic state arises from the redistribution of electronic states below T$_C$, while a strong enhancement of the A$_{2g}$ continuum is linked to the dynamics of fermions near the Fermi level $E_{\rm F}$ being characterized by spin-momentum locking near Weyl points. The A$_{1g}$ phonon modulates the position of these Weyl points and couples strongly to the related fermions close to $E_{\rm F}$. These results allow a comprehensive understanding of the bulk band structure evolution as a function of temperature in Co$_3$Sn$_2$S$_2$, offering key insights for further studies of the driving force behind the long-range magnetic order and novel topological states in this compound.

cond-mat.str-el↗

arXiv2022

Evolution of lattice, spin, and charge properties across the phase diagram of FeSe$_{1-x}$S$_x$

A Raman scattering study covering the entire substitution range of the FeSe$_{1-x}$S$_x$ solid solution is presented. Data were taken as a function of sulfur concentration $x$ for $0\le x \le 1$, of temperature and of scattering symmetry. All type of excitations including phonons, spins and charges are analyzed in detail. It is observed that the energy and width of iron-related B$_{1g}$ phonon mode vary continuously across the entire range of sulfur substitution. The A$_{1g}$ chalcogenide mode disappears above $x=0.23$ and reappears at a much higher energy for $x=0.69$. In a similar way the spectral features appearing at finite doping in A$_{1g}$ symmetry vary discontinuously. The magnetic excitation centered at approximately 500 cm$^{-1}$ disappears above $x=0.23$ where the A$_{1g}$ lattice excitations exhibit a discontinuous change in energy. The low-energy mode associated with fluctuations displays maximal intensity at the nemato-structural transition and thus tracks the phase boundary.

cond-mat.supr-con↗

arXiv2021

Probing charge density wave phases and the Mott transition in $1T$-TaS$_2$ by inelastic light scattering

We present a polarization-resolved, high-resolution Raman scattering study of the three consecutive charge density wave (CDW) regimes in $1T$-TaS$_2$ single crystals, supported by \textit{ab initio} calculations. Our analysis of the spectra within the low-temperature commensurate (C-CDW) regime shows $\mathrm{P3}$ symmetry of the system, thus excluding the previously proposed triclinic stacking of the "star-of-David" structure, and promoting trigonal or hexagonal stacking instead. The spectra of the high-temperature incommensurate (IC-CDW) phase directly project the phonon density of states due to the breaking of the translational invariance, supplemented by sizeable electron-phonon coupling. Between 200 and 352\,K, our Raman spectra show contributions from both the IC-CDW and the C-CDW phase, indicating their coexistence in the so-called nearly-commensurate (NC-CDW) phase. The temperature-dependence of the symmetry-resolved Raman conductivity indicates the stepwise reduction of the density of states in the CDW phases, followed by a Mott transition within the C-CDW phase. We determine the size of the Mott gap to be $\Omega_{\rm gap}\approx 170-190$ meV, and track its temperature dependence.

cond-mat.str-el↗

arXiv2020

Calculation of an enhanced A1g symmetry mode induced by Higgs oscillations in the Raman spectrum of high-temperature cuprate superconductors

In superconductors the Anderson-Higgs mechanism allows for the existence of a collective amplitude (Higgs) mode which can couple to eV-light mainly in a non-linear Raman-like process. The experimental non-equilibrium results on isotropic superconductors have been explained going beyond the BCS theory including the Higgs mode. Furthermore, in anisotropic d-wave superconductors strong interaction effects with other modes are expected. Here we calculate the Raman contribution of the Higgs mode from a new perspective, including many-body Higgs oscillations effects and their consequences in conventional, spontaneous Raman spectroscopy. Our results suggest a significant contribution to the intensity of the A1g symmetry Raman spectrum in d-wave superconductors. In order to test our theory, we predict the presence of measurable characteristic oscillations in THz quench-optical probe time-dependent reflectivity experiments.

cond-mat.supr-con↗

arXiv2019

Measuring the imaginary time dynamics of quantum materials

Theoretical analysis typically involves imaginary-time correlation functions. Inferring real-time dynamical response functions from this information is notoriously difficult. However, as we articulate here, it is straightforward to compute imaginary-time correlators from the measured frequency dependence of (real-time) response functions. In addition to facilitating comparison between theory and experiment, the proposed approach can be useful in extracting certain aspects of the (long-time relaxational) dynamics from a complex data set. We illustrate this with an analysis of the nematic response inferred from Raman scattering spectroscopy on the iron-based superconductor Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$, which includes a new method for identifying a putative quantum critical contribution to that response.

cond-mat.str-el↗

arXiv2018

Interplay of lattice, electronic and spin degrees of freedom in detwinned BaFe$_{2}$As$_{2}$: a Raman scattering study

We report results of Raman scattering experiments on twin-free BaFe$_{2}$As$_{2}$ with the main focus placed on understanding the influence of electronic and spin degrees of freedom on the lattice dynamics. In particular, we scrutinize the $E_g$ modes and the As $A_{1g}$ mode. Each of the two $E_g$ phonons in the tetragonal phase is observed to split into a $B_{2g}$ and a $B_{3g}$ mode upon entering the orthorhombic stripe-magnetic phase. The splitting amounts to approximately 10\,cm$^{-1}$ and less than 5\,cm$^{-1}$ for the low- and the high-energy $E_g$ mode, respectively. The detailed study of the fully symmetric As mode using parallel incident and outgoing photon polarizations along either the antiferromagnetic or the ferromagnetic Fe-Fe direction reveals an anisotropic variation of the spectral weight with the energy of the exciting laser indicating a polarization-dependent resonance effect. Along with the experiments we present results from density functional theory calculations of the phonon eigenvectors, the dielectric function, and the Raman tensor elements. The comparison of theory and experiment indicates that (i) orbital-selective electronic correlations are crucial to understand the lattice dynamics and (ii) all phonon anomalies originate predominantly from the magnetic ordering and the corresponding reconstruction of the electronic bands at all energies.

cond-mat.str-el↗

arXiv2017

Phonon anomalies in FeS

We present results from light scattering experiments on tetragonal FeS with the focus placed on lattice dynamics. We identify the Raman active A1g and B1g phonon modes, a second order scattering process involving two acoustic phonons, and contributions from potentially defect-induced scattering. The temperature dependence between 300 and 20K of all observed phonon energies is governed by the lattice contraction. Below 20K the phonon energies increase by 0.5-1 cm$^{-1}$ thus indicating putative short range magnetic order. Along with the experiments we performed lattice-dynamical simulations and a symmetry analysis for the phonons and potential overtones and find good agreement with the experiments. In particular, we argue that the two-phonon excitation observed in a gap between the optical branches becomes observable due to significant electron-phonon interaction.

cond-mat.supr-con↗

arXiv2017

Off-axis parabolic mirror optics for polarized Raman spectroscopy at low temperature

We report the development of a detection optics for the integration of Raman scattering and scanning probe microscopy at low temperature based on a parabolic mirror. In our set-up half of the paraboloid mirror covers a solid angle of $\pi$ corresponding to a numerical aperture of N.A.\,$\approx 0.85$. The optical system can be used for far- and near-field spectroscopy. In the far field the polarizations can be maintained to within 80-90\%. In combination with a scanning microscope (AFM/STM), tunneling or near-field experiments are possible with less than 10\% loss of aperture. Our set-up provides ideal conditions for the future development of tip-enhanced Raman spectroscopy (TERS) at low temperature.

physics.ins-det↗

arXiv2016

Probing the pairing interaction and multiple Bardasis-Schrieffer modes using Raman spectroscopy

In unconventional superconductors, understanding the form of the pairing interaction is the primary goal. In this regard, Raman spectroscopy is a very useful tool, as it identifies the ground state and also the subleading pairing channels by probing collective modes. Here we propose a general theory for multiband Raman response and identify new features in the spectrum that can provide a robust test for a pairing theory. We identify multiple Bardasis-Schrieffer type collective modes and connect the weights of these modes to the sub-leading gap structures within a microscopic pairing theory. The conclusions are completely general, and we apply our approach to interpret the B1g Raman scattering in hole-doped BaFe2As2.

cond-mat.supr-con↗

arXiv2016

Superconductivity and fluctuation in Ba$_{1-p}$K$_p$Fe$_2$As$_2$ and Ba(Fe$_{1-n}$Co$_n$)$_2$As$_2$

We study the interplay of fluctuations and superconductivity in BaFe$_2$As$_2$ (Ba-122) compounds with Ba and Fe substituted by K ($p$ doping) and Co ($n$ doping), respectively. To this end we measured electronic Raman spectra as a function of polarisation and temperature. We observe gap excitations and fluctuations for all doping levels studied. The response from fluctuations is much stronger for Co substitution and, according to the selection rules and the temperature dependence, originates from the exchange of two critical spin fluctuations with characteristic wave vectors $(\pm\pi, 0)$ and $(0,\pm\pi)$. At 22\% K doping ($p=0.22$), we find the same selection rules and spectral shape for the fluctuations but the intensity is smaller by a factor of 5. Since there exists no nematic region above the orthorhombic spin-density-wave (SDW) phase the identification of the fluctuations via the temperature dependence is not possible. The gap excitations in the superconducting state indicate strongly anisotropic near-nodal gaps for Co substitution which make the observation of collective modes difficult. The variation with doping of the spectral weights of the $A_{1g}$ and $B_{1g}$ gap features does not support the influence of fluctuations on Cooper pairing. Therefore, the observation of Bardasis-Schrieffer modes inside the nearly clean gaps on the K-doped side remains the only experimental evidence for the relevance of fluctuations for pairing.

cond-mat.supr-con↗

arXiv2015

Signatures of nematic quantum critical fluctuations in the Raman spectra of lightly doped cuprates

We consider the lightly doped cuprates Y$_{0.97}$Ca$_{0.03}$BaCuO$_{6.05}$ and La$_{2-x}$Sr$_x$CuO$_4$ (with $x=0.02$,0.04), where the presence of a fluctuating nematic state has often been proposed as a precursor of the stripe (or, more generically, charge-density wave) phase, which sets in at higher doping. We phenomenologically assume a quantum critical character for the longitudinal and transverse nematic, and for the charge-ordering fluctuations, and investigate the effects of these fluctuations in Raman spectra. We find that the longitudinal nematic fluctuations peaked at zero transferred momentum account well for the anomalous Raman absorption observed in these systems in the $B_{2g}$ channel, while the absence of such effect in the $B_{1g}$ channel may be due to the overall suppression of Raman response at low frequencies, associated with the pseudogap. While in Y$_{0.97}$Ca$_{0.03}$BaCuO$_{6.05}$ the low-frequency lineshape is fully accounted by longitudinal nematic collective modes alone, in La$_{2-x}$Sr$_x$CuO$_4$ also charge-ordering modes with finite characteristic wavevector are needed to reproduce the shoulders observed in the Raman response. This different involvement of the nearly critical modes in the two materials suggests a different evolution of the nematic state at very low doping into the nearly charge-ordered state at higher doping.

cond-mat.supr-con↗

arXiv2014

A balancing act: Evidence for a strong subdominant d-wave pairing channel in ${\rm Ba_{0.6}K_{0.4}Fe_2As_2}$

We present an analysis of the Raman spectra of optimally doped ${\rm Ba_{0.6}K_{0.4}Fe_2As_2}$ based on LDA band structure calculations and the subsequent estimation of effective Raman vertices. Experimentally a narrow, emergent mode appears in the $B_{1g}$ ($d_{x^2-y^2}$) Raman spectra only below $T_c$, well into the superconducting state and at an energy below twice the energy gap on the electron Fermi surface sheets. The Raman spectra can be reproduced quantitatively with estimates for the magnitude and momentum space structure of the s$_{+-}$ pairing gap on different Fermi surface sheets, as well as the identification of the emergent sharp feature as a Bardasis-Schrieffer exciton, formed as a Cooper pair bound state in a subdominant $d_{x^2-y^2}$ channel. The binding energy of the exciton relative to the gap edge shows that the coupling strength in this subdominant $d_{x^2-y^2}$ channel is as strong as 60% of that in the dominant $s_{+-}$ channel. This result suggests that $d_{x^2-y^2}$ may be the dominant pairing symmetry in Fe-based sperconductors which lack central hole bands.

cond-mat.str-el↗

arXiv2014

A Raman study of the temperature and magnetic field dependence of electronic and lattice properties in MnSi

The temperature and magnetic field dependence of lattice and carrier excitations in MnSi is studied in detail using inelastic light scattering. The pure symmetry components of the electronic response are derived from the polarization dependent spectra. The $E$ and $T_2$ responses agree by and large with longitudinal and optical transport data. However, an anomaly is observed right above the magnetic ordering temperature $T_{\rm C}=29\,{\rm K}$ that is associated with the fluctuations that drive the transition into the helimagnetic phase first order. The $T_1$ spectra, reflecting mostly chiral spin excitations, have a temperature dependence similar to that of the $E$ and $T_2$ symmetries. The response in the fully symmetric $A$ representation has a considerably weaker temperature dependence than that in the other symmetries. All nine Raman active phonon lines can be resolved at low temperature. The positions and line widths of the strongest four lines in $E$ and $T_2$ symmetry are analyzed in the temperature range $4<T<310\,{\rm K}$. Above $50\,{\rm K}$, the temperature dependence is found to be conventional and given by anharmonic phonon decay and the lattice expansion. Distinct anomalies are observed in the range of the helimagnetic transition and in the ordered phase. Applying a magnetic field of $4\,{\rm T}$, well above the critical field, removes all anomalies and restores a conventional behavior highlighting the relationship between the anomalies and magnetism. The anomaly directly above $T_{\rm C}$ in the fluctuation range goes along with an anomaly in the thermal expansion. While the lattice constant changes continuously and has only a kink at $T_{\rm C}$, all optical phonons soften abruptly suggesting a direct microscopic coupling between spin order and optical phonons rather than a reaction to magnetostriction effects.

cond-mat.str-el↗

arXiv2013

Localized states in the Mott insulator \kappa-(BEDT-TTF)_2Cu[N(CN)_2]Cl as probed by photoluminescence

We compare the photoluminescence spectra of the low-temperature Mott insulator \etcl (T_{MIT}=40 K) with spectra of metallic \kappa-(BEDT-TTF)_2Cu[N(CN)_2]Br, which is superconducting below T_c=11.8 K, in the temperature range between 300 and 20 K. In the Mott insulating state of \kappa-(BEDT-TTF)_2Cu[N(CN)_2]Cl we observe a luminescence band at 1.95 eV due to the recombination of an exciton created by a HOMO-LUMO optical excitation. This luminescence is quenched both in the high-temperature bad metal state of \kappa-(BEDT-TTF)_2Cu[N(CN)_2]Cl and in metallic \kappa-(BEDT-TTF)_2Cu[N(CN)_2]Br. The observation of the luminescence of an exciton provides evidence for the local character of excitations in the Mott insulating state.

cond-mat.str-el↗

arXiv2012

Alternative route to charge density wave formation in multiband systems

Charge and spin density waves, periodic modulations of the electron and magnetization densities, respectively, are among the most abundant and non-trivial low-temperature ordered phases in condensed matter. The ordering direction is widely believed to result from the Fermi surface topology. However, several recent studies indicate that this common view needs to be supplemented. Here, we show how an enhanced electron-lattice interaction can contribute to or even determine the selection of the ordering vector in the model charge density wave system ErTe3. Our joint experimental and theoretical study allows us to establish a relation between the selection rules of the electronic light scattering spectra and the enhanced electron-phonon coupling in the vicinity of band degeneracy points. This alternative proposal for charge density wave formation may be of general relevance for driving phase transitions into other broken-symmetry ground states, particularly in multiband systems such as the iron based superconductors.

cond-mat.str-el↗

arXiv2011

Relationship among superconductivity, pseudogap, and high-energy magnetic fluctuations in a model high-Tc superconductor from electronic Raman scattering

We use electronic Raman scattering to study the model single-layer cuprate superconductor HgBa2CuO4+d. In an overdoped sample, we observe a pronounced amplitude enhancement of a high-energy peak related to two-magnon excitations in insulating cuprates upon cooling below the critical temperature Tc. This effect is accompanied by the appearance of the superconducting gap and a pairing peak above the gap in the Raman spectrum, and it can be understood as a consequence of feedback of the Cooper pairing interaction on the high-energy magnetic fluctuations. All of these effects occur already above Tc in two underdoped samples, demonstrating a related feedback mechanism associated with the pseudogap.

cond-mat.supr-con↗

arXiv2011

An Investigation of Particle-Hole Asymmetry in the Cuprates via Electronic Raman Scattering

In this paper we examine the effects of electron-hole asymmetry as a consequence of strong correlations on the electronic Raman scattering in the normal state of copper oxide high temperature superconductors. Using determinant quantum Monte Carlo simulations of the single-band Hubbard model, we construct the electronic Raman response from single particle Green's functions and explore the differences in the spectra for electron and hole doping away from half filling. The theoretical results are compared to new and existing Raman scattering experiments on hole-doped La$_{2-x}$Sr$_{x}$CuO$_{4}$ and electron-doped Nd$_{2-x}$Ce$_{x}$CuO$_{4}$. These findings suggest that the Hubbard model with fixed interaction strength qualitatively captures the doping and temperature dependence of the Raman spectra for both electron and hole doped systems, indicating that the Hubbard parameter U does not need to be doping dependent to capture the essence of this asymmetry.

cond-mat.str-el↗

arXiv2010

Light scattering study of low-energy vibrational excitations in the metallic glass Ni$_{67}$Zr$_{33}$ using electronic Raman scattering

The Raman response of the metallic glass Ni$_{67}$Zr$_{33}$ is measured as a function of polarization and temperature and analyzed theoretically. Unexpectedly, the intensity in the range up to 300\wn increases upon cooling, which is counterintuitive when the response originates from vibrations alone as in insulators. The increase finds a natural explanation if the conduction electrons are assumed to scatter on localized vibrations with a scattering probability proportional to the Debye-Waller factor. None of our assumptions is material specific, and the results are expected to be relevant for disordered systems in general.

cond-mat.dis-nn↗