arXiv subjects

C. A. Kuntscher

Publications and source records attributed to C. A. Kuntscher.

At least 19 recordsLinked to original sources

arXiv2026

Charge dynamics in the Weyl semimetals NbIrTe$_4$ and TaIrTe$_4$ under pressure: Signatures of an electronic phase transition

A high-pressure investigation of the Weyl semimetals NbIrTe$_4$ and TaIrTe$_4$ is presented, using infrared spectroscopy supplemented by density functional theory calculations. The experimental optical conductivity spectra as a function of pressure suggest the occurrence of a pressure-induced phase transition at a critical pressure $P_\text{c}=7\text{--}8$ GPa. This transition is most likely electronic in nature, as Raman scattering measurements provide no evidence of a significant structural phase transition. Above $P_\text{c}$ a significant redistribution of spectral weight occurs in the optical conductivity spectrum for both materials. A Drude-Lorentz analysis of the optical data indicates a sharp reduction in the free carrier concentration at $P_\text{c}$, concomitant with the appearance of a low-energy phonon, which was initially screened by free charge carriers. A predominantly electronic origin of the phase transition is supported by the calculated electronic band structure, Fermi surface, and interband optical conductivity as a function of pressure. Our findings provide collective evidence for a pressure-induced, most likely electronic phase transition in both van der Waals materials at $P_\text{c}=7\text{--}8$ GPa, highlighting the tunability of their electronic band structure by hydrostatic pressure.

cond-mat.mtrl-sci↗

arXiv2025

Suppression of magnetism in Co$_3$Sn$_2$S$_2$ under external pressure

The ability to control the magnetic state provides a powerful means to tune the underlying band topology, enabling transitions between distinct electronic phases and the emergence of novel quantum phenomena. In this work, we address the evolution of ferromagnetic state upon applying external pressures up to 10.8~GPa using a combined experimental and theoretical study. The standard \emph{ab initio} Density Functional Theory computation including ionic relaxations grossly overestimates the unit cell magnetization as a function of pressure. In our theoretical analysis we identify two possible mechanisms to remedy this shortcoming. Matching the experimental observations is achieved by a symmetry-preserving adjustment of the sulfur atoms position within the unit cell. Alternatively, we explore various combinations of the exchange and correlation parts of the effective potential which reproduce the experimental magnetization, the structural parameters and the measured optical conductivity spectra. Thus, the pressure-dependent behavior of magnetization demands a careful theoretical treatment and analysis of theoretical and experimental data.

cond-mat.mtrl-sci↗

arXiv2024

Optical conductivity of the metallic pyrochlore iridate Pr$_2$Ir$_2$O$_7$: Influence of spin-orbit coupling and electronic correlations on the electronic structure

The synergy of strong spin-orbit coupling and electron-electron interactions gives rise to unconventional topological states, such as topological Mott insulator, Weyl semimetal, and quantum spin liquid. In this study, we have grown single crystals of the pyrochlore iridate Pr$_2$Ir$_2$O$_7$ and explored its magnetic, lattice dynamical, and electronic properties. While Raman spectroscopy data reveal six phonon modes confirming the cubic \textit{Fd$\bar{3}$m} crystal symmetry, dc magnetic susceptibility data show no anomalies and hence indicate the absence of magnetic phase transitions down to 2~K. Both temperature-dependent electric transport and optical conductivity data reveal the metallic character of Pr$_2$Ir$_2$O$_7$. The optical conductivity spectrum contains a mid-infrared absorption band, which becomes more pronounced with decreasing temperature due to spectral weight transfer from high to low energies. The presence of the mid-infrared band hints at the importance of correlation physics. The optical response furthermore suggests that Pr$_2$Ir$_2$O$_7$ is close to the Weyl semimetal phase.

cond-mat.str-el↗

arXiv2024

Optical study of the charge dynamics evolution in the topological insulators MnBi$_2$Te$_4$ and Mn(Bi$_{0.74}$Sb$_{0.26}$)$_2$Te$_4$ under high pressure

The van der Waals material MnBi$_2$Te$_4$ and the related Sb-substituted compounds Mn(Bi$_{1-x}$Sb$_x$)$_2$Te$_4$ are prominent members of the family of magnetic topological insulators, in which rare quantum mechanical states can be realized. In this work, we study the evolution of the charge dynamics in MnBi$_2$Te$_4$ and the Sb-substituted compound Mn(Bi$_{1-x}$Sb$_x$)$_2$Te$_4$ with $x=0.26$ under hydrostatic pressure. For MnBi$_2$Te$_4$, the pressure dependence of the screened plasma frequency, the dc conductivity, and the reflectance at selected frequencies shows weak anomalies at $\sim$2 and $\sim$4~GPa, which might be related to an electronic phase transition driven by the enhanced interlayer interaction. We observe a pressure-induced decrease in the optical gap, consistent with the decrease in and closing of the energy gap reported in the literature. Both studied materials show an unusual decrease in the low-energy optical conductivity under pressure, which we attribute to a decreasing spectral weight of the Drude terms describing the free charge carrier excitations. Our results suggest a localization of conduction electrons under pressure, possibly due to hybridization effects.

cond-mat.mtrl-sci↗

arXiv2024

Optical signatures of type-II Weyl fermions in the noncentrosymmetric semimetals $R$AlSi ($R$=La, Ce, Pr, Nd, Sm)

Weyl semimetals with magnetic ordering provide a promising platform for the investigation of rare topological effects such as the anomalous Hall effect, resulting from the interplay of nontrivial bands with various spin configurations. The materials $R$AlSi, where $R$ represents a rare-earth element, are prominent representatives of Weyl semimetals, where the Weyl states are induced by space inversion symmetry breaking and in addition, for several rare-earth elements $R$, enhanced by time-reversal symmetry breaking through the formation of a magnetic order at low temperature. We report optical signatures of Weyl fermions in the magnetic compounds CeAlSi, PrAlSi, NdAlSi, and SmAlSi as well as the non-magnetic family member LaAlSi by broad-frequency infrared spectroscopy at room temperature, i.e., in the paramagnetic phase. A similar profile of the optical conductivity spectrum and a metallic character are observed for all compounds, with LaAlSi showing the strongest free charge carrier contribution. Furthermore, the linear-in-frequency behavior of the optical conductivity of all investigated compounds indicates the presence of Weyl nodes in close vicinity of the Fermi energy, resulting from inversion symmetry breaking in noncentrosymmetric structures. According to the characteristics of these linear slopes, the $R$AlSi compounds are expected to host mainly type-II Weyl states with overtilted Weyl cones. The results are compared to the optical response of the closely related $R$AlGe materials, which are considered as potential hybridization-driven Weyl-Kondo systems.

cond-mat.mtrl-sci↗

arXiv2024

Optical anisotropy of the kagome magnet FeSn: Dominant role of excitations between kagome and Sn layers

Antiferromagnetic FeSn is considered to be a close realization of the ideal two-dimensional (2D) kagome lattice, hosting Dirac cones, van Hove singularities, and flat bands, as it comprises Fe$_3$Sn kagome layers well separated by Sn buffer layers. We observe a pronounced optical anisotropy, with the low-energy optical conductivity being surprisingly higher perpendicular to the kagome planes than along the layers. This finding contradicts the prevalent picture of dominantly 2D electronic structure for FeSn. Our material-specific theory reproduces the measured conductivity spectra remarkarbly well. A site-specific decomposition of the optical response to individual excitation channels shows that the optical conductivity for polarizations both parallel and perpendicular to the kagome plane is dominated by interlayer transitions between kagome layers and adjacent Sn-based layers. Moreover, the matrix elements corresponding to these transitions are highly anisotropic, leading to larger out-of-plane conductivity. Our results evidence the crucial role of interstitial layers in charge dynamics even in seemingly 2D systems.

cond-mat.mtrl-sci↗

arXiv2023

Signatures of van Hove singularities in the anisotropic in-plane optical conductivity of the topological semimetal Nb$_3$SiTe$_6$

We present a temperature-dependent infrared spectroscopy study on the layered topological semimetal Nb$_3$SiTe$_6$ combined with density-functional theory (DFT) calculations of the electronic band structure and optical conductivity. Our results reveal an anisotropic behavior of the in-plane ($ac$-plane) optical conductivity, with three pronounced excitations located at around 0.15, 0.28, and 0.41~eV for the polarization of the incident radiation along the $c$ axis. These excitations are well reproduced in the theoretical spectra. Based on the \textit{ab initio} results, the excitations around 0.15 eV and 0.28 eV are interpreted as fingerprints of van Hove singularities in the electronic band structure and compared to the findings for other topological semimetals.

cond-mat.mtrl-sci↗

arXiv2022

Evolution of the optical response of the magnetic topological insulators Mn(Bi$_{1-x}$Sb$_{x}$)$_2$Te$_4$ with Sb content

MnBi$_2$Te$_4$ is a promising representative of intrinsic antiferromagnetic topological insulators, which could enable rare quantum mechanical effects like the quantum anomalous Hall effect. Especially at low temperatures, numerous studies have been reported, demonstrating the great potential of this compound in the magnetically ordered state below $T_{\mathrm{N}}$. Among recent findings, the alloy compound Mn(Bi$_{1-x}$Sb$_x$)$_2$Te$_4$ has been suggested to be an interesting candidate for the realization of an ideal Weyl semimetal state. By exchanging Bi by Sb, the electronic structure is influenced in terms of a shift of the Fermi energy, and a decrease in the energy gap has been predicted. In this work, we investigate and compare the optical conductivity of Mn(Bi$_{1-x}$Sb$_x$)$_2$Te$_4$ single crystals with various Sb doping levels $x$ by infrared reflectivity measurements. We observe a big impact of the Sb content on the low-energy excitations characterizing the metallic state of our samples. Different $x$=0.26 crystals show significant differences in their optical response and also a strong position dependence. The findings are compared to the recently reported optical conductivity spectrum of the pure compound MnBi$_2$Te$_4$.

cond-mat.str-el↗

arXiv2022

Fluorite-related iridate Pr$_3$IrO$_7$: Crystal growth, structure, magnetism, thermodynamic, and optical properties

Spin-orbit coupling in heavy 5$d$ metal oxides, in particular, iridates have received tremendous interest in recent years due to the realization of exotic electronic and magnetic phases. Here, we report the synthesis, structural, magnetic, thermodynamic, and optical properties of the ternary iridate Pr$_3$IrO$_7$. Single crystals of Pr$_3$IrO$_7$ have been grown by the KF flux method. Structural analysis shows that Pr$_3$IrO$_7$ crystallizes in an orthorhombic phase with $Cmcm$ symmetry. The electron energy loss spectroscopy study indicates that Pr is in a 3+ valence state, which implies a 5+ oxidation state of Ir. Magnetization data measured at high and low magnetic fields do not exhibit any bifurcation between $M_{ZFC}$ and $M_{FC}$, however, a weak hump in $M(T)$ is observed at $T^*$$\sim$10.4~K. The specific heat data reveal two maxima at $\sim$253 K and $\sim$4.8 K. The optical conductivity $σ_1(ω)$ spectrum shows 24 infrared-active phonon modes and reveals an insulating behavior with an optical gap $Δ_{OP}$ of size $\sim$500~meV. During cooling down, the temperature-dependent reflectivity spectrum reveals eight extra phonon modes below the structural phase transition ($\sim$ 253 K). An anomaly is observed at around $T^*$ in the temperature evolution of infrared-active mode frequencies suggesting the presence of significant spin-phonon coupling in the system.

cond-mat.str-el↗

arXiv2022

In-plane and out-of-plane optical response of the nodal-line semimetals ZrGeS and ZrGeSe

Polarization-dependent reflectivity measurements were carried out over a broad frequency range on single-crystalline ZrGeSe and ZrGeS compounds, which are closely related to the prototype nodal-line semimetal ZrSiS. These measurements revealed the strongly anisotropic character of both ZrGeSe and ZrGeS, with a reduced plasma frequency for the out-of-plane direction {\bf E}$\| c$ as compared to the in-plane direction {\bf E}$\| ab$. For {\bf E}$\| ab$ the optical conductivity spectrum consists of two Drude terms followed by a shoulder or plateau-like behavior and a distinct U shape at higher energies, while for {\bf E}$\| c$ one Drude term is followed by a peak-like behavior and the U shape of the profile is less developed. Under external pressure, two prominent excitations appear in the out-of-plane optical conductivity spectrum of ZrGeSe, whose frequency position and oscillator strength show a weak anomaly at $\sim$3~GPa. Overall, the pressure-induced changes in the profile of the {\bf E}$\| c$ conductivity spectrum are much enhanced above $\sim$3~GPa. We compare our results to those recently reported for ZrSiS in a quantitative manner.

cond-mat.mtrl-sci↗

arXiv2022

Infrared study of the layered, magnetic insulator Mn(Bi$_{0.07}$Sb$_{0.93}$)$_2$Te$_4$ at low temperatures

Topological insulators with intrinsic magnetic ordering, potentially hosting rare quantum effects, recently attracted extensive attention. MnBi$_2$Te$_4$ is the first established example. The Sb-doped variant Mn(Bi$_{1-x}$Sb$_x$)$_2$Te$_4$ shows a great variety of electronic properties depending on the Sb content~$x$, such as shifts in the Fermi level and the Neel temperature $T_{\mathrm N}$, and the change of the free charge carrier type from $n$- to $p$-type at high Sb substitution ratios. Here, we investigate the effect of magnetic ordering on the bulk electronic structure of Mn(Bi$_{1-x}$Sb$_x$)$_2$Te$_4$ with high Sb content $x=0.93$ by temperature-dependent reflectivity measurements over a broad frequency range. We observe anomalies in the optical response across $T_{\mathrm N}$ when the antiferromagnetic order sets, which suggests a coupling between the magnetic ordering and the electronic structure of the material.

cond-mat.mtrl-sci↗

arXiv2022

Magneto-optical detection of topological contributions to the anomalous Hall effect in a kagome ferromagnet

A single ferromagnetic kagome layer is predicted to realize a Chern insulator with quantized Hall conductance, which upon stacking can become a Weyl-semimetal with large anomalous Hall effect (AHE) and magneto-optical activity. Indeed, in the kagome bilayer material Fe$_3$Sn$_2$, a large AHE was detected, however, it still awaits the direct probing of the responsible band structure features by bulk sensitive methods. We measure the optical, both diagonal and Hall, conductivity spectra over a broad spectral range and identify the origin of the intrinsic AHE with the help of momentum- and band-decomposed first-principles calculations. We find that low-energy transitions, tracing "helical volumes" in momentum space reminiscent of the formerly predicted helical nodal lines, substantially contribute to the AHE, which is further increased by contributions from multiple higher-energy interband transitions. Our study also reveals that local Coulomb interactions lead to band reconstructions near the Fermi level.

cond-mat.str-el↗

arXiv2021

Pressure-induced excitations in the out-of-plane optical response of the nodal-line semimetal ZrSiS

The anisotropic optical response of the layered, nodal-line semimetal ZrSiS at ambient and high pressure is investigated by frequency-dependent reflectivity measurements for the polarization along and perpendicular to the layers. The highly anisotropic optical conductivity is in very good agreement with results from density functional theory calculations and confirms the anisotropic character of ZrSiS. Whereas the in-plane optical conductivity shows only modest pressure-induced changes, we found strong effects on the out-of-plane optical conductivity spectrum of ZrSiS, with the appearance of two prominent excitations. These pronounced pressure-induced effects can neither be attributed to a structural phase transition according to our single-crystal x-ray diffraction measurements, nor can they be explained by electronic correlation and electron-hole pairing effects, as revealed by theoretical calculations. Our findings are discussed in the context of the recently proposed excitonic insulator phase in ZrSiS.

cond-mat.mtrl-sci↗

arXiv2020

Optical conductivity of the type-II Weyl semimetal WTe$_2$ under pressure

Tungsten ditelluride WTe$_2$ is a type-II Weyl semimetal with electronic properties highly sensitive to external pressure, as demonstrated by the superconductivity emerging under pressure. Here, we study the optical conductivity of the type-II Weyl semimetal WTe$_2$ under external pressure at room temperature. With increasing pressure, a pronounced spectral weight transfer occurs from the high-energy to the low-energy interband transitions, with drastic changes in the profile of the optical conductivity spectrum indicating a high sensitivity of the electronic band structure to external pressure. The detailed analysis of the pressure-dependent optical conductivity furthermore reveals anomalies at the pressures $\sim$2 and $\sim$4.5~GPa, where an electronic and a structural phase transition, respectively, were reported in the literature.

cond-mat.mtrl-sci↗

arXiv2020

Influence of magnetic ordering on the optical response of the antiferromagnetic topological insulator MnBi$_2$Te$_4$

The layered topological insulator MnBi$_2$Te$_4$ has attracted great interest recently due to its intrinsic antiferromagnetic order, potentially hosting various topological phases. By temperature-dependent infrared spectroscopy over a broad frequency range, we studied the changes in the optical conductivity of MnBi$_2$Te$_4$ at the magnetic ordering temperature. The temperature dependence of several optical parameters reveals an anomaly at the magnetic phase transition, which suggests the correlation between the bulk electronic band structure and the magnetism. We relate our findings to recent reports on the temperature dependence of the electronic band structure of MnBi$_2$Te$_4$.

cond-mat.mtrl-sci↗

arXiv2020

Lattice dynamics and electronic excitations in a large family of lacunar spinels with a breathing pyrochlore lattice structure

Reproducing the electronic structure of AM$_4$X$_8$ lacunar spinels with a breathing pyrochlore lattice is a great theoretical challenge due to the interplay of various factors. The character of the M$_4$X$_4$ cluster orbitals is critically influenced by the Jahn-Teller instability, the spin-orbit interaction, and also by the magnetic state of the clusters. Consequently, to reproduce the narrow-gap semiconducting nature of these moderately correlated materials requires advanced approaches, since the strength of the inter-cluster hopping is strongly affected by the character of the cluster orbitals. In order to provide a solid experimental basis for theoretical studies, we performed broadband optical spectroscopy on a large set of lacunar spinels, with systematically changing ions at the A and M sites as well as the ligand (A=Ga, Ge, Al; M=V, Mo, Nb, Ta; X=S, Se). Our study covers the range of phonon excitations and also electronic transitions near the gap edge. In the phonon excitation spectrum a limited subset of the symmetry allowed modes is observed in the cubic state, with a few additional modes emerging upon the symmetry-lowering structural transition. All the infrared active modes are assigned to vibrations of the ligands and ions at the A sites, with no obvious contribution from the M-site ions. Concerning the electronic states, we found that all compounds are narrow-gap semiconductors ($E_\mathrm{g} = 130 - 350\,$meV) already in their room-temperature cubic state and their structural transitions induce weak, if any, changes in the band gap. The gap value is decreased when substituting S with Se and also when replacing $3d$ ions by $4d$ or $5d$ ions at the M sites.

cond-mat.str-el↗

arXiv2020

Indications for Lifshitz transitions in the nodal-line semimetal ZrSiTe induced by interlayer interaction

The layered material ZrSiTe is currently extensively investigated as a nodal-line semimetal with Dirac-like band crossings protected by nonsymmorphic symmetry close to the Fermi energy. A recent infrared spectroscopy study on ZrSiTe under external pressure found anomalies in the optical response, providing hints for pressure-induced phase transitions at $\approx$4.1 and $\approx$6.5 GPa. By pressure-dependent Raman spectroscopy and x-ray diffraction measurements combined with electronic band structure calculations we find indications for two pressure-induced Lifshitz transitions with major changes in the Fermi surface topology in the absence of lattice symmetry changes. These electronic phase transitions can be attributed to the enhanced interlayer interaction induced by external pressure. Our findings demonstrate the crucial role of the interlayer distance for the electronic properties of layered van der Waals topological materials.

cond-mat.mtrl-sci↗

arXiv2019

Optical spectroscopy on the photo-response in multiferroic BiFeO$_3$ at high pressure

The pressure dependence of light-induced effects in single-crystalline BiFeO$_3$ is studied by optical spectroscopy. At low pressures, we observe three light-induced absorption features with energies just below the two crystal field excitations and the absorption onset, respectively. These absorption features were previously ascribed to excitons, possibly connected with the ultra-fast photostriction effect in BiFeO$_3$. The pressure-induced redshift of the absorption features follows the pressure dependence of the corresponding crystal field excitations and absorption onset, suggesting the link between them. Above the structural phase transition at $P_{\mathrm{c1}}\approx{}3.5$ GPa the three absorption features disappear, suggesting their connection to the polar phase in BiFeO$_3$. The pressure-induced disappearance of the photo-induced features is irreversible upon pressure release.

cond-mat.mtrl-sci↗