Search

We report temperature-dependent reflectivity spectra of the layered van der Waals magnet CrSBr in the far-infrared region. Polarization-dependent measurements resolve the vibrational modes along the E$\|a$- and $b$-axes and reveal the clear structural anisotropy. While the $a$-axis phonons notably harden on cooling, the $b$-axis phonon frequencies are almost temperature-independent. A phonon splitting due to the antiferromagnetic phase transition is observed for the 180~cm$^{-1}$ $a$-axis vibrational mode, accompanied by a phonon softening below $T_N$. Furthermore, an additional mode with strong magnetic characteristics at $\sim$360~cm$^{-1}$ is identified and attributed to the magnon excitation of CrSBr., Comment: 6 pages, 3 figures

The properties of kagome metals are governed by the interdependence of band topology and electronic correlations resulting in remarkably rich phase diagrams. Here, we study the temperature evolution of the bulk electronic structure of the antiferromagnetic kagome metal FeGe using infrared spectroscopy. We uncover drastic changes in the low-energy interband absorption at the 100 K structural phase transition that has been linked to a charge-density-wave (CDW) instability. We explain this effect by the minuscule Fe displacement in the kagome plane, which results in parallel bands in the vicinity of the Fermi level. In contrast to conventional CDW materials, however, the spectral weight shifts to low energies, ruling out the opening of a CDW gap in FeGe.

The magneto-optical properties of (001)-oriented NbAs single crystals have been studied in the spectral range from 5 to 150 meV and in magnetic fields of up to 13 T. A rich spectrum of inter-Landau-level transitions is revealed by these measurements. The transitions follow a square-root-like dependence with magnetic field, but the simple linear-band approximation is unable to accurately reproduce the observed behavior of the transitions in applied fields. We argue that the detected magneto-optical spectra should be related to crossing hyperbolic bands, which form the W1 cones. We propose a model Hamiltonian, which describes coupled hyperbolic bands and reproduces the shape of the relevant bands in NbAs. The magneto-optical spectra computed from this Hamiltonian nicely reproduce our observations. We conclude that the hyperbolic-band approach is a minimal model to adequately describe the magneto-optical response of NbAs and that the chiral (conical) bands do not explicitly manifest themselves in the spectra., Comment: 10 pages, SM included

We measured the magneto-reflectivity spectra (4 - 90 meV, 0 - 16 T) of the triple-point semimetal GdPtBi and found them to demonstrate two unusual broad features emerging in field. The electronic bands of GdPtBi are expected to experience large exchange-mediated shifts, which lends itself to a description via effective Zeeman splittings with a large g factor. Based on this approach, along with an ab initio band structure analysis, we propose a model Hamiltonian that describes our observations well and allows us to estimate the effective g factor, g* = 95. We conclude that we directly observe the exchange-induced $\Gamma_{8}$ band inversion in GdPtBi by means of infrared spectroscopy., Comment: 9 pages, SM included

Temperature- and fluence-dependent carrier dynamics of the magnetic Kagome metal Fe$_3$Sn$_2$ were studied using the ultrafast optical pump-probe technique. Two carrier relaxation processes ($\tau_1$ and $\tau_2$) and a laser induced coherent optical phonon were observed. By using the two-temperature model for metals, we ascribe the shorter relaxation $\tau_1$ (~1 ps) to hot electrons transferring their energy to the crystal lattice via electron-phonon scattering. $\tau_2$ (~25 ps), on the other hand, cannot be explained as a conventional process and is attributed to the unconventional (localized) carriers in the material. The observed coherent oscillation is assigned to be a totally symmetric A$_{1g}$ optical phonon dominated by Sn displacements out of the Kagome planes, and possesses a prominently large amplitude, on the order of 10$^{-3}$, comparable to the maximum of the reflectivity change ($\Delta$R/R). This amplitude is equivalent to charge-density-wave (CDW) systems, although no signs of such an instability were hitherto reported in Fe$_3$Sn$_2$. Our results set an unexpected connection between Fe$_3$Sn$_2$ and kagome metals with CDW instabilities, and suggest a unique interplay between phonon and electron dynamics in this compound., Comment: 12 pages, 14 figures

Kagome metals possess peculiar optical spectra consisting of contributions from free charge carriers in a Drude-type response, localized carriers seen as a strongly temperature-dependent localization peak, and, in some cases, phonons displaying strong anomalies. The rare-earth kagome metal series, $R$Mn$_6$Sn$_6$, provides a marvelous playground to study the electronic properties of kagome metals in the presence of variable magnetic order. Here, we report temperature-dependent reflectivity studies on two members of the $R$Mn$_6$Sn$_6$ family, GdMn$_6$Sn$_6$ (in-plane ferrimagnet) and TbMn$_6$Sn$_6$ (out-of-plane ferrimagnet), in a broad energy range (50 - 18000 cm$^{-1}$, equivalent to 6.2 meV - 2.23 eV) down to 10 K. At high temperatures, a phonon mode at approximately 160 cm$^{-1}$ is observed, which becomes screened out in TbMn$_6$Sn$_6$ below $\sim$ 150 K as the localization peak linearly passes through the mode. In GdMn$_6$Sn$_6$, the disappearance of the phonon is accompanied by the onset of saturation of the peak position, suggesting an unusual interplay between the two features., Comment: 7 pages, 3 figures

Temperature-dependent reflectivity studies on the non-magnetic kagome metal RbV$_3$Sb$_5$ in a broad energy range (50 cm$^{-1}$ $-$ 20000 cm$^{-1}$, equivalent to 6 meV $-$ 2.5 eV) down to 10 K are reported. Below $T_{\rm CDW}=102$ K, the optical spectra demonstrate a prominent spectral-weight transfer from low to higher energies as the fingerprint of the charge-density wave (CDW) formation with the opening of a partial gap. A detailed analysis reveals two energy scales of, respectively, $\sim$ 800 cm$^{-1}$ (100 meV) and 360 cm$^{-1}$ (45 meV), the latter visible below 50 K only. Additionally, two modes at, respectively, 160 cm$^{-1}$ (20 meV) and 430 cm$^{-1}$ (53 meV) can be traced both above and below $T_{\rm CDW}$. They show strong anomalies already above $T_{\rm CDW}$ with a further renormalization across the transition, suggesting the importance of the electron-phonon coupling in RbV$_3$Sb$_5$ in both normal and CDW states. While the 160 cm$^{-1}$ mode can be attributed to the E$_{1u}$ phonon, the 430 cm$^{-1}$ mode could not be reproduced in our phonon calculations. The antiresonance nature of this mode suggests a nontrivial electron-phonon coupling in RbV$_3$Sb$_5$. A distinct localization peak observed at all temperatures signals damped electron dynamics, whereas the reduced Drude spectral weight manifests moderate deviations from the band picture in RbV$_3$Sb$_5$., Comment: 14 pages, 12 figures

In order to understand the physical properties of the series of organic conductors $\kappa$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]$X$ with $X$ = Cl, Br, and I, not only electronic correlations but also the effect of disorder has to be taken into account. While for Cl- and Br-containing salts the influence of both parameters were investigated and a universal phase diagram was proposed, the position of $\kappa$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]I is still not settled. Here we have conducted transport, infrared, and dielectric measurements on single crystals of the title compound to clarify its electronic state at low temperatures. The correlation strength was determined as $U/W \approx 2.2$; thus this salt is placed deeper in an insulating state compare to the two sister compounds. We found that inherent disorder leads to a Coulomb localized insulating state similar to the moderately x-ray-irradiated $\kappa$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl.

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., Comment: 6 pages, 3 figures, accepted for publication in Phys. Rev. Lett

Temperature-dependent reflectivity measurements on the kagome metal CsV$_3$Sb$_5$ in a broad frequency range of $50-20000$ cm$^{-1}$ down to $T$=10 K are reported. The charge-density wave (CDW) formed below $T_{\rm CDW}$ = 94 K manifests itself in a prominent spectral-weight transfer from low to higher energy regions. The CDW gap of 60-75 meV is observed at the lowest temperature and shows significant deviations from an isotropic BCS-type mean-field behavior. Absorption peaks appear at frequencies as low as 200 cm$^{-1}$ and can be identified with interband transitions according to density-functional calculations. The change in the interband absorption compared to KV$_3$Sb$_5$ reflects the inversion of band saddle points between the K and Cs compounds. Additionally, a broader and strongly temperature-dependent absorption feature is observed below 1000 cm$^{-1}$ and assigned to a displaced Drude peak. It reflects localization effects on charge carriers., Comment: 9 pages, 7 figures

We present an optical conductivity study of the multifold semimetal PdGa, performed in a broad spectral range (100 - 20000 cm-1; 12 meV - 2.5 eV) down to T = 10 K. The conductivity at frequencies below 4000 cm-1 is dominated by free carriers while at higher frequencies interband transitions provide the major contribution. The spectra do not demonstrate a significant temperature evolution: only the intraband part changes as a function of temperature with the plasma frequency remaining constant. The interband contribution to the conductivity exhibits a broad peak at around 5500 cm-1 and increases basically monotonously at frequencies above 9000 cm-1. The band-structure-based computations reproduce these features of the interband conductivity and predict its linear-in-frequency behavior as frequency diminishes., Comment: 7+ pages, published in PRB

Coexisting density-wave and superconducting states along with the large anomalous Hall effect in the absence of local magnetism remain intriguing and enigmatic features of the AV$_3$Sb$_5$ kagome metals (A = K, Rb, Cs). Here, we demonstrate via optical spectroscopy and density-functional calculations that low-energy dynamics of KV$_3$Sb$_5$ is characterized by unconventional localized carriers, which are strongly renormalized across the density-wave transition and indicative of electronic correlations. Strong phonon anomalies are prominent not only below the density-wave transition, but also at high temperatures, suggesting an intricate interplay of phonons with the underlying electronic structure. We further propose the star-of-David and tri-hexagon (inverse star-of-David) configurations for the density-wave order in KV$_3$Sb$_5$. These configurations are strongly reminiscent of $p$-wave states expected in the Hubbard model on the kagome lattice at the filling level of the van Hove singularity. The proximity to this regime should have intriguing and far-reaching implications for the physics of KV$_3$Sb$_5$ and related materials., Comment: Main text + Supplementary

Temperature- and frequency-dependent infrared spectroscopy identifies two contributions to the electronic properties of the magnetic kagome metal Fe$_3$Sn$_2$: two-dimensional Dirac fermions and strongly correlated flat bands. The interband transitions within the linearly dispersing Dirac bands appear as a two-step feature along with a very narrow Drude component due to intraband contribution. Low-lying absorption features indicate flat bands with multiple van Hove singularities. Localized charge carriers are seen as a Drude-peak shifted to finite frequencies. The spectral weight is redistributed when the spins are reoriented at low temperatures; a sharp mode appears suggesting the opening of a gap due to the spin reorientation as the sign of additional Weyl nodes in the system.

The dimer Mott insulator $\kappa$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ can be tuned into a metallic and superconducting state upon applying pressure of 1.5 kbar and more. We have performed dielectric spectroscopy measurements (7 kHz to 5 MHz) on $\kappa$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ single crystals as a function of temperature (down to $T=8$ K) and pressure (up to $p=4$ kbar). At ambient conditions, a relaxor-like dielectric behavior develops below 50 K that shifts toward lower temperatures as the crystal is pressurized. Interestingly, a second peak emerges in $\varepsilon_{1}(T)$ around $T=15$ K, which becomes strongly enhanced with pressure and is attributed to a small volume fraction of metallic puddles in the insulating host phase. When approaching the phase boundary, this peak diverges rapidly reaching $\varepsilon_{1} \approx 10^{5}$. Our dynamical mean-field theory calculations substantiate that the dielectric catastrophe at the Mott transition is not caused by closing the energy gap, but due to the spatial coexistence of correlated metallic and insulating regions. We discuss the percolative nature of the first-order Mott insulator-to-metal transition in all details.

We measured the reflectivity of the multifold semimetal RhSi in a frequency range from 80 to 20000 cm$^{-1}$ (10 meV - 2.5 eV) at temperatures down to 10 K. The optical conductivity, calculated from the reflectivity, is dominated by the free-carrier (Drude) contribution below 1000 cm$^{-1}$ (120 meV) and by interband transitions at higher frequencies. The temperature-induced changes in the spectra are generally weak: only the Drude bands narrow upon cooling, with an unscreened plasma frequency that is constant with temperature at approximately 1.4 eV, in agreement with a weak temperature dependence of the free-carrier concentration determined by Hall measurements. The interband portion of conductivity exhibits two linear-in-frequency regions below 5000 cm$^{-1}$ ($\sim$ 600 meV), a broad flat maximum at around 6000 cm$^{-1}$ (750 meV), and a further increase starting around 10000 cm$^{-1}$ ($\sim$ 1.2 eV). We assign the linear behavior of the interband conductivity to transitions between the linear bands near the band crossing points. Our findings are in accord with the predictions for the low-energy conductivity behavior in multifold semimetals and with earlier computations based on band structure calculations for RhSi., Comment: 7 pages, supplemental material added, figures improved

Broad-band dielectric spectroscopy, heat capacity measurements and molecular dynamic simulations are applied to study excitations of interacting electric dipoles spatially arranged in a network with an inter-dipole distance of 5-10 A. The dipoles with magnitude of 1.85 Debye are represented by single H2O molecules located in voids (0.5 nm size) formed by ions of the crystal lattice of cordierite. We discover emergence of nontrivial disordered paraelectric phase of dipolar system with signs of phase transition below 3 K., Comment: 3 pages, 4 figures

We present a far-infrared magneto-optical study of the gapped nodal-line semimetal ZrSiS in magnetic fields $B$ up to 7 T. The observed field-dependent features, which represent intra- (cyclotron resonance) and interband transitions, develop as $\sqrt{B}$ in increasing field and can be consistently explained within a simple 2D Dirac band model with a gap of 26 meV and an averaged Fermi velocity of $3\times10^{5}$ m/s. This indicates a rather narrow distribution of these parameters along the in-plane portions of the nodal line in the Brillouin zone. A field-induced feature with an energy position that does not depend on $B$ is also detected in the spectra. Possible origins of this feature are discussed., Comment: accepted to Phys. Rev. Research

The most common species in liquid water, next to neutral H$_2$O molecules, are the H$_3$O$^+$ and OH$^-$ ions. In a dynamic picture, their exact concentrations depend on the time scale at which these are probed. Here, using a spectral-weight analysis, we experimentally resolve the fingerprints of the elusive fluctuations-born short-living H$_3$O$^+$, DH$_2$O$^+$, HD$_2$O$^+$, and D$_3$O$^+$ ions in the IR spectra of light (H$_2$O), heavy (D$_2$O), and semi-heavy (HDO) water. We find that short-living ions, with concentrations reaching $\sim 2\%$ of the content of water molecules, coexist with long-living pH-active ions on the picosecond timescale, thus making liquid water an effective ionic liquid in femtochemistry.

The correlation-driven Mott transition is commonly characterized by a drop in resistivity across the insulator-metal phase boundary; yet, the complex permittivity provides a deeper insight into the microscopic nature. We investigate the frequency- and temperature-dependent dielectric response of the Mott insulator $\kappa$-(BEDT-TTF)$_{2}$-Cu$_2$(CN)$_3$ when tuning from a quantum spin liquid into the Fermi-liquid state by applying external pressure and chemical substitution of the donor molecules. At low temperatures the coexistence region at the first-order transition leads to a strong enhancement of the quasi-static dielectric constant $\epsilon_1$ when the effective correlations are tuned through the critical value. Several dynamical regimes are identified around the Mott point and vividly mapped through pronounced permittivity crossovers. All experimental trends are captured by dynamical mean-field theory of the single-band Hubbard model supplemented by percolation theory., Comment: 6 pages, 4 figures

Transport, magnetic and optical investigations on EuRbFe$_4$As$_4$ single crystals evidence that the ferromagnetic ordering of the Eu$^{2+}$ magnetic moments at $T_N=15$ K, below the superconducting transition ($T_c=36$ K), affects superconductivity in a weak but intriguing way. Upon cooling below $T_N$, the zero resistance state is preserved and the superconductivity is affected by the in-plane ferromagnetism mainly at domain boundaries; a perfect diamagnetism is recovered at low temperatures. The infrared conductivity is strongly suppressed in the far-infrared region below $T_c$, associated with the opening of a complete superconducting gap at $2\Delta = 10$ meV. A gap smaller than the weak coupling limit suggests the strong orbital effects or, within a multiband superconductivity scenario, the existence of a larger yet unrevealed gap., Comment: 4 pages, 5 figures

We report a room-temperature optical reflectivity study performed on [112]-oriented Cd$_3$As$_2$ single crystals over a broad energy range under external pressure up to 10 GPa. The abrupt drop of the band dispersion parameter ($z$-parameter) and the interruption of the gradual redshift of the bandgap at $\sim$4~GPa confirms the structural phase transition from a tetragonal to a monoclinic phase in this material. The pressure-induced increase of the overall optical conductivity at low energies and the continuous redshift of the high-energy bands indicate that the system evolves towards a topologically trivial metallic state, although a complete closing of the band gap could not be observed in the studied pressure range. Furthermore, a detailed investigation of the low-pressure regime suggests the possible existence of an intermediate state between 2 and 4~GPa , that might be a precursor of the structural phase transition or due to the lifted degeneracy of the Dirac nodes. Several optical parameters show yet another anomaly at 8~GPa, where low-temperature superconductivity was found in an earlier study., Comment: submitted to PRB

Temperature-dependent reflectivity measurements in the frequency range 85 - 7000 cm$^{-1}$ were performed on BaFe$_2$As$_2$ single crystals under pressure up to $\sim$5 GPa. The corresponding pressure- and temperature-dependent optical conductivity was analyzed with the Drude-Lorentz model to extract the coherent and incoherent contributions. The gradual suppression of the spin-density wave (SDW) state with increasing pressure and the appearance of the superconducting phase coexisting with the SDW phase at 3.6~GPa were observed. At 3.6~GPa, the reflectivity reaches unity below $\sim$95~cm$^{-1}$ indicating the opening of the superconducting gap and shows a full gap tendency at 6 K., Comment: 9 pages, 7 figures, Accepted for a publication in Phys. Rev. B

We measured the temperature dependence of the in-plane polarized reflectivity spectra of twin-free Y$_{1-x}$Ca$_{x}$Ba$_{2}$Cu$_{3}$O$_{7-{\delta}}$ single crystals with different Ca-concentrations (x=0,0.11 and 0.16) from optimally doped to heavily overdoped region. Low energy optical conductivity spectra showed a Drude-like residual conductivity at temperatures far below the superconducting transition temperature, which indicates the presence of unpaired-normal carriers in the superconducting state. Comparing the spectra at a fixed Ca-content or at a fixed doping level, we have revealed that the carrier overdoping increases unpaired carriers in addition to those induced by the Ca-disorder. We also found the superconducting behavior of the one-dimensional CuO chains for the Ca-free samples., Comment: 8 pages, 9 figures