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C. Shekhar

Publications and source records attributed to C. Shekhar.

At least 19 recordsLinked to original sources

Symmetry-Selective Stabilization of Charge-Density Wave in ScV$_6$Sn$_6$

Charge-density-wave (CDW) order in kagome metals is highly sensitive to external tuning parameters such as chemical substitution and hydrostatic pressure, which generally suppress long-range order. Here, using high-resolution X-ray diffraction under controlled uniaxial strain, we show that anisotropic lattice deformation instead stabilizes and enhances the CDW state in ScV$_6$Sn$_6$. Compression along the [H00] and [HH0] directions lowers the crystal symmetry from hexagonal to orthorhombic, lifts the degeneracy between symmetry-equivalent in-plane CDW domains, and promotes long-range order while preserving the underlying trimer instability. Phonon calculations indicate only a moderate stabilization of the imaginary flat phonon mode, demonstrating that the increase in T$_\mathrm{CDW}$ is primarily driven by the in-plane ordering of the Sn$^\mathrm{T}$--Sc--Sn$^\mathrm{T}$ \textit{rattling} chains within the frustrated kagome lattice. A phenomenological model incorporating strain-dependent Ising couplings within a three-state Potts framework successfully reproduces the evolution of T$_\mathrm{CDW}$ under compression and captures the continuous nature of the transition. Our results establish uniaxial strain as a powerful symmetry-selective tuning parameter for order-disorder transformations in frustrated lattices.

cond-mat.str-el

Revealing magnetism in the distorted kagome $R$Ti$_3$Bi$_4$ ($R$ = Nd, Sm, Gd) via ARPES and XMCD

Kagome materials are known for hosting emergent quantum phenomena driven by the interaction between different lattice, charge and spin orders. Here, we present a detailed angle resolved photoemission (ARPES), density functional theory (DFT) and x-ray magnetic circular dichroism (XMCD) study of the electronic and magnetic structure of $R$Ti$_3$Bi$_4$ ($R$ = Nd, Sm, Gd). ARPES and DFT demonstrate that the bulk electronic band structure is dominated by the hybridization of the Ti bands, and the weak electron-like pocket at $\Gamma$ is identified as a surface state. The isotropic XAS profile of the $M_{4,5}$-edge of the rare earth is consistent with the presence of $R^{3+}$ oxidation state. Using the XMCD sum rules, backed by the atomic multiplet theory calculations, we obtain the spin and orbital magnetic moments. The Ti $L_{2,3}$-edge XMCD reveals the presence of a small magnetic moment in GdTi$_3$Bi$_4$, presumably driven by the proximity of the {Ti} kagome layers to the $zigzag$ chains of Gd, while the total magnetic moment of Gd is shared by the $f$ and $d$ electrons. Our combined XMCD, ARPES and DFT study brings an important piece of information to understand the spin flip transitions and anomalous Hall effect observed in the $R$Ti$_3$Bi$_4$ kagome metals.

cond-mat.mtrl-sci

Structural and magnetic phases of topological kagome metal Fe$_3$Sn$_2$ under pressure

We investigate the pressure-induced evolution of crystal structure and magnetism in the kagome ferromagnet Fe$_3$Sn$_2$ by combining X-ray diffraction, X-ray Emission Spectroscopy, X-ray Magnetic Circular Dichroism, and spin-polarized density functional theory calculations. X-ray diffraction reveals a structural phase transition above $\sim$20~GPa, which coincides with a pronounced reduction of the local Fe magnetic moment evidenced by X-ray emission spectroscopy, indicating a high-spin to low-spin transition. While XES probes the amplitude of the local moment, XMCD provides direct information on the orientation of the ordered magnetic moments and uncovers a rich pressure--temperature magnetic phase diagram. At room temperature, a collinear ferromagnetic phase with moments aligned along the $c$ axis persists up to the structural transition. At low temperature, a tilted magnetic configuration remains stable to significantly higher pressures, while at intermediate temperatures pressure stabilizes the low-temperature magnetic phase at the expense of the high-temperature one. Spin-polarized first-principles calculations show that, although isotropic ferromagnetic exchange interactions remain robust under compression, pressure enhances spin--orbit--driven magnetic anisotropy and Dzyaloshinskii--Moriya interactions, favoring non-collinear magnetic configurations. Our results demonstrate that pressure reshapes the magnetic energy landscape of Fe$_3$Sn$_2$ by coupling lattice, spin state, and relativistic magnetic interactions, establishing hydrostatic pressure as an effective control parameter to engineer magnetic anisotropy and potentially topological phases in kagome materials.

cond-mat.str-el

Emergent Spin-Singlet Pairing in the Frustrated Kagome Metal Sc$_3$Mn$_3$Al$_7$Si$_5$

The metallic kagome compound Sc$_3$Mn$_3$Al$_7$Si$_5$ has attracted attention as a candidate platform where geometric frustration and itinerant electrons may cooperate to stabilize a quantum-disordered magnetic ground state. Here, we combine bulk thermodynamic probes, low-noise FIB-device transport, and comprehensive $^{55}$Mn Nuclear Magnetic Resonance (NMR) measurements to elucidate the low-temperature spin dynamics of this system. The bulk data reveal strongly reduced magnetic entropy, a negative magnetoresistance arising from spin scattering, and field-dependent transport indicates the spin fluctuations, while showing no signatures of long-range magnetic order. NMR provides a direct local view of the correlated Mn moments: the nuclear spin-spin relaxation $T_2$ exhibits a pronounced low-temperature enhancement driven by an indirect internuclear coupling through electronic spin fluctuations, whose temperature and distance dependence point to partially gapped low-energy spin excitations. The spin-lattice relaxation rate $T_1^{-1}$ displays a Hebel-Slichter-like coherence peak near \SI{10}{K}, coincident with the resistivity crossover and a subtle heat-capacity anomaly, indicating the formation of short-range spin-singlet correlations. Together, our results demonstrate that Sc$_3$Mn$_3$Al$_7$Si$_5$ hosts an unconventional correlated state dominated by frustrated, gapped spin dynamics, placing it among the rare metallic kagome systems proximate to a quantum spin liquid.

cond-mat.str-el

Unravelling disorder in kagome Yb$_{0.5}$Co$_3$Ge$_3$

The presence of phonon instabilities that leads to the formation of charge modulated states in kagome metals has allowed their classification based on the atomic displacements. Here, we use diffuse and inelastic x-ray scattering, backed by Monte Carlo simulations to describe a type-I instability in the kagome metal Yb$_{0.5}$Co$_3$Ge$_3$. We find that the in-plane distortion of Co in the kagome plane drives a structural transition with the appearance of new Bragg peaks at odd $L$, which are surrounded by a hexagonal diffuse signal. The anisotropic diffuse scattering, characteristic of a highly frustrated triangular lattice was simulated following a combination of Ising hamiltonian and Lennard-Jones potential, and demonstrate that the structural phase transition in Yb$_{0.5}$Co$_3$Ge$_3$ is of an order-disorder transformation type. The inelastic spectra reveals no softening but an anomalous broadening of the $\Gamma-A$ low energy acoustic mode. Our results highlight the critical role of the geometric frustration in promoting ordering from disorder in kagome lattices and power of diffuse scattering to disentangle the internal atomic displacements and correlated disorder.

cond-mat.str-el

Interlayer charge transfer induced by electronic instabilities in the natural van der Waals hetrostructure 4H$_b$-TaS$_2$

The natural van der Waals heterostructure 4H$_b$-TaS$_2$ composed of alternating 1T- and 1H-TaS$_2$ layers serves as a platform for investigating the electronic correlations and layer-dependent properties of novel quantum materials. The temperature evolution of the conductivity spectra $\sigma(\omega)$ obtained through infrared spectroscopy elucidates the influence of band modifications associated with the charge-density-wave (CDW) superlattice on the 1T layer, resulting in a room-temperature energy gap, $\Delta_{\rm CDW}\approx$ 0.35 eV. However, there is no gap associated to the 1H layer. Supported by density functional theory calculations, we attribute the behavior of interband transitions to the convergence of the layers, which amplifies the charge transfer from the 1T to the 1H layers, progressing as the temperature decreases. This phenomenon leads to an enhanced low-energy spectral weight and carrier density. The presence of an energy gap and the temperature-tunable charge transfer within the bulk of 4H$_b$-TaS$_2$ driven by layer-dependent CDW states contribute to a more comprehensive understanding of other complex compounds of transition-metal dichalcogenides.

cond-mat.mes-hall

Cascade of pressure induced competing CDWs in the kagome metal FeGe

Electronic ordering is prevalent in correlated systems, which commonly exhibit competing interactions. Here, we use x-ray diffraction to demonstrate a cascade of pressure induced order-disorder transformations, with propagation vectors $\mathbf{q}_\mathrm{CDW}$= $\left(\frac{1}{2}\ 0\ \frac{1}{2}\right)$, $\mathbf{q}^*$=$\left(\frac{1}{3}\ \frac{1}{3}\ \frac{1}{2}\right)$ and $\mathbf{q}^\dagger$=$\left(\frac{1}{3}\ \frac{1}{3}\ \frac{1}{3}\right)$, in the kagome metal FeGe. In the pressure interval between 4$<p<$10 GPa, $\mathbf{q}_\mathrm{CDW}$ and $\mathbf{q}^*$ coexist and the spatial extent of the $\sqrt{3}\times\sqrt{3}$ order is nearly long-range at $\sim$15 GPa, $\sim$30 unit cells. Above $\sim$25 GPa, the periodic lattice distortion has a propagation wavevector of $\mathbf{q}^\dagger$=$\left(\frac{1}{3}\ \frac{1}{3}\ \frac{1}{3}\right)$ at room temperature. The cascade of phase transitions are captured by the Ising model of frustrated triangular lattices and modeled by Monte Carlo simulations based on the dimerization of trigonal Ge$_1$. The pressure dependence of the integrated intensities and correlation lengths of $\mathbf{q}_\mathrm{CDW}$, $\mathbf{q}^*$ and $\mathbf{q}^\dagger$ demonstrate a competition between the 2$\times$2 and $\sqrt{3}\times\sqrt{3}$ phases prove the tunability of order-disorder phase transitions under pressure and the rich landscape of metastable/fragile phases of FeGe.

cond-mat.str-el

Frustrated charge density wave and quasi-long-range bond-orientational order in the magnetic kagome FeGe

The intrinsic frustrated nature of a kagome lattice is amenable to the realization of exotic phases of matter, such as quantum spin liquids or spin ices, and more recently the multiple-$\mathrm{\textbf{q}}$ charge density waves (CDW) in the kagome metals. Despite intense efforts to understand the mechanism driving the electronic modulations, its origin is still unknown and hindered by competing interactions and intertwined orders. Here, we identify a dimerization-driven 2D hexagonal charge-diffuse precursor in the antiferromagnetic kagome metal FeGe and demonstrate that the fraction of dimerized/undimerized states is the relevant order parameter of the multiple-$\mathrm{\textbf{q}}$ CDW of a continuous phase transition. The pretransitional charge fluctuations with propagation vector $\mathrm{\textbf{q}=\textbf{q}_M}$ at T$_{\mathrm{CDW}}$$<$T$<$T$^*$(125 K) are anisotropic, hence holding a quasi-long-range bond-orientational order. The broken translational symmetry emerges from the anisotropic diffuse precursor, akin to the Ising scenario of antiferromagnetic triangular lattices. The temperature and momentum dependence of the critical scattering show parallels to the stacked hexatic $\mathrm{B}$-phases reported in liquid crystals and transient states of CDWs and highlight the key role of the topological defect-mediated melting of the CDW in FeGe.

cond-mat.str-el

Pressure-dependent Electronic Superlattice in the Kagome-Superconductor CsV$_3$Sb$_5$

We present a high-resolution single crystal x-ray diffraction study of kagome-superconductor \cvs, exploring its response to variations in pressure and temperature. We discover that at low temperatures, the structural modulations of the electronic superlattice, commonly associated with charge-density-wave order, undergo a transformation around $p \sim$ 0.7 GPa from the familiar $2\times2$ pattern to a long-range-ordered modulation at wavevector $q=(0, 3/8, 1/2)$. Our observations align with inferred changes in the CDW pattern from prior transport and nuclear-magnetic-resonance studies, providing new insights into these transitions. Interestingly, the pressure-induced variations in the electronic superlattice correlate with two peaks in the superconducting transition temperature as pressure changes, hinting that fluctuations within the electronic superlattice could be key to stabilizing superconductivity. However, our findings contrast with the minimal pressure dependency anticipated by ab initio calculations of the electronic structure. They also challenge prevailing scenarios based on a Peierls-like nesting mechanism involving van Hove singularities.

cond-mat.supr-con

Intriguing Low-Temperature Phase in the Antiferromagnetic Kagome Metal FeGe

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.

cond-mat.str-el

Magneto-optical response of the Weyl semimetal NbAs: Experimental results and hyperbolic-band computations

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.

cond-mat.mes-hall

Exchange gap in GdPtBi probed by magneto-optics

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.

cond-mat.mes-hall

Softening of a flat phonon mode in the kagome ScV$_6$Sn$_6$

The long range electronic modulations recently discovered in the geometrically frustrated kagome lattice have opened new avenues to explore the effect of correlations in materials with topological electron flat bands. The observation of the lattice response to the emergent new phases of matter, a soft phonon mode, has remained elusive and the microscopic origin of charge density waves (CDWs) is still unknown. Here, we show, for the first time, a complete melting of the ScV$_ 6$Sn$_ 6$ (166) kagome lattice. The low energy phonon with propagation vector $\frac{1}{3} \frac{1}{3} \frac{1}{2}$ collapses at 98 K, without the emergence of long-range charge order, which sets in with a propagation vector $\frac{1}{3} \frac{1}{3} \frac{1}{3}$. The CDW is driven (but locks at a different vector) by the softening of an overdamped phonon flat plane at k$_z$=$\pi$. We observe broad phonon anomalies in momentum space, pointing to (1) the existence of approximately flat phonon bands which gain some dispersion due to electron renormalization, and (2) the effects of the momentum dependent electron-phonon interaction in the CDW formation. Ab initio and analytical calculations corroborate the experimental findings to indicate that the weak leading order phonon instability is located at the wave vector $\frac{1}{3} \frac{1}{3} \frac{1}{2}$ of a rather flat collapsed mode. We analytically compute the phonon frequency renormalization from high temperatures to the soft mode, and relate it to a peak in the orbital-resolved susceptibility, obtaining an excellent match with both ab initio and experimental results, and explaining the origin of the approximately flat phonon dispersion. Our data report the first example of the collapse of a softening of a flat phonon plane and promote the 166 compounds of the kagome family as primary candidates to explore correlated flat phonon-topological flat electron physics.

cond-mat.str-el

Temperature-driven reorganization of electronic order in CsV$_3$Sb$_5$

We report a temperature dependent x-ray diffraction study of the electronic ordering instabilities in the kagome material CsV$_3$Sb$_5$. Our measurements between 10 K and 120 K reveal an unexpected reorganization of the three-dimensional electronic order in the bulk of CsV$_3$Sb$_5$: At 10 K, a 2x2x2 superstructure modulation due to electronic order is observed, which upon warming changes to a 2x2x4 superstructure at 60 K. The electronic order-order transition discovered here involves a change in the stacking of electronically ordered V$_3$Sb$_5$-layers and agrees perfectly with anomalies previously observed in magneto-transport measurements. This implies that the temperature dependent three-dimensional electronic order plays a decisive role for transport properties, which are related to the Berry-curvature of the V-bands. Our data also show that the bulk electronic order in CsV$_3$Sb$_5$ breaks the 6-fold rotational symmetry of the underlying $P6/mmm$ lattice structure.

cond-mat.str-el

Observation of pressure-induced Weyl state and superconductivity in a chirality-neutral Weyl semimetal candidate SrSi2

Quasi-particle excitations in solids described by the Weyl equation have attracted significant attention in recent years. Thus far, a wide range of solids that have been experimentally realized as Weyl semimetals (WSMs) lack either mirror or inversion symmetry. For the first time, in the absence of both mirror and inversion symmetry, SrSi2 has been predicted as a robust WSM by recent theoretical works. Herein, supported by first-principles calculations, we present systematic angle-resolved photoemission studies of undoped SrSi2 and Ca-doped SrSi2 single crystals. Our results show no evidence of the predicted Weyl fermions at the kz = 0 plane or the Fermi arcs on the (001) surface. With external pressure, the electronic band structure evolved and induced Weyl fermions in this compound, as revealed by first-principle calculations combined with electrical transport property measurements. Moreover, a superconducting transition was observed at pressures above 20 GPa. Our investigations indicate that the SrSi2 system is a good platform for studying topological transitions and correlations with superconductivity.

cond-mat.mtrl-sci

Observation of the Critical State to Multiple-Type Dirac Semimetal Phases in KMgBi

Dirac semimetals (DSMs) are classified into different phases based on the types of the Dirac fermions. Tuning the transition among different types of the Dirac fermions in one system remains challenging. Recently, KMgBi was predicted to be located at a critical state that various types of Dirac fermions can be induced owing to the existence of a flat band. Here, we carried out systematic studies on the electronic structure of KMgBi single crystal by combining angle-resolve photoemission spectroscopy (ARPES) and scanning tunneling microscopy/spectroscopy (STM/STS). The flat band was clearly observed near the Fermi level. We also revealed a small bandgap of ~ 20 meV between the flat band and the conduction band. These results demonstrate the critical state of KMgBi that transitions among various types of Dirac fermions can be tuned in one system.

cond-mat.mtrl-sci

Field induced charge symmetry in topological insulator Bi$_2$Te$_3$ revealed by nuclear magnetic resonance

Nuclear magnetic resonance (NMR) was recently shown to measure the bulk band inversion of Bi$_2$Se$_3$ through changes in the $^{209}$Bi nuclear quadrupole interaction, and the corresponding tensor of the local electric field gradient was found to follow, surprisingly, the direction of the external magnetic field if the sample is rotated. This manifests a hidden property of the charge carriers in the bulk of this topological insulator, which is explored here with another material, Bi$_2$Te$_3$. It is found that two electric field gradients appear to be present at $^{209}$Bi, one rests with the lattice, as usual, while a second follows the external field if it is rotated with respect to the crystal axes. These electronic degrees of freedom correspond to an effective rotation of $j$-electrons, and their level life time is believed to be responsible for a new quadrupolar relaxation that should lead to other special properties including the electronic specific heat.

cond-mat.mtrl-sci

Magneto-optics of a Weyl semimetal beyond the conical band approximation: the case study of TaP

Landau-level spectroscopy, the optical analysis of electrons in materials subject to a strong magnetic field, is a versatile probe of the electronic band structure and has been successfully used in the identification of novel states of matter such as Dirac electrons, topological materials or Weyl semimetals. The latter arise from a complex interplay between crystal symmetry, spin-orbit interaction and inverse ordering of electronic bands. Here, we report on unusual Landau-level transitions in the monopnictide TaP that decrease in energy with increasing magnetic field. We show that these transitions arise naturally at intermediate energies in time-reversal-invariant Weyl semimetals where the Weyl nodes are formed by a partially gapped nodal-loop in the band structure. We propose a simple theoretical model for electronic bands in these Weyl materials that captures the collected magneto-optical data to great extent.

cond-mat.mes-hall