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Abstract The coexistence of the charge-density wave (CDW) and superconducting phases and their tunability under external pressure remains one of the key points in understanding the electronic structure of AV3Sb5 (A = K, Rb, Cs) kagome metals. Here, we employ synchrotron-based infrared spectroscopy assisted by density-functional calculations to study the pressure evolution of the electronic structure at room temperature up to 17 GPa experimentally. The optical spectrum of CsV3Sb5 is characterized by the presence of localized carriers seen as a broad peak at finite frequencies in addition to the conventional metallic Drude response. The non-monotonic pressure dependence of this low-energy peak reflects the re-entrant behavior of superconductivity and may be interpreted in terms of electron-phonon coupling, varying with the growth and shrinkage of the Fermi surface under pressure. Moreover, drastic modifications in the low-energy interband absorptions are observed upon the suppression of CDW. These changes are related to the upward shift of the Sb2 p x + p y band that eliminates part of the Fermi surface around the M-point, whereas band saddle points do not move significantly. These observations shed new light on the mixed electronic and lattice origin of the CDW in CsV3Sb5.

Abstract Kagome metals AV3Sb5 (A = K, Cs, Rb) provide a rich platform for intertwined orders, where evidence for time-reversal symmetry breaking, likely due to the long-sought loop currents, has emerged in STM and muon spin relaxation experiments. An isotropic component in the spontaneous optical rotation has also been reported and was interpreted as the magneto-optic Kerr effect. Intriguingly, the observed rotations differ by five orders of magnitude between different wavelengths and samples, suggesting more intricate physics. Here we report optical rotation and polar Kerr measurements in CsV3Sb5 crystals at the same wavelength. We observe large isotropic components of 1 milliradian in the optical rotation that do not respond to applied magnetic fields, while the spontaneous Kerr signal is less than 20 nanoradians. Our results prove unambiguously that the reported isotropic rotation is not from time-reversal symmetry breaking but represents the long-sought specular optical rotation and indicates a new intertwined order.

Abstract The class of AV3Sb5 (A=K, Rb, Cs) kagome metals hosts unconventional charge density wave states seemingly intertwined with their low temperature superconducting phases. The nature of the coupling between these two states and the potential presence of nearby, competing charge instabilities however remain open questions. This phenomenology is strikingly highlighted by the formation of two ‘domes’ in the superconducting transition temperature upon hole-doping CsV3Sb5. Here we track the evolution of charge correlations upon the suppression of long-range charge density wave order in the first dome and into the second of the hole-doped kagome superconductor CsV3Sb5−x Sn x . Initially, hole-doping drives interlayer charge correlations to become short-ranged with their periodicity diminished along the interlayer direction. Beyond the peak of the first superconducting dome, the parent charge density wave state vanishes and incommensurate, quasi-1D charge correlations are stabilized in its place. These competing, unidirectional charge correlations demonstrate an inherent electronic rotational symmetry breaking in CsV3Sb5, and reveal a complex landscape of charge correlations within its electronic phase diagram. Our data suggest an inherent 2k f charge instability and competing charge orders in the AV3Sb5 class of kagome superconductors.

In this work, we study the effect of electron doping on the kagome superconductor CsV3Sb5. Single crystals and powders of CsV3Sb5−xTex are synthesized and characterized via magnetic susceptibility, nuclear quadrupole resonance, and x-ray diffraction measurements, where we observe a slight suppression of the charge density wave transition temperature and superconducting temperature with the introduction of electron dopants. In contrast to hole doping, both transitions survive relatively unperturbed up to the solubility limit of Te within the lattice. A comparison is presented between the electronic phase diagrams of electron- and hole-tuned CsV3Sb5.

The mechanism of the charge density wave in kagome metals is under intense debate. Here, by using a combination of diffuse scattering and inelastic x-ray scattering, the authors show that the charge density wave transition in (Cs,Rb)V3Sb5 is of the order-disorder type.

Predictions suggest enhanced correlation effect due to multiple van Hove singularities (VHS) in the vicinity of the Fermi level in the recently discovered AV3Sb5 kagome metals. Here the authors identify three VHSs close to the Fermi level with diverse sublattice characters in CsV3Sb5, and one of them shows flat dispersion suggesting the higher-order nature.

The recently discovered vanadium-based Kagome metals AV_{3}Sb_{5} (A = K, Rb, Cs) undergo a unique phase transition into charge-density wave (CDW) order which precedes both unconventional superconductivity and time-reversal symmetry breaking. Therefore the essential first step in building a full understanding of the role of CDW in establishing these unconventional phases is to unveil the symmetries and the microscopic nature of the charge-ordered phase. Here, we determine the exact structure of the 2×2×2 superlattice that develops below the charge-density wave ordering temperature (T_{CDW}) in RbV_{3}Sb_{5}. We present a comprehensive set of ^{51}V, ^{87}Rb, and ^{121}Sb nuclear magnetic resonance (NMR) measurements and density functional theory simulations of NMR observables to provide a unique site-selective view into the local nature of the charge-ordered phase. The combination of these experimental results with simulations provides compelling evidence that the CDW structure prevailing below 103 K in RbV_{3}Sb_{5} is the so-called inverse Star of David pattern, π-shifted along the c axis. These findings put severe constraints on the topology of these Kagome compounds and thus provide essential guidance for the development of an appropriate theoretical framework for predicting properties of exotic electronic orders arising within the CDW phase.

Abstract 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 AV3Sb5 kagome metals (A = K, Rb, Cs). Here, we demonstrate via optical spectroscopy and density-functional calculations that low-energy dynamics of KV3Sb5 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 KV3Sb5. 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 KV3Sb5 and related materials.

The kagome superconductor family AV_{3}Sb_{5} (A=Cs, K, Rb) emerged as an exciting platform to study exotic Fermi surface instabilities. Here, we use spectroscopic-imaging scanning tunneling microscopy (SI-STM) and angle-resolved photoemission spectroscopy (ARPES) to reveal how the surprising cascade of higher- and lower-dimensional density waves in CsV_{3}Sb_{5} is intimately tied to a set of small reconstructed Fermi pockets. ARPES measurements visualize the formation of these pockets generated by a 3D charge density wave transition. The pockets are connected by dispersive q^{*} wave vectors observed in Fourier transforms of STM differential conductance maps. As the additional 1D charge order emerges at a lower temperature, q^{*} wave vectors become substantially renormalized, signaling further reconstruction of the Fermi pockets. Remarkably, in the superconducting state, the superconducting gap modulations give rise to an in-plane Cooper pair density wave at the same q^{*} wave vectors. Our work demonstrates the intrinsic origin of the charge stripes and the pair density wave in CsV_{3}Sb_{5} and their relationship to the Fermi pockets. These experiments uncover a unique scenario of how Fermi pockets generated by a parent charge density wave state can provide a favorable platform for the emergence of additional density waves.

Abstract There is tremendous interest in measuring the strong electron–phonon interactions seen in topological Weyl semimetals. The semimetal NbIrTe4 has been proposed to be a Type-II Weyl semimetal with 8 pairs of opposite Chirality Weyl nodes which are very close to the Fermi energy. We show using polarized angular-resolved micro-Raman scattering at two excitation energies that we can extract the phonon mode dependence of the Raman tensor elements from the shape of the scattering efficiency versus angle. This van der Waals semimetal with broken inversion symmetry and 24 atoms per unit cell has 69 possible phonon modes of which we measure 19 modes with frequencies and symmetries consistent with Density Functional Theory calculations. We show that these tensor elements vary substantially in a small energy range which reflects a strong variation of the electron–phonon coupling for these modes.

The recently discovered family of AV_{3}Sb_{5} (A: K, Rb Cs) kagome metals possess a unique combination of nontrivial band topology, superconducting ground states, and signatures of electron correlations manifest via competing charge density wave order. Little is understood regarding the nature of the charge density wave (CDW) instability inherent to these compounds and the potential correlation with the onset of a large anomalous Hall response. To understand the impact of the CDW order on the electronic structure in these systems, we present quantum oscillation measurements on single crystals of CsV_{3}Sb_{5}. Our data provide direct evidence that the CDW invokes a substantial reconstruction of the Fermi surface pockets associated with the vanadium orbitals and the kagome lattice framework. In conjunction with density functional theory modeling, we are able to identify split oscillation frequencies originating from reconstructed pockets built from vanadium orbitals and Dirac-like bands. Complementary diffraction measurements are further able to demonstrate that the CDW instability has a correlated phasing of distortions between neighboring V_{3}Sb_{5} planes, and the average structure in the CDW state is proposed. These results provide critical insights into the underlying CDW instability in AV_{3}Sb_{5} kagome metals and support minimal models of CDW order arising from within the vanadium-based kagome lattice.

Pressure evolution of the superconducting kagome metal CsV$_3$Sb$_5$ is studied with single-crystal x-ray diffraction and density-functional band-structure calculations. A highly anisotropic compression observed up to 5 GPa is ascribed to the fast shrinkage of the Cs-Sb distances and suppression of Cs rattling motion. This prevents Sb displacements required to stabilize the three-dimensional charge-density-wave (CDW) order and elucidates the disappearance of the CDW already at 2 GPa despite only minor changes in the electronic structure of the normal state. At higher pressures, vanadium bands still change only marginally, whereas antimony bands undergo a major reconstruction caused by the gradual formation of the interlayer Sb-Sb bonds. Our results exclude pressure tuning of vanadium kagome bands as the main mechanism for the non-trivial evolution of superconductivity in real-world kagome metals. Concurrently, we establish the central role of Sb atoms in the stabilization of a three-dimensional CDW and Fermi surface reconstruction.