The synthesis and characterization of vanadium-based kagome metals YV$_6$Sn$_6$ and GdV$_6$Sn$_6$ are presented. X-ray diffraction, magnetization, magnetotransport, and heat capacity measurements reveal an ideal kagome network of V-ions coordinated b
y Sn and separated by triangular lattice planes of rare-earth ions. The onset of low-temperature, likely noncollinear, magnetic order of Gd spins is detected in GdV$_6$Sn$_6$, while V-ions in both compounds remain nonmagnetic. Density functional theory calculations are presented modeling the band structures of both compounds, which can be classified as $mathbb{Z}_2$ topological metals in the paramagnetic state. Both compounds exhibit high mobility, multiband transport and present an interesting platform for controlling the interplay between magnetic order associated with the $R$-site sublattice and nontrivial band topology associated with the V-based kagome network. Our results invite future exploration of other $R$V$_6$Sn$_6$ ($R$=rare earth) variants where this interplay can be tuned via $R$-site substitution.
The recently discovered layered kagome metals AV$_3$Sb$_5$ (A=K, Rb, Cs) exhibit diverse correlated phenomena, which are intertwined with a topological electronic structure with multiple van Hove singularities (VHSs) in the vicinity of the Fermi leve
l. As the VHSs with their large density of states enhance correlation effects, it is of crucial importance to determine their nature and properties. Here, we combine polarization-dependent angle-resolved photoemission spectroscopy with density functional theory to directly reveal the sublattice properties of 3d-orbital VHSs in CsV$_3$Sb$_5$. Four VHSs are identified around the M point and three of them are close to the Fermi level, with two having sublattice-pure and one sublattice-mixed nature. Remarkably, the VHS just below the Fermi level displays an extremely flat dispersion along MK, establishing the experimental discovery of higher-order VHS. The characteristic intensity modulation of Dirac cones around K further demonstrates the sublattice interference embedded in the electronic structure. The crucial insights into the electronic structure, revealed by our work, provide a solid starting point for the understanding of the intriguing correlation phenomena in the kagome metals AV$_3$Sb$_5$.
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 sh
rinkage 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) state and elucidates the disappearance of the CDW already at 2 GPa despite only minor changes in the electronic structure. 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 highlight the central role of Sb atoms in the stabilization of a three-dimensional CDW and re-entrant superconductivity of a kagome metal.
The diversity of emergent phenomena in quantum materials often arises from the interplay between different physical energy scales or broken symmetries. Cooperative interactions among them are rare; however, when they do occur, they often stabilize fu
ndamentally new ground states or phase behaviors. For instance, a pair density wave can form when the superconducting order parameter borrows spatial periodical variation from charge order; a topological superconductor can arise when topologically nontrivial electronic states proximitize with or participate in the formation of the superconducting condensate. Here, we report spectroscopic evidence for a unique synergy of topology and correlation effects in the kagome superconductor CsV$_3$Sb$_5$ - one where topologically nontrivial surface states are pushed below the Fermi energy (E$_F$) by charge order, making the topological physics active near E$_F$ upon entering the superconducting state. Flat bands are observed, indicating that electron correlation effects are also at play in this system. Our results reveal the peculiar electronic structure of CsV$_3$Sb$_5$, which holds the potential for realizing Majorana zero modes and anomalous superconducting states in kagome lattices. They also establish CsV$_3$Sb$_5$ as a unique platform for exploring the cooperation between the charge order, topology, correlation effects and superconductivity.
Recently discovered kagome superconductors AV3Sb5 (A=K, Rb, Cs) provide a fresh opportunity to realize and study correlation-driven electronic phenomena on a kagome lattice. The observation of a 2a0 by 2a0 charge density wave (CDW) in the normal stat
e of all members of AV3Sb5 kagome family has generated an enormous amount of interest, in an effort to uncover the nature of this CDW state, and identify any hidden broken symmetries. We use spectroscopic-imaging scanning tunneling microscopy to reveal a pronounced intensity anisotropy between different 2a0 CDW directions in KV3Sb5. In particular, by examining the strength of ordering wave vectors as a function of energy in Fourier transforms of differential conductance maps, we find that one of the CDW directions is distinctly different compared to the other two. This observation points towards an intrinsic rotation symmetry broken electronic ground state, where the symmetry is reduced from C6 to C2. Furthermore, in contrast to previous reports, we find that the CDW phase is insensitive to magnetic field direction, regardless of the presence or absence of atomic defects. Our experiments, combined with earlier observations of a stripe 4a0 charge ordering in CsV3Sb5, establish correlation-driven rotation symmetry breaking as a unifying feature of AV3Sb5 kagome superconductors.
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 ord
er. Little is understood regarding the nature of the charge density wave (CDW) instability inherent to these compounds and the potential correlation with the accompanying 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 provides 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 between neighboring V$_3$Sb$_5$ planes. 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.
The kagome lattice of transition metal atoms provides an exciting platform to study electronic correlations in the presence of geometric frustration and nontrivial band topology, which continues to bear surprises. In this work, using spectroscopic im
aging scanning tunneling microscopy, we discover a cascade of different symmetry-broken electronic states as a function of temperature in a new kagome superconductor, CsV3Sb5. At a temperature far above the superconducting transition Tc ~ 2.5 K, we reveal a tri-directional charge order with a 2a0 period that breaks the translation symmetry of the lattice. As the system is cooled down towards Tc, we observe a prominent V-shape spectral gap opening at the Fermi level and an additional breaking of the six-fold rotation symmetry, which persists through the superconducting transition. This rotation symmetry breaking is observed as the emergence of an additional 4a0 unidirectional charge order and strongly anisotropic scattering in differential conductance maps. The latter can be directly attributed to the orbital-selective renormalization of the V kagome bands. Our experiments reveal a complex landscape of electronic states that can co-exist on a kagome lattice, and provide intriguing parallels to high-Tc superconductors and twisted bilayer graphene.
Recently discovered alongside its sister compounds KV$_3$Sb$_5$ and RbV$_3$Sb$_5$, CsV$_3$Sb$_5$ crystallizes with an ideal kagome network of vanadium and antimonene layers separated by alkali metal ions. This work presents the electronic properties
of CsV$_3$Sb$_5$, demonstrating bulk superconductivity in single crystals with a T$_{c} = 2.5$K. The normal state electronic structure is studied via angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT), which categorize CsV$_3$Sb$_5$ as a $mathbb{Z}_2$ topological metal. Multiple protected Dirac crossings are predicted in close proximity to the Fermi level ($E_F$), and signatures of normal state correlation effects are also suggested by a high temperature charge density wave-like instability. The implications for the formation of unconventional superconductivity in this material are discussed.
The ability to control carrier concentration based on the extent of Cu solubility in the $mathrm{Cu_{2x}Hg_{2-x}GeTe_4}$ alloy compound (where 0 $leq$ x $leq$ 1) makes $mathrm{Cu_{2x}Hg_{2-x}GeTe_4}$ an interesting case study in the field of thermoel
ectrics. While Cu clearly plays a role in this process, it is unknown exactly how Cu incorporates into the $mathrm{Cu_{2x}Hg_{2-x}GeTe_4}$ crystal structure and how this affects the carrier concentration. In this work, we use a combination of resonant energy X-ray diffraction (REXD) experiments and density functional theory (DFT) calculations to elucidate the nature of Cu incorporation into the $mathrm{Cu_{2x}Hg_{2-x}GeTe_4}$ structure. REXD across the $mathrm{Cu_k}$ edge facilitates the characterization of Cu incorporation in the $mathrm{Cu_{2x}Hg_{2-x}GeTe_4}$ alloy and enables direct quantification of anti-site defects. We find that Cu substitutes for Hg at a 2:1 ratio, wherein Cu annihilates a vacancy and swaps with a Hg atom. DFT calculations confirm this result and further reveal that the incorporation of Cu occurs preferentially on one of the z = 1/4 or z = 3/4 planes before filling the other plane. Furthermore, the amount of $mathrm{Cu_{Hg}}$ anti-site defects quantified by REXD was found to be directly proportional to the experimentally measured hole concentration, indicating that the $mathrm{Cu_{Hg}}$ defects are the driving force for tuning carrier concentration in the $mathrm{Cu_{2x}Hg_{2-x}GeTe_4}$ alloy. The link uncovered here between crystal structure, or more specifically anti-site defects, and carrier concentration can be extended to similar cation-disordered material systems and will aid the development of improved thermoelectric and other functional materials through defect engineering.
The electronic anomalous Hall effect (AHE), where charge carriers acquire a velocity component orthogonal to an applied electric field, is one of the most fundamental and widely studied phenomena in physics. There are several different AHE mechanisms
known, and material examples are highly sought after, however in the highly conductive (skew scattering) regime the focus has centered around ferromagnetic metals. Here we report the observation of a giant extrinsic AHE in KV$_3$Sb$_5$, an exfoliable, Dirac semimetal with a Kagome layer of Vanadium atoms. Although there has been no reports of magnetic ordering down to 0.25 K, the anomalous Hall conductivity (AHC) reaches $approx$ 15,507 $Omega^{-1}$cm$^{-1}$ with an anomalous Hall ratio (AHR) of $approx$ 1.8$ %$; an order of magnitude larger than Fe. Defying expectations from skew scattering theory, KV$_3$Sb$_5$ shows an enhanced skew scattering effect that scales quadratically, not linearly, with the longitudinal conductivity ($sigma_{xx}$), opening the possibility of reaching an anomalous Hall angle (AHA) of 90$^{circ}$ in metals; an effect thought reserved for quantum anomalous Hall insulators. This observation raises fundamental questions about the AHE and opens a new frontier for AHE (and correspondingly SHE) exploration, stimulating investigation in a new direction of materials, including metallic geometrically frustrated magnets, spin-liquid candidates, and cluster magnets.
