The recently discovered Kagome family ${\mathrm{AV}}_3{\mathrm{Sb}}_5$ (A = K, Rb, Cs) exhibits rich physical phenomena, including non-trivial topological electronic structure, giant anomalous Hall effect, charge density waves (CDW) and superconductivity. Notably, CDW in ${\mathrm{AV}}_3{\mathrm{Sb}}_5$ is evidenced to intertwine with its superconductivity and topology, but its nature remains elusive. Here, we combine x-ray scattering experiments and density-functional theory calculations to investigate the CDWs in ${\mathrm{CsV}}_3{\mathrm{Sb}}_5$ and demonstrate the coexistence of 2 $\times$ 2 $\times$ 2 and 2 $\times$ 2 $\times$ 4 CDW stacking phases. Competition between these CDW phases is revealed by tracking the temperature evolution of CDW intensities, which also manifests in different transition temperatures during warming- and cooling measurements. We also identify a meta-stable quenched state of ${\mathrm{CsV}}_3{\mathrm{Sb}}_5$ after fast-cooling process. Our study demonstrates the coexistence of competing CDW stacking in ${\mathrm{CsV}}_3{\mathrm{Sb}}_5$, offering new insights in understanding the novel properties of this system.
We report the transport properties of kagome superconductor CsV$_{3}$Sb$_{5}$ single crystals at magnetic field up to 32 T. The Shubnikov de Haas (SdH) oscillations emerge at low temperature and four frequencies of $F_α=$ 27 T, $F_β=$ 73 T, $F_ε=$ 727 T, and $F_η=$ 786 T with relatively small cyclotron masses are observed. For $F_β$ and $F_ε$, the Berry phases are close to $π$, providing a clear evidence of nontrivial topological band structures of CsV$_{3}$Sb$_{5}$. Furthermore, the consistence between theoretical calculations and experimental results implies that these frequencies can be ass…
We report $^{121}$Sb nuclear quadrupole resonance (NQR) measurements on kagome superconductor CsV$_3$Sb$_5$ with $T_{\rm c}=2.5$ K. $^{121}$Sb NQR spectra split after a charge density wave (CDW) transition at $94$ K, which demonstrates a commensurate CDW state. The coexistence of the high temperature phase and the CDW phase between $91$ K and $94$ K manifests that it is a first order phase transition. The CDW order exhibits Tri-Hexagonal deformation with a lateral shift between the adjacent kagome layers, which is consistent with $2 \times 2 \times 2$ superlattice modulation. The superconducti…
The layered vanadium antimonides AV3Sb5 (A = K, Rb, Cs) are a recently discovered family of topological kagome metals with a rich phenomenology of strongly correlated electronic phases including charge order and superconductivity. Understanding how the singularities inherent to the kagome electronic structure are linked to the observed many-body phases is a topic of great interest and relevance. Here, we combine angle-resolved photoemission spectroscopy and density functional theory to reveal multiple kagome-derived van Hove singularities (vHs) coexisting near the Fermi level of CsV3Sb5 and an…
We report $^{121/123}$Sb nuclear quadrupole resonance (NQR) and $^{51}$V nuclear magnetic resonance (NMR) measurements on kagome metal CsV$_3$Sb$_5$ with $T_{\rm c}=2.5$ K. Both $^{51}$V NMR spectra and $^{121/123}$Sb NQR spectra split after a charge density wave (CDW) transition, which demonstrates a commensurate CDW state. The coexistence of the high temperature phase and the CDW phase between $91$ K and $94$ K manifests that it is a first order phase transition. At low temperature, electric-field-gradient fluctuations diminish and magnetic fluctuations become dominant. Superconductivity eme…
Recently synthesized Kagome compounds AV$_3$Sb$_5$ attract great attention due to the unusual coexistence of the topology, charge density wave and superconductivity. In this {\it Letter}, based on the band structures for CsV$_3$Sb$_5$ in pristine phase, we fit an effective 6-band model for the low-energy processes; utilizing the random phase approximation (RPA) on the effective minimal model, we obtain the momentum-resolved static spin susceptibility attributing the spin-fluctuation pairing mechanism, we find that the superconducting pairing strengths increase with the lift of the Coulomb corr…
CsV$_3$Sb$_5$ is a newly discovered Kagome superconductor that attracts great interest due to its topological nontrivial band structure and the coexistence of superconductivity and charge-density-wave (CDW) with many exotic properties. Here, we report the detailed characterization of the CDW gap in high-quality CsV$_3$Sb$_5$ single crystals using high-resolution angle-resolved photoemission spectroscopy. We find that the CDW gap is strongly momentum dependent. While gapped around the $M$ point, the electronic states remain gapless around the $Γ$ point and along the $Γ$-$K$ direction. Such mome…
We report the observation of two-fold rotation symmetry in charge density wave (CDW) state in the newly discovered Kagome superconductor CsV$_3$Sb$_5$. Below its CDW transition temperature ($T_{CDW}$), the polarization rotation of the reflected laser beam promptly emerges and increases close to about 1 mrad, and the rotation angle shows two-fold rotation symmetry. With femtosecond laser pulse pumping, the rotation angle can be easily suppressed and then recovers in several picoseconds accompanied with coherent oscillations. Significantly, the oscillations in the signal also experience a 180 de…
Fermi surface fluctuations and lattice instabilities in the 2D metallic kagome superconductor CsV$_3$Sb$_5$ are elucidated via polarization-resolved Raman spectroscopy. The presence of a weak electronic continuum in high-quality samples marks the cross-over into the charge-density-wave (CDW) ordered phase, while impurity-rich samples promote strong defect-induced electronic scattering processes that affect the coherence of the CDW phase. CDW-induced phonon anomalies appear below $T_{\mathrm{CDW}}$, with emergent $C2$ symmetry for one of the CDW amplitude modes, alluding to nematicity. In conju…
The connection between unconventional superconductivity and charge density waves (CDW) has intrigued the condensed matter community and found much interest in the recently discovered superconducting Kagome family of AV$_3$Sb$_5$ (A = K, Cs, Rb). Xray diffraction and Raman spectroscopy measurements established that the CDW order in CsV$_3$Sb$_5$ comprises of a 2x2x4 structure with stacking of layers of star-of-David (SD) and inverse-star-of-David (ISD) pattern along the $c$-axis direction. Such interlayer ordering will induce a vast normalization of the electronic ground state; however, it has …
Compounds with kagome lattice usually host many exotic quantum states, including the quantum spin liquid, non-trivial topological Dirac bands and a strongly renormalized flat band, etc. Recently an interesting vanadium based kagome family $A$V$_{3}$Sb$_{5}$ ($A$ = K, Rb, or Cs) was discovered, and these materials exhibit multiple interesting properties, including unconventional saddle-point driving charge density wave (CDW) state, superconductivity, etc. Furthermore, some experiments show anomalous Hall effect which inspires that there might be some chiral flux current states. Here we report s…
We report two new members of V-based kagome metals CsV$_{6}$Sb$_{6}$ and CsV$_{8}$Sb$_{12}$. The most striking structural feature of CsV$_{6}$Sb$_{6}$ is the V kagome bilayers. For CsV$_{8}$Sb$_{12}$, there is an intergrowth of two-dimensional V kagome layers and one-dimensional V chains and the latter lead to the orthorhombic symmetry of this material. Further measurements indicate that these two materials exhibit metallic and Pauli paramagnetic behaviors. More importantly, different from CsV$_{3}$Sb$_{5}$, the charge density wave state and superconductivity do not emerge in CsV$_{6}$Sb$_{6}$…
The ${\mathbb{Z}}_{2}$ topological metals $R$V$_3$Sb$_5$ ($R$ = K, Rb, Cs) with a layered kagome structure provide a unique opportunity to investigate the interplay between charge order, superconductivity and topology. Here, we report muon-spin relaxation/rotation ($μ$SR) measurements performed on CsV$_3$Sb$_5$ across a broad temperature range, in order to uncover the nature of the charge-density wave order and superconductivity in this material. From zero-field $μ$SR, we find that spontaneous magnetic fields appear below 50 K which is well below the charge-density wave transition ($T^* \sim 9…
In transition metal compounds, due to the interplay of charge, spin, lattice and orbital degrees of freedom, many intertwined orders exist with close energies. One of the commonly observed states is the so-called nematic electron state, which breaks the in-plane rotational symmetry. This nematic state appears in cuprates, iron-based superconductor, etc. Nematicity may coexist, affect, cooperate or compete with other orders. Here we show the anisotropic in-plane electronic state and superconductivity in a recently discovered kagome metal CsV$_3$Sb$_5$ by measuring $c$-axis resistivity with the …
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 imaging 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 l…
$A$V$_3$Sb$_5$ ($A$ = K, Rb, Cs) is a novel kagome superconductor coexisting with the charge density wave (CDW) order. Identifying the structure of the CDW order is crucial for understanding the exotic normal state and superconductivity in this system. Here, we report $^{51}$V nuclear magnetic resonance (NMR) and $^{121/123}$Sb nuclear quadrupole resonance (NQR) studies on kagome-metal CsV$_3$Sb$_5$. Below the CDW transition temperature $T_\textrm{CDW} \sim$ 98 K, an abrupt change of spectra was observed, indicating that the transition is of the first order. By further analysing the spectra, w…
Thickness-driven crossover from conventional to chiral nonreciprocal superconductivity in kagome metal CsV3Sb5
National University of Singapore（新加坡国立大学）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；The Chinese University of Hong Kong（香港中文大学）；Research Center for Electronic and Optical Materials（电子与光学材料研究中心）；Research Center for Materials Nanoarchitectonics（材料纳米架构研究中心）；State Key Laboratory of Quantum Information Technologies and Materials（量子信息技术与材料国家重点实验室）；Hunan University（湖南大学）
The transition-metal-based kagome metals provide a versatile platform for correlated topological phases hosting various electronic instabilities. While superconductivity is rare in layered kagome compounds, its interplay with nontrivial topology could offer an engaging space to realize exotic excitations of quasiparticles. Here, we use scanning tunneling microscopy (STM) to study a newly discovered Z$_2$ topological kagome metal CsV$_3$Sb$_5$ with a superconducting ground state. We observe charge modulation associated with the opening of an energy gap near the Fermi level. When across single-u…
Phase transitions governed by spontaneous time reversal symmetry breaking (TRSB) have long been sought in many quantum systems, including materials with anomalous Hall effect (AHE), cuprate high temperature superconductors, Iridates and so on. However, experimentally identifying such a phase transition is extremely challenging because the transition is hidden from many experimental probes. Here, using zero-field muon spin relaxation (ZF-$μ$SR) technique, we observe strong TRSB signals below 70 K in the newly discovered kagome superconductor CsV$_3$Sb$_5$. The TRSB state emerges from the 2 x 2 …
We report on a detailed study of the optical properties of CsV$_{3}$Sb$_{5}$ at a large number of temperatures above and below the charge-density-wave (CDW) transition. Above the CDW transition, the low-frequency optical conductivity reveals two Drude components with distinct widths. An examination of the band structure allows us to ascribe the narrow Drude to multiple light and Dirac bands, and the broad Drude to the heavy bands near the $M$ points which form saddle points near the Fermi level. Upon entering the CDW state, the opening of the CDW gap is clearly observed. A large portion of the…
The recently discovered kagome superconductors $A$V$_3$Sb$_5$ ($A$ = K, Rb, Cs) possess a unique band structure with van Hove singularities and Dirac dispersions, in which unusual charge-density-wave (CDW) orders with time-reversal and rotational symmetry breaking have been reported. One of the most crucial unresolved issues is identifying the symmetry of the superconductivity that develops inside the CDW phase. Theory predicts a variety of unconventional superconducting symmetries, including exotic states with chiral and topological properties accompanied by a sign-changing superconducting ga…
Recently, kagome lattice metal AV$_3$Sb$_5$ (A = K, Rb, Cs) family has received wide attention due to its presence of superconductivity, charge density wave (CDW) and peculiar properties from topological nontrivial electronic structure. With time-resolved pump-probe spectroscopy, we show that the excited quasiparticle relaxation dynamics can be explained by formation of energy gap below the phase transition being similar to a usual second-order CDW condensate, by contrast, the structure change is predominantly first order phase transition. Furthermore, no CDW amplitude mode is identified in th…
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 …
Recently superconductivity was discovered in the Kagome metal AV3Sb5 (A = K, Rb, and Cs), which has an ideal Kagome lattice of vanadium. These V-based superconductors also host charge density wave (CDW) and topological nontrivial band structure. Here we report the ultralow-temperature thermal conductivity and high pressure resistance measurements on CsV3Sb5 with Tc = 2.5 K, the highest among AV3Sb5. A finite residual linear term of thermal conductivity at zero magnetic field and its rapid increase in fields suggest nodal superconductivity. By applying pressure, the Tc of CsV3Sb5 increases firs…
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 fundamentally 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 c…
The superconductivity of a kagome superconductor CsV3Sb5 is studied by scanning tunneling microscopy / spectroscopy at an ultralow temperature with high resolution. Two kinds of superconducting gaps with multiple sets of coherent peaks and residual zero-energy density of states are observed on both half-Cs and Sb surfaces, implying multiband superconductivity with gap nodes. Sixfold star-shaped magnetic vortex is observed with conventional Caroli-de Gennes-Matricon bound states inside. Magnetic impurities suppress the superconductivity, while nonmagnetic impurities do not, suggesting the absen…
Recently, competing electronic instabilities, including superconductivity and density-wave-like order, have been discovered in vanadium-based kagome metals AV3Sb5 (A = K, Rb, Cs) with a nontrivial band topology. This finding stimulates wide interests to study the interplay of these competing electronic orders and possible exotic excitations in the superconducting state. Here, in order to further clarify the nature of density-wave-like transition in these kagome superconductors, we performed 51V and 133Cs nuclear magnetic resonance (NMR) measurements on the CsV3Sb5 single crystal. A first-order…
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 pred…
The cascade of electronic phases in CsV$_3$Sb$_5$ raises the prospect to disentangle their mutual interactions in a clean, strongly interacting Kagome lattice. When the Kagome planes are stacked into a crystal, its electronic dimensionality encodes how much of the Kagome physics and its topological aspects survive. The layered structure of CsV$_3$Sb$_5$ reflects in Brillouin-zone-sized quasi-2D Fermi surfaces and a significant transport anisotropy. Yet here we demonstrate that CsV$_3$Sb$_5$ is a three-dimensional metal within the charge-density-wave (CDW) state. Small 3D pockets play a crucial…
Soft Mode Origin of Charge Ordering in Superconducting Kagome CsV$_3$Sb$_5$
Institute for Quantum Materials and Technologies, Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院量子材料与技术研究所）；Centro de Física de Materiales (CFM-MPC), CSIC-UPV/EHU（巴斯克大学/西班牙国家研究委员会材料物理中心）；Department of Applied Physics, University of the Basque Country (UPV/EHU)（巴斯克大学应用物理系）；Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）；ESRF, The European Synchrotron（欧洲同步辐射装置）；Materials Dynamics Laboratory, RIKEN SPring-8 Center（理化学研究所SPring-8中心物质动力学实验室）；Precision Spectroscopy Division, SPring-8/JASRI（SPring-8/JASRI精密光谱部）
The vanadium-based kagome superconductor CsV3Sb5 has attracted tremendous attention due to its unexcepted anomalous Hall effect (AHE), charge density waves (CDWs), nematicity, and a pseudogap pair density wave (PDW) coexisting with unconventional strong-coupling superconductivity (SC). The origins of CDWs, unconventional SC, and their correlation with different electronic states in this kagome system are of great significance, but so far, are still under debate. Chemical doping in the kagome layer provides one of the most direct ways to reveal the intrinsic physics, but remains unexplored. Her…
Superconductivity in topological kagome metals has recently received great research interests. Here, charge density wave (CDW) orders and the evolution of superconductivity under various pressures in CsV3Sb5 single crystal with V kagome lattice are investigated. By using high-resolution scanning tunnelling microscopy /spectroscopy (STM/STS), two CDW orders in CsV3Sb5 are observed which correspond to 4a*1a and 2a*2a superlattices. By applying pressure, the superconducting transition temperature Tc is significantly enhanced and reaches a maximum value of 8.2 K at around 1 GPa. Accordingly, CDW s…
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 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 si…
The kagome lattice is host to flat bands, topological electronic structures, Van Hove singularities and diverse electronic instabilities, providing an ideal platform for realizing highly tunable electronic states. Here, we report soft- and mechanical- point-contact spectroscopy (SPCS and MPCS) studies of the kagome superconductors KV$_3$Sb$_5$ and CsV$_3$Sb$_5$. Compared to the superconducting transition temperature $T_{\rm c}$ from specific heat measurements (2.8~K for CsV$_3$Sb$_5$ and 1.0~K for KV$_3$Sb$_5$), significantly enhanced values of $T_{\rm c}$ are observed via the zero-bias conduc…
Strain-Tuned Nodal Superconductivity in the Charge-Ordered Kagome Metal CsV$_3$Sb$_5$
Okayama University（冈山大学）；Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；Beijing National Laboratory for Condensed Matter Physics（北京凝聚态物理国家实验室）；Fujian Provincial Collaborative Innovation Center for Advanced High-Field Superconducting Materials and Engineering（福建省先进高场超导材料与工程协同创新中心）；College of Physics and Energy, Fujian Normal University（福建师范大学物理与能源学院）；Guang’an Institute of Technology
The recently discovered kagome metal series $A$V$_3$Sb$_5$ ($A$=K, Rb, Cs) exhibits topologically nontrivial band structures, chiral charge order and superconductivity, presenting a unique platform for realizing exotic electronic states. The nature of the superconducting state and the corresponding pairing symmetry are key questions that demand experimental clarification. Here, using a technique based on the tunneling diode oscillator, the magnetic penetration depth $Δλ(T)$ of CsV$_3$Sb$_5$ was measured down to 0.07 K. A clear exponential behavior in $Δλ(T)$ with marked deviations from a $T$ o…
Recent high pressure experiments discovered abnormal double-dome superconductivities in the newly-synthesized kagome materials $A$V$_3$Sb$_5$ ($A$ = K, Rb, Cs), which also host abundant emergent quantum phenomena such as charge density wave (CDW), anomalous Hall effect, nontrivial topological property, etc. In this work, by using first-principles electronic structure calculations, we have studied the CDW state, superconductivity, and topological property in CsV$_3$Sb$_5$ under pressures ($<$ 50 GPa). Based on the electron-phonon coupling theory, our calculated superconducting $T_\text{c}$s are…
Symmetry Origins of the Field-Free Superconducting Diode Effect in the Kagome Superconductor CsV$_3$Sb$_5$
University of Science and Technology Beijing（北京科技大学）；International Quantum Academy, and Shenzhen Branch, Hefei National Laboratory（国际量子学院合肥国家实验室深圳分院）；Southern University of Science and Technology（南方科技大学）；Hong Kong University of Science and Technology（香港科技大学）；Ningxia University（宁夏大学）；Sun Yat-sen University（中山大学）；Peking University（北京大学）；Anhui University（安徽大学）
The recently discovered layered kagome metals AV$_3$Sb$_5$ (A = K, Rb, and Cs) with vanadium kagome networks provide a novel platform to explore correlated quantum states intertwined with topological band structures. Here we report the prominent effect of hole doping on both superconductivity and charge density wave (CDW) order, achieved by selective oxidation of exfoliated thin flakes. A superconducting dome is revealed as a function of the effective doping content. The superconducting transition temperature ($T_{\mathrm{c}}$) and upper critical field in thin flakes are significantly enhanced…
Nonreciprocal charge transport phenomena are widely studied in two-dimensional superconductors, which demonstrate unidirectional-anisotropy magnetoresistances as a result of symmetry breaking. Here, we report a strong nonreciprocal transport phenomenon in superconducting CsV$_{3}$Sb$_{5}$ thin flakes. The second harmonic voltages, mainly originating from the rectification effect of vortex motion, are unambiguously developed with in-plane and out-of-plane magnetic fields, and their magnitudes are comparable to those in noncentrosymmetric superconductors. The second harmonic magnetoresistances s…
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 level. 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 V…
Linear nonsaturating magnetoresistance (LMR) represents a class of anomalous resistivity response to external magnetic field that has been observed in a variety of materials including but not limited to topological semi-metals, high-Tc superconductors and materials with charge/spin density wave (CDW/SDW) orders. Here we report the observation of LMR in layered kagome superconductor and CDW material CsV3Sb5 thin flakes, as well as the dimensional crossover and temperature (T) crossover of such LMR. Specifically, in ultrathin CsV3Sb5 crystals, the magnetoresistance (MR) exhibits a crossover from…
