The family of metallic kagome compounds $A$V$_3$Sb$_5$ ($A$=K, Rb, Cs) was recently discovered to exhibit both superconductivity and charge order. The nature of the charge-density wave (CDW) phase is presently unsettled, which complicates the interpretation of the superconducting ground state. In this paper, we use group-theory and density-functional theory (DFT) to derive and solve a phenomenological Landau model for this CDW state. The DFT results reveal three unstable phonon modes with the same in-plane momentum but different out-of-plane momenta, whose frequencies depend strongly on the electronic temperature. This is indicative of an electronically-driven CDW, stabilized by features of the in-plane electronic dispersion. Motivated by the DFT analysis, we construct a Landau free-energy expansion for coupled CDW order parameters with wave-vectors at the $M$ and $L$ points of the hexagonal Brillouin zone. We find an unusual trilinear term coupling these different order parameters, which can promote the simultaneous condensation of both CDWs even if the two modes are not nearly-degenerate. We classify the different types of coupled multi-$\bf{Q}$ CDW orders, focusing on those that break the sixfold rotational symmetry and lead to a unit-cell doubling along all three crystallographic directions, as suggested by experiments. We determine a region in parameter space, characterized by large nonlinear Landau coefficients, where these phases - dubbed staggered tri-hexagonal and staggered Star-of-David - are the leading instabilities of the system. Finally, we discuss the implications of our results for the kagome metals.
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…
In kagome metals AV3Sb5 (A = K, Rb, Cs), three-dimensional charge order (3D-CO) is the primary instability that sets the stage for other collective orders to emerge, including unidirectional stripe order, orbital flux order, electronic nematicity, and superconductivity. Here, we use high-resolution angle-resolved photoemission spectroscopy to determine the microscopic structure of three-dimensional charge order (3D-CO) in AV3Sb5 and its interplay with superconductivity. Our approach is based on identifying an unusual splitting of kagome bands induced by 3D-CO, which provides a sensitive way to…
The nature of superconductivity in newly discovered Kagome materials, $\text{AV}_3\text{Sb}_5$ (A=K, Rb, Cs), has been a subject of intense debate. Recent experiments suggest the presence of orbital current order on top of the charge density wave (CDW) and superconductivity. Since the orbital current order breaks time-reversal symmetry, it may fundamentally affect possible superconducting states. In this work, we investigate the mutual influence between the orbital current order and superconductivity in Kagome metal with characteristic van Hove singularity (vHS). By explicitly deriving the Lan…
Here we report the observation of bulk superconductivity in single crystals of the two-dimensional kagome metal KV$_3$Sb$_5$. Magnetic susceptibility, resistivity, and heat capacity measurements reveal superconductivity below $T_c = 0.93$K, and density functional theory (DFT) calculations further characterize the normal state as a $\mathbb{Z}_2$ topological metal. Our results demonstrate that the recent observation of superconductivity within the related kagome metal CsV$_3$Sb$_5$ is likely a common feature across the AV$_3$Sb$_5$ (A: K, Rb, Cs) family of compounds and establish them as a rich…
As one of the most fundamental physical phenomena, the anomalous Hall effect (AHE) typically occurs in ferromagnetic materials but is not expected in the conventional superconductors. Here, we have observed a giant AHE in kagome superconductor CsV3Sb5 with transition temperature (Tc) of 2.7 K. The anomalous Hall conductivity reaches up to 2.1*10^4 Ω-1 cm-1 which is larger than those observed in most of the ferromagnetic metals. Strikingly, the emergence of AHE exactly follows the higher-temperature charge-density-wave (CDW) transition with TCDW ~ 94 K, indicating a strong correlation between t…
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…
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…
Metal-organic frameworks (MOFs), which are self-assemblies of metal ions and organic ligands, provide a tunable platform to search a new state of matter. A two-dimensional (2D) perfect kagome lattice, whose geometrical frustration is a key to realizing quantum spin liquids, has been formed in the $π$-${d}$ conjugated 2D MOF [Cu$_{3}$(C$_{6}$S$_{6}$)]$_{n}$ (Cu-BHT). The recent discovery of its superconductivity with a critical temperature $T_{\rm c}$ of 0.25\,kelvin raises fundamental questions about the nature of electron pairing. Here, we show that Cu-BHT is a strongly correlated unconventio…
The binary intermetallic materials, $M_3$Sn$_2$ ($M$ = 3d transition metal) present a new class of strongly correlated systems that naturally allows for the interplay of magnetism and metallicity. Using first principles calculations we confirm that bulk Fe$_3$Sn$_2$ is a ferromagnetic metal, and show that $M$ = Ni and Cu are paramagnetic metals with non-trivial band structures. Focusing on Fe$_3$Sn$_2$ to understand the effect of enhanced correlations in an experimentally relevant atomistically thin single kagome-bilayer, our ab-initio results show that dimensional confinement naturally expose…
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 …
Exotic quantum phase transitions in metals, such as the nematic and smectic states, were discovered one after another and found to be universal now. The emergence of unconventional density-wave order in frustrated kagome metal AV$_3$Sb$_5$ and its interplay with exotic superconductivity attract increasing attention. We reveal that the smectic bond-density-wave is naturally caused by the paramagnon interference mechanism, because strong scatterings among different van-Hove singularity points are induced. In addition, the fluctuations of the bond-order induce sizable "beyond-Migdal" pairing glue…
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$_{6}$…
University of Bologna（博洛尼亚大学）；Universität Zürich（苏黎世大学）；Universität Würzburg（维尔茨堡大学）；Massachusetts Institute of Technology（麻省理工学院）；Boston College（波士顿学院）；University of California Santa Barbara（加州大学圣巴巴拉分校）
Motivated by recent experiments on the kagome metals $A\text{V}_3\text{Sb}_5$ with $A=\text{K}$, $\text{Rb}$, and $\text{Cs}$, which show a charge density wave (CDW) at $\sim100$ K and the superconductivity at $\sim1$ K, we explore the onset of the superconductivity, taking the perspective that it descends from a parent CDW. We argue that viewing the superconductivity as a weak-coupling instability of a reconstructed (by the CDW) Fermi surface naturally explains the experimentally observed 'multidome' nonmonotonic dependence on pressure, with the 'peaks' in the superconducting critical tempera…
Kagome metals $A$V$_3$Sb$_5$ ($A=$ K, Rb, and Cs) exhibit intriguing superconductivity below $0.9 \sim 2.5 $ K, a charge density wave (CDW) transition around $80\sim 100 $ K, and $\mathbb{Z}_{2}$ topological surface states. The nature of the CDW phase and its relation to superconductivity remains elusive. In this work, we investigate the electronic and structural properties of CDW by first-principles calculations. We reveal an inverse Star of David deformation as the $2\times2\times2$ CDW ground state of the kagome lattice. The kagome lattice shows softening breathing-phonon modes, indicating …
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…
Materials with transition metals in triangular lattices are of great interest for their potential combination of strong correlation, exotic magnetism and electronic topology. Kagome nets are of particular importance since the discovery of geometrically frustrated magnetism and topological band structures in crystals like Herbertsmithite and Fe3Sn2, respectively. KV3Sb5 was discovered to be a layered topological metal with a Kagome net of vanadium. Here, we fabricated Josephson Junctions (JJ) of K1-xV3Sb5 and induced superconductivity over long junction lengths. Through magnetoresistance and cu…
Recent experiments on kagome metals AV$_3$Sb$_5$ (A=K,Rb,Cs) [M. Kang et al., Nat. Phys. 18, 301-308 (2022)] identify twofold van Hove singularities (TvHS) with opposite concavity near the Fermi energy, generating two approximately hexagonal Fermi surfaces -- one electron-like and the other hole-like. Here we propose that a TvHS generates a novel time-reversal symmetry breaking excitonic order -- arising due to bound pairs of electrons and holes located at opposite concavity van Hove singularities. We introduce a minimal model for the TvHS and investigate interaction induced many-body instabil…
Quantum materials with layered kagome structures have drawn considerable attention due to their unique lattice geometry, which gives rise to flat bands co-existing with Dirac-like dispersions. The interplay between strong Coulomb correlations and nontrivial band topology in these systems results in various exotic phenomena. Recently, vanadium-based materials with layered kagome structures are discovered to be topological metals, which exhibit charge density wave (CDW) properties, significant anomalous Hall effect, and unusual superconductivity at low temperatures. Here we exploit high-resoluti…
A group of newly discovered non-magnetic metal kagome structures AV3Sb5 (A=K, Rb, Cs) have aroused widespread interest in experiment and theory due to their unusual charge density wave (CDW) and intertwined superconductivity. However, they all possess weak electron-phonon coupling (EPC) and low superconducting transition temperature. Here, we performed high-throughput first-principles calculations on novel kagome candidates with AV3Sb5 prototype structure, and proposed 24 dynamically stable novel kagome metals. The calculation based on Bardeen-Cooper-Schrieffer theory shows that most of these …
The family of AV$_3$Sb$_5$ (A = K, Rb, Cs) kagome metals exhibit charge density wave (CDW) order, proposed to be chiral, followed by a lower temperature superconducting state. Recent studies have proposed the importance of band structure saddle points proximal to the Fermi energy in governing these two transitions. Here we show the effects of hole-doping achieved via chemical substitution of Sn for Sb on the CDW and superconducting states in both KV$_3$Sb$_5$ and RbV$_3$Sb$_5$, and generate a phase diagram. Hole-doping lifts the $Γ$ pocket and van Hove singularities (vHs) toward $E_F$ causing …
Prediction of 1:1 kagome metals with superconductivity and band topology
School of Physics and Physical Engineering, Qufu Normal University（曲阜师范大学物理与光电工程学院）；Hunan Provincial Key laboratory of Thin Film Materials and Devices, School of Materials Science and Engineering, Xiangtan University（湘潭大学材料科学与工程学院薄膜材料与器件湖南省重点实验室）；Institute of Applied Physics and Computational Mathematics（应用物理与计算数学研究所）
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…
Kagome metals AV3Sb5 (A = K, Rb, and Cs) with a V-Kagome lattice acting as a fertile platform to investigate geometric frustration, electron correlation, superconductivity, and nontrivial band topology, have attracted tremendous attention. Here we reported the structure and properties of ATi3Bi5 (A = Rb, Cs) family with a Ti-Kagome lattice, specifically focusing on the electronic structure and nontrivial band topology of RbTi3Bi5. ATi3Bi5 (A = Rb, Cs) is found to be non-superconducting metal with strong quasi-two-dimensional feature, moderate electron correlation, and small Pauli paramagnetism…
Superconductivity and Electron Correlations in Kagome Metal LuOs3B2
Southwest Jiaotong University（西南交通大学）；Tsung-Dao Lee Institute, Shanghai Jiao Tong University（上海交大李政道研究所）；Shanghai Jiao Tong University（上海交通大学）；Zhejiang University（浙江大学）；Fujian Provincial Collaborative Innovation Center for Advanced High-Field Superconducting Materials and Engineering（福建省先进强磁场超导材料与工程协同创新中心）；Fujian Normal University（福建师范大学）
Cavity Tuning of the CDW--Superconductivity Interplay in a Kagome Metal
Tsientang Institute for advaced study（钱塘高等研究院）；Songshan Lake Materials Laboratory（松山湖材料实验室）；Max Planck Institute for the Structure and Dynamics of Matter and Center for Free-Electron Laser Science（马普物质结构与动力学研究所及自由电子激光科学中心）；Department of Materials Science and Engineering, City University of Hong Kong（香港城市大学材料科学与工程系）；Department of Physics and Photon Science, Gwangju Institute of Science and Technology (GIST)（光州科学技术院物理与光子科学系）；The Flatiron Institute（平顿研究所）
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…
We report on in situ low-temperature (4 K) scanning tunneling microscope measurements of atomic and electronic structures of the cleaved surfaces of an alkali-based kagome metal RbV$_3$Sb$_5$ single crystals. We find that the dominant pristine surface exhibits Rb-1x1 structure, in which a unique unidirectional $\sqrt{3}a_0$ charge order is discovered. As the sample temperature slightly rises, Rb-$\sqrt{3}$x1 and Rb-$\sqrt{3}$x$\sqrt{3}$ reconstructions form due to desorption of surface Rb atoms. Our conductance mapping results demonstrate that Rb desorption not only gives rise to hole doping, …
Spatially anisotropic Kondo resonance coupled with the superconducting gap in a kagome metal
Beijing National Center for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Hefei National Laboratory（合肥国家实验室）；Beijing Key Laboratory of Optoelectronic Functional Materials & Micro-Nano Devices, School of Physics, Renmin University of China（中国人民大学物理学院）；Department of Physics, Boston College（波士顿学院物理系）
The interplay of superconductivity with electronic and structural instabilities on the kagome lattice provides a fertile ground for the emergence of unusual phenomena. The vanadium-based kagome metals $A$V$_3$Sb$_5$ ($A=$ K, Rb, Cs) exhibit superconductivity on an almost ideal kagome lattice, with the superconducting transition temperature $T_{\rm c}$ forming two domes upon pressure-tuning. The first dome arises from the competition between superconductivity and a charge-density-wave, whereas the origin for the second dome remains unclear. Herein, we show that the appearance of the second supe…
The kagome lattice, the most prominent structural motif in quantum physics, benefits from inherent nontrivial geometry to host diverse quantum phases, ranging from spin-liquid phases, topological matter to intertwined orders, and most rarely unconventional superconductivity. Recently, charge sensitive probes have suggested that the kagome superconductors AV_3Sb_5 (A = K, Rb, Cs) (A = K, Rb, Cs) exhibit unconventional chiral charge order, which is analogous to the long-sought-after quantum order in the Haldane model or Varma model. However, direct evidence for the time-reversal symmetry-breakin…
Recently, the superconductivity in a metal-organic framework (MOF) has been discovered for the first time in copper(II) benzenehexathiolate ([Cu$_3$(C$_6$S$_6$)]$_n$, Cu-BHT). The Cu atoms form a two-dimensional perfect Kagome lattice, which has the potential to host a metallic quantum spin liquid state. Here we present high-precision measurements of in-plane magnetic penetration depth $λ$ in Cu-BHT films down to 40\,mK. The temperature dependence of $λ$ shows a non-exponential, quasi-linear behavior at low temperatures, suggesting that unconventional superconductivity with low-energy quasipar…
We report the discovery of superconductivity and detailed normal-state physical properties of RbV3Sb5 single crystals with V kagome lattice. RbV3Sb5 single crystals show a superconducting transition at Tc ~ 0.92 K. Meanwhile, resistivity, magnetization and heat capacity measurements indicate that it exhibits anomalies of properties at T* ~ 102 - 103 K, possibly related to the formation of charge ordering state. When T is lower than T*, the Hall coefficient RH undergoes a drastic change and sign reversal from negative to positive, which can be partially explained by the enhanced mobility of hol…
Kagome lattice, made of corner-sharing triangles, provides an excellent platform for hosting exotic topological quantum states. Here we systematically studied the magnetic and transport properties of RMn6Sn6 (R = Tb, Dy, Ho) with clean Mn kagome lattice. All the compounds have a collinear ferrimagnetic structure with different easy axis at low temperature. The low-temperature magnetoresistance (MR) is positive and has no tendency to saturate below 7 T, while the MR gradually declines and becomes negative with the increasing temperature. A large intrinsic anomalous Hall conductivity about 250 Ω…
