New kagome prototype materials: Discovery of KV3Sb5,RbV3Sb5, and CsV3Sb5
Colorado School of Mines1, University of California, Santa Barbara2, University of Illinois at Urbana–Champaign3, National Center for Supercomputing Applications4, Johns Hopkins University5, Gdańsk University of Technology6, Colorado State University7, University of Maryland, College Park8, National Institute of Standards and Technology9
TL;DR: In this paper, a new kagome prototype structure is presented, which is based on vanadium, with the Fermi level in close proximity to several Dirac points.
Abstract: In this work, we present our discovery and characterization of a new kagome prototype structure, ${\mathrm{KV}}_{3}{\mathrm{Sb}}_{5}$. We also present the discovery of the isostructural compounds ${\mathrm{RbV}}_{3}{\mathrm{Sb}}_{5}$ and ${\mathrm{CsV}}_{3}{\mathrm{Sb}}_{5}$. All materials exhibit a structurally perfect two-dimensional kagome net of vanadium. Density-functional theory calculations indicate that the materials are metallic, with the Fermi level in close proximity to several Dirac points. Powder and single-crystal syntheses are presented, with postsynthetic treatments shown to deintercalate potassium from single crystals of ${\mathrm{KV}}_{3}{\mathrm{Sb}}_{5}$. Considering the proximity to Dirac points, deintercalation provides a convenient means to tune the Fermi level. Magnetization measurements indicate that ${\mathrm{KV}}_{3}{\mathrm{Sb}}_{5}$ exhibits behavior consistent with a the Curie-Weiss model at high temperatures, although the effective moment is low $(0.22{\ensuremath{\mu}}_{\text{B}}$ per vanadium ion). An anomaly is observed in both magnetization and heat capacity measurements at 80 K, below which the moment is largely quenched. Elastic neutron scattering measurements find no obvious evidence of long-range or short-range magnetic ordering below 80 K. The possibility of an orbital-ordering event is considered. Single-crystal resistivity measurements show the effect of deintercalation on the electron transport and allow estimation of the Kadowaki-Woods ratio in ${\mathrm{KV}}_{3}{\mathrm{Sb}}_{5}$. We find that $A/{\ensuremath{\gamma}}^{2}\ensuremath{\sim}61\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{Ohm}$ cm ${\mathrm{mol}}_{\text{FU}}^{2}\phantom{\rule{4pt}{0ex}}{\mathrm{K}}^{2}\phantom{\rule{4pt}{0ex}}{\mathrm{J}}^{\ensuremath{-}2}$, suggesting that correlated electron transport may be possible. ${\mathrm{KV}}_{3}{\mathrm{Sb}}_{5}$ and its cogeners ${\mathrm{RbV}}_{3}{\mathrm{Sb}}_{5}$ and ${\mathrm{CsV}}_{3}{\mathrm{Sb}}_{5}$ represent a new family of kagome metals, and our results demonstrate that they deserve further study as potential model systems.
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TL;DR: The electronic properties of CsV_{3}Sb_{5} are presented, demonstrating bulk superconductivity in single crystals with a T_{c}=2.5 K, and the implications for the formation of unconventional super conductivity in this material are discussed.
Abstract: A cesium-rich ``kagome'' metal is both a topological insulator and a superconductor, making it a compelling material for future quantum technologies.
456 citations
TL;DR: KV3Sb5 shows enhanced skew scattering that scales quadratically, not linearly, with the longitudinal conductivity, possibly arising from the combination of highly conductive Dirac quasiparticles with a frustrated magnetic sublattice, which allows the possibility of reaching an anomalous Hall angle of 90° in metals.
Abstract: The anomalous Hall effect (AHE) is one of the most fundamental phenomena in physics. In the highly conductive regime, ferromagnetic metals have been the focus of past research. Here, we report a giant extrinsic AHE in KV3Sb5, an exfoliable, highly conductive semimetal with Dirac quasiparticles and a vanadium Kagome net. Even without report of long range magnetic order, the anomalous Hall conductivity reaches 15,507 Ω-1 cm-1 with an anomalous Hall ratio of ≈ 1.8%; an order of magnitude larger than Fe. Defying theoretical expectations, KV3Sb5 shows enhanced skew scattering that scales quadratically, not linearly, with the longitudinal conductivity, possibly arising from the combination of highly conductive Dirac quasiparticles with a frustrated magnetic sublattice. This allows the possibility of reaching an anomalous Hall angle of 90° in metals. This observation raises fundamental questions about AHEs and opens new frontiers for AHE and spin Hall effect exploration, particularly in metallic frustrated magnets.
326 citations
Cites background from "New kagome prototype materials: Dis..."
...(33) found that the compound displays paramagnetic behavior at high temperatures, before undergoing a transition at 80 K to either a dilute trimerized state from orbital ordering effects or a highly frustrated state with localized moments....
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...Figure 1C shows the typical temperature dependence of xx for a 105-nm-thick device (see the Supplementary Materials for fabrication information); with decreasing temperature, a kink is visible in xx around 80 K, corresponding to the known magnetization and heat capacity anomaly (33)....
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...(33) comparing disordered AFM and ferrimagnetic ordering also support this expectation....
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...25 K (33), the anomalous Hall conductivity (AHC), at 2 K, reaches as high as ≈15,507 ohm−1cm−1 with an anomalous Hall ratio (AHR) of ≈1....
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TL;DR: In this paper, the authors used high-resolution scanning tunnelling microscopy to discover an unconventional chiral charge order in a kagome material, KV3Sb5, with both a topological band structure and a superconducting ground state.
Abstract: Intertwining quantum order and non-trivial topology is at the frontier of condensed matter physics1–4. A charge-density-wave-like order with orbital currents has been proposed for achieving the quantum anomalous Hall effect5,6 in topological materials and for the hidden phase in cuprate high-temperature superconductors7,8. However, the experimental realization of such an order is challenging. Here we use high-resolution scanning tunnelling microscopy to discover an unconventional chiral charge order in a kagome material, KV3Sb5, with both a topological band structure and a superconducting ground state. Through both topography and spectroscopic imaging, we observe a robust 2 × 2 superlattice. Spectroscopically, an energy gap opens at the Fermi level, across which the 2 × 2 charge modulation exhibits an intensity reversal in real space, signalling charge ordering. At the impurity-pinning-free region, the strength of intrinsic charge modulations further exhibits chiral anisotropy with unusual magnetic field response. Theoretical analysis of our experiments suggests a tantalizing unconventional chiral charge density wave in the frustrated kagome lattice, which can not only lead to a large anomalous Hall effect with orbital magnetism, but also be a precursor of unconventional superconductivity. An unconventional chiral charge order is observed in a kagome superconductor by scanning tunnelling microscopy. This charge order has unusual magnetic tunability and intertwines with electronic topology.
275 citations
TL;DR: In this article, the discovery of superconductivity and detailed normal-state physical properties of RbV3Sb5 single crystals with V kagome lattice were reported.
Abstract: 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 hole-type carriers. In addition, the results of quantum oscillations show that there are some very small Fermi surfaces with low effective mass, consistent with the existence of multiple highly dispersive Dirac band near the Fermi energy level.
258 citations
TL;DR: In this paper, the authors reported the observation of bulk superconductivity in single crystals of the two-dimensional kagome metal (KV, Rb, Cs) with magnetic susceptibility, resistivity, and heat capacity measurements.
Abstract: Here we report the observation of bulk superconductivity in single crystals of the two-dimensional kagome metal ${\mathrm{KV}}_{3}{\mathrm{Sb}}_{5}$. Magnetic susceptibility, resistivity, and heat capacity measurements reveal superconductivity below ${T}_{c}=0.93\phantom{\rule{0.28em}{0ex}}\mathrm{K}$, 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 ${\mathrm{CsV}}_{3}{\mathrm{Sb}}_{5}$ is likely a common feature across the $A{\mathrm{V}}_{3}{\mathrm{Sb}}_{5}$ ($A$: K, Rb, Cs) family of compounds and establishes them as a rich arena for studying the interplay between bulk superconductivity, topological surface states, and likely electronic density wave order in an exfoliable kagome lattice.
242 citations
References
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Abstract: Generalized gradient approximations (GGA’s) for the exchange-correlation energy improve upon the local spin density (LSD) description of atoms, molecules, and solids. We present a simple derivation of a simple GGA, in which all parameters (other than those in LSD) are fundamental constants. Only general features of the detailed construction underlying the Perdew-Wang 1991 (PW91) GGA are invoked. Improvements over PW91 include an accurate description of the linear response of the uniform electron gas, correct behavior under uniform scaling, and a smoother potential. [S0031-9007(96)01479-2] PACS numbers: 71.15.Mb, 71.45.Gm Kohn-Sham density functional theory [1,2] is widely used for self-consistent-field electronic structure calculations of the ground-state properties of atoms, molecules, and solids. In this theory, only the exchange-correlation energy EXC › EX 1 EC as a functional of the electron spin densities n"srd and n#srd must be approximated. The most popular functionals have a form appropriate for slowly varying densities: the local spin density (LSD) approximation Z d 3 rn e unif
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TL;DR: An efficient scheme for calculating the Kohn-Sham ground state of metallic systems using pseudopotentials and a plane-wave basis set is presented and the application of Pulay's DIIS method to the iterative diagonalization of large matrices will be discussed.
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IBM1
TL;DR: An approach for electronic structure calculations is described that generalizes both the pseudopotential method and the linear augmented-plane-wave (LAPW) method in a natural way and can be used to treat first-row and transition-metal elements with affordable effort and provides access to the full wave function.
Abstract: An approach for electronic structure calculations is described that generalizes both the pseudopotential method and the linear augmented-plane-wave (LAPW) method in a natural way. The method allows high-quality first-principles molecular-dynamics calculations to be performed using the original fictitious Lagrangian approach of Car and Parrinello. Like the LAPW method it can be used to treat first-row and transition-metal elements with affordable effort and provides access to the full wave function. The augmentation procedure is generalized in that partial-wave expansions are not determined by the value and the derivative of the envelope function at some muffin-tin radius, but rather by the overlap with localized projector functions. The pseudopotential approach based on generalized separable pseudopotentials can be regained by a simple approximation.
61,450 citations
TL;DR: In this article, a method for generating sets of special points in the Brillouin zone which provides an efficient means of integrating periodic functions of the wave vector is given, where the integration can be over the entire zone or over specified portions thereof.
Abstract: A method is given for generating sets of special points in the Brillouin zone which provides an efficient means of integrating periodic functions of the wave vector. The integration can be over the entire Brillouin zone or over specified portions thereof. This method also has applications in spectral and density-of-state calculations. The relationships to the Chadi-Cohen and Gilat-Raubenheimer methods are indicated.
51,059 citations
TL;DR: A detailed description and comparison of algorithms for performing ab-initio quantum-mechanical calculations using pseudopotentials and a plane-wave basis set is presented in this article. But this is not a comparison of our algorithm with the one presented in this paper.
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