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Evidence of a hidden flux phase in the topological kagome metal CsV$_3$Sb$_5$

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 Added by Li Yu
 Publication date 2021
  fields Physics
and research's language is English




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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-$mu$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 charge density wave (CDW) phase present below ~ 95 K. By carrying out optical second-harmonic generation (SHG) experiments, we also find that inversion symmetry is maintained in the temperature range of interest. Combining all the experimental results and symmetry constraints, we conclude that the interlayer coupled chiral flux phase (CFP) is the most promising candidate for the TRSB state among all theoretical proposals of orbital current orders. Thus, this prototypical kagome metal CsV3Sb5 can be a platform to establish a TRSB current-ordered state and explore its relationship with CDW, giant AHE, and superconductivity.



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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 $Deltalambda(T)$ of CsV$_3$Sb$_5$ was measured down to 0.07 K. A clear exponential behavior in $Deltalambda(T)$ with marked deviations from a $T$ or $T^2$ temperature dependence is observed at low temperatures, indicating a deficiency of nodal quasiparticles. Temperature dependence of the superfluid density and electronic specific heat can be described by two-gap $s$-wave superconductivity, consistent with the presence of multiple Fermi surfaces in CsV$_3$Sb$_5$. These results evidence nodeless superconductivity in CsV$_3$Sb$_5$ under ambient pressure, and constrain the allowed pairing symmetry.
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.
Using first-principles calculations, we identify the origin of the observed charge density wave (CDW) formation in a layered kagome metal CsV$_3$Sb$_5$. It is revealed that the structural distortion of kagome lattice forming the trimeric and hexameric V atoms is accompanied by the stabilization of quasimolecular states, which gives rise to the opening of CDW gaps for the V-derived multibands lying around the Fermi level. This Jahn-Teller-like instability having the local lattice distortion and its derived quasimolecular states is a driving force of the CDW order. Specifically, the saddle points of multiple Dirac bands near the Fermi level, located at the $M$ point, are hybridized to disappear along the $k_z$ direction, therefore not supporting the widely accepted Peierls-like electronic instability due to Fermi surface nesting. It is further demonstrated that applied hydrostatic pressure significantly reduces the interlayer spacing to destabilize the quasimolecular states, leading to a disappearance of the CDW phase at a pressure of ${sim}$2 GPa. The presently proposed underlying mechanism of the CDW order in CsV$_3$Sb$_5$ can also be applicable to other isostructural kagome lattices such as KV$_3$Sb$_5$ and RbV$_3$Sb$_5$.
The recently discovered kagome superconductor CsV$_3$Sb$_5$ ($T_c simeq 2.5$ K) has been found to host charge order as well as a non-trivial band topology, encompassing multiple Dirac points and probable surface states. Such a complex and phenomenologically rich system is, therefore, an ideal playground for observing unusual electronic phases. Here, we report on microscopic studies of its anisotropic superconducting properties by means of transverse-field muon spin rotation ($mu$SR) experiments. The temperature dependences of the in-plane and out-of-plane components of the magnetic penetration depth $lambda_{ab}^{-2}(T)$ and $lambda_{c}^{-2}(T)$ indicate that the superconducting order parameter exhibits a two-gap ($s+s$)-wave symmetry, reflecting the multiple Fermi surfaces of CsV3Sb5. The multiband nature of its superconductivity is further validated by the different temperature dependences of the anisotropic magnetic penetration depth $gamma_lambda(T)$ and upper critical field $gamma_{rm B_{c2}}(T)$, both in close analogy with the well known two-gap superconductor MgB$_2$. Remarkably, the high value of the $T_c/lambda^{-2}(0)$ ratio in both field orientations strongly suggests the unconventional nature of superconductivity. The relaxation rates obtained from zero field $mu$SR experiments do not show noticeable change across the superconducting transition, indicating that superconductivity does not break time reversal symmetry.
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) 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.
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