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Revealing the energy and spatial characteristics of impurity induced states in superconductors is essential for understanding their mechanism and fabricating new quantum state by manipulating impurities. Here by using high-resolution scanning tunneling microscopy/spectroscopy, we investigated the spatial distribution and magnetic field response of the impurity states in (Li1-xFex)OHFeSe. We detected two pairs of strong in-gap states on the "dumbbell" shaped defects. They display clear damped oscillations with different phase shifts and a direct phase-energy correlation. These features have long been predicted for classical Yu-Shiba-Rusinov (YSR) state, which are demonstrated here with unprecedented resolution for the first time. Moreover, upon applying magnetic field, all the in-gap state peaks remarkably split into two rather than shift, and the splitting strength is field orientation dependent. Via detailed numerical model calculations, we found such anisotropic splitting behavior can be naturally induced by a high-spin impurity coupled to anisotropic environment, highlighting how magnetic anisotropy affects the behavior of YSR states., Comment: Main text with supplementary (accepted by Phys. Rev. Lett.)

Intertwined spin and charge orders have been widely studied in high-temperature superconductors, since their fluctuations may facilitate electron pairing; however, they are rarely identified in heavily electron-doped iron selenides. Here, using scanning tunneling microscopy, we show that when the superconductivity of (Li0.84Fe0.16OH)Fe1-xSe is suppressed by introducing Fe-site defects, a short-ranged checkerboard charge order emerges, propagating along the Fe-Fe directions with an approximately 2aFe period. It persists throughout the whole phase space tuned by Fe-site defect density, from a defect-pinned local pattern in optimally doped samples to an extended order in samples with lower Tc or non-superconducting. Intriguingly, our simulations indicate that the charge order is likely driven by multiple-Q spin density waves originating from the spin fluctuations observed by inelastic neutron scattering. Our study proves the presence of a competing order in heavily electron-doped iron selenides, and demonstrates the potential of charge order as a tool to detect spin fluctuations., Comment: 16 pages, 5 figures

We report the observation for the p$_{z}$ electron band and the band inversion in Fe$_{1+y}$Te$_{x}$Se$_{1-x}$ with angle-resolved photoemission spectroscopy. Furthermore, we found that excess Fe (y>0) inhibits the topological band inversion in Fe$_{1+y}$Te$_{x}$Se$_{1-x}$, which explains the absence of Majorana zero modes in previous reports for Fe$_{1+y}$Te$_{x}$Se$_{1-x}$ with excess Fe. Based on our analysis of different amounts of Te doping and excess Fe, we propose a delicate topological phase in this material. Thanks to this delicate phase, one may be able to tune the topological transition via applying lattice strain or carrier doping.

The intercalated iron selenide (Li,Fe)OHFeSe has a strongly layered structure analogous to the quasi two-dimensional (2D) bismuth cuprate superconductors, and exhibits both high-temperature (Tc) and topological superconductivity. However, the issue of its superconductivity dimensionality has not yet been fully investigated so far. Here we report that the quasi-2D superconductivity features, including the high anisotropy {\gamma} = 151 and the associated quasi-2D vortices, are also revealed for (Li,Fe)OHFeSe, based on systematic experiments of the electrical transport and magnetization and model fittings. Thus, we establish a new vortex phase diagram for (Li,Fe)OHFeSe, which delineates an emergent quasi-2D vortex-liquid state, and a subsequent vortex-solid dimensional crossover from a pancake-like to a three-dimensional state with decreasing temperature and magnetic field. Furthermore, we find that all the quasi-2D characteristics revealed here for the high-Tc iron selenide superconductor are very similar to those reported for the high-Tc bismuth cuprate superconductors., Comment: 20 pages, 6 figures

Using angle-resolved photoemission spectroscopy (ARPES), we studied the evolution of the electronic structure of Fe1-xCuxSe from x = 0 to 0.10. We found that the Cu dopant introduces extra electron carriers. The hole bands near the gamma point are observed to steadily shift downward with increasing doping and completely sink down below the Fermi level (EF) for x > 0.05. Meanwhile, the electron pocket near the M point becomes larger but loses the spectral weight near EF. We also observed that effective mass of the electron band near the M point increases with doping. Our result explains why superconductivity disappears and metal insulator transition (MIT) like behavior occurs upon Cu doping in terms of electronic structure, and provide insight into emergent magnetic fluctuation in Fe1-xCuxSe.

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. Here, we report, for the first time, the synthesis of Ti-substituted CsV3Sb5 single crystals and its rich phase diagram mapping the evolution of intertwining electronic states. The Ti atoms directly substitute for V in the kagome layers. CsV3-xTixSb5 shows two distinct SC phases upon substitution. The Ti slightly-substituted phase displays an unconventional V-shaped SC gap, coexisting with weakening CDW, PDW, AHE, and nematicity. The Ti highly-substituted phase has a U-shaped SC gap concomitant with a short-range rotation symmetry breaking CDW, while long-range CDW, twofold symmetry of in-plane resistivity, AHE, and PDW are absent. Furthermore, we also demonstrate the chemical substitution of V atoms with other elements such as Cr and Nb, showing a different modulation on the SC phase and CDWs. These findings open up a way to synthesise a new family of doped CsV3Sb5 materials, and further representing a new platform for tuning the different correlated electronic states and superconducting pairing in kagome superconductors., Comment: Science Bulletin (2022,in press)

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., Comment: 17 pages, 3 figures

The angular-dependent magnetoresistance (AMR) of the ab plane is measured on the single crystals of FeSe1-xSx (x = 0, 0.07, 0.13 and 1) and FeSe1-yTey (y = 0.06, 0.61 and 1) at various temperatures under fields up to 9 T. A pronounced twofold-anisotropic carrier-scattering effect is identified by AMR, and attributed to a magnetic-field-induced spin nematicity that emerges from the tetragonal normal-state regime below a characteristic temperature Tsn. This magnetically polarized spin nematicity is found to be ubiquitous in the isoelectronic FeSe1-xSx and FeSe1-yTey systems, no matter whether the sample shows an electronic nematic order at Ts < Tsn, or an antiferromagnetic order at TN < Tsn, or neither order. Importantly, we find that the isoelectronic substitution with sulfur does not suppress but even enhances the characteristic Tsn of the induced spin nematicity in FeSe1-xSx samples. This contrasts sharply with their rapidly suppressed Ts, the transition temperature of the spontaneous electronic nematicity. Furthermore, we find that the superconductivity is significantly suppressed with the enhancement of the induced spin nematicity in both FeSe1-xSx and FeSe1-yTey samples., Comment: 13 pages, 5 figures, plus supplemental material

The electronic and superconducting properties of Fe1-xSe single-crystal flakes grown hydrothermally are studied by the transport measurements under zero and high magnetic fields up to 38.5 T. The results contrast sharply with those previously reported for nematically ordered FeSe by chemical-vapor-transport (CVT) growth. No signature of the electronic nematicity, but an evident metal-to-nonmetal crossover with increasing temperature, is detected in the normal state of the present hydrothermal samples. Interestingly, a higher superconducting critical temperature Tc of 13.2 K is observed compared to a suppressed Tc of 9 K in the presence of the nematicity in the CVT FeSe. Moreover, the upper critical field in the zero-temperature limit is found to be isotropic with respect to the field direction and to reach a higher value of ~42 T, which breaks the Pauli limit by a factor of 1.8., Comment: 11 pages, 3 figures

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 $\Gamma$ point and along the $\Gamma$-$K$ direction. Such momentum dependence indicates that the CDW is driven by the scattering of electrons between neighboring $M$ points, where the band structure hosts multiple saddle points and the density of state diverges near the Fermi level. Our observations of the partially gapped Fermi surface and strongly momentum-dependent CDW gap not only provide a foundation for uncovering the mechanism of CDW in CsV$_3$Sb$_5$, but also shed light on the understanding of how the CDW coexists with superconductivity in this topological Kagome superconductor., Comment: 10 pages, 4 figures

We systematically measure the superconducting (SC) and mixed state properties of high-quality CsV3Sb5 single crystals with Tc ~ 3.5 K. We find that the upper critical field Hc2(T) exhibits a large anisotropic ratio of Hc2^(ab)/Hc2^(c) ~ 9 at zero temperature and fitting its temperature dependence requires a minimum two-band effective model. Moreover, the ratio of the lower critical field, Hc1^(ab)/Hc1^(c), is also found to be larger than 1, which indicates that the in-plane energy dispersion is strongly renormalized near Fermi energy. Both Hc1(T) and SC diamagnetic signal are found to change little initially below Tc ~ 3.5 K and then to increase abruptly upon cooling to a characteristic temperature of ~2.8 K. Furthermore, we identify a two-fold anisotropy of in-plane angular-dependent magnetoresistance in the mixed state. Interestingly, we find that, below the same characteristic T ~ 2.8 K, the orientation of this two-fold anisotropy displays a peculiar twist by an angle of 60o characteristic of the Kagome geometry. Our results suggest an intriguing superconducting state emerging in the complex environment of Kagome lattice, which, at least, is partially driven by electron-electron correlation., Comment: 11 pages, 4 figures