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Stabilized FeSe thin films in ambient pressure with tunable superconducting critical temperature would be a promising candidate for superconducting electronic devices. By carefully controlling the depositions on twelve kinds of substrates using a pulsed laser deposition technique single crystalline FeSe thin films were fabricated. The high quality of the thin films was confirmed by X-ray diffraction with a full width at half maximum of 0.515° in the rocking curve and clear four-fold symmetry in φ -scan. The films have a maximum T c ~ 15 K on the CaF 2 substrate and were stable in ambient conditions air for more than half a year. Slightly tuning the stoichiometry of the FeSe targets, the superconducting critical temperature becomes adjustable below 15 K with quite narrow transition width less than 2 K. These FeSe thin films deposited on different substrates are optimized respectively. The T c of these optimized films show a relation with the out-of-plane ( c -axis) lattice parameter of the FeSe films.

The transition metal kagome lattice materials host frustrated, correlated and topological quantum states of matter 1 – 9 . Recently, a new family of vanadium-based kagome metals, AV 3 Sb 5 (A = K, Rb or Cs), with topological band structures has been discovered 10 , 11 . These layered compounds are nonmagnetic and undergo charge density wave transitions before developing superconductivity at low temperatures 11 – 19 . Here we report the observation of unconventional superconductivity and a pair density wave (PDW) in CsV 3 Sb 5 using scanning tunnelling microscope/spectroscopy and Josephson scanning tunnelling spectroscopy. We find that CsV 3 Sb 5 exhibits a V-shaped pairing gap Δ  ~ 0.5 meV and is a strong-coupling superconductor (2 Δ / k B T c  ~ 5) that coexists with 4 a 0 unidirectional and 2 a 0  × 2 a 0 charge order. Remarkably, we discover a 3Q PDW accompanied by bidirectional 4 a 0 /3 spatial modulations of the superconducting gap, coherence peak and gap depth in the tunnelling conductance. We term this novel quantum state a roton PDW associated with an underlying vortex–antivortex lattice that can account for the observed conductance modulations. Probing the electronic states in the vortex halo in an applied magnetic field, in strong field that suppresses superconductivity and in zero field above T c , reveals that the PDW is a primary state responsible for an emergent pseudogap and intertwined electronic order. Our findings show striking analogies and distinctions to the phenomenology of high- T c cuprate superconductors, and provide groundwork for understanding the microscopic origin of correlated electronic states and superconductivity in vanadium-based kagome metals. A study reports unconventional superconductivity and a pair density wave in the kagome superconductor CsV 3 Sb 5 , and provides a basis for understanding the microscopic origin of correlated electronic states and superconductivity in vanadium-based kagome metals.

Superconducting FeSe single crystals of (001) orientation are synthesized via a hydrothermal ion-release route. An Ising spin-nematic order is identified by our systematic measurements of in-plane angular-dependent magnetoresistance (AMR) and static magnetization. The turn-on temperature of anisotropic AMR signifies the Ising spin-nematic ordering temperature Tsn, below which a two-fold rotational symmetry is observed in the iron plane. A downward curvature appears below Tsn in the temperature dependence of static magnetization for the weak in-plane magnetic field as reported previously. Remarkably, we find a universal linear relationship between Tc and Tsn among various superconducting samples, indicating that the spin nematicity and the superconductivity in FeSe have a common microscopic origin.

The magneto-transport properties are systematically measured under c-direction fields up to 33 T for a series of single-crystal films of intercalated iron-selenide superconductor (Li,Fe)OHFeSe. The film samples with varying degree of disorder are grown hydrothermally. We observe a magnetic-field-enhanced shoulder-like feature in the mixed state of the high-Tc (Li,Fe)OHFeSe films with weak disorder, while the feature fades away in the films with enhanced disorder. The irreversibility field is significantly suppressed to lower temperatures with the appearance of the shoulder feature. Based on the experiment and model analysis, we establish a new vortex phase diagram for the weakly disordered high-Tc (Li,Fe)OHFeSe, which features an emergent dissipative vortex phase intermediate between the common vortex glass and liquid phases. The reason for the emergence of this intermediate vortex state is further discussed based on related experiments and models.

The transition-metal kagome lattice materials host frustrated, correlated, and topological quantum states of matter. Recently, a new family of vanadium-based kagome metals AV3Sb5 (A=K, Rb, and Cs) with topological band structures has been discovered. These layered compounds are nonmagnetic and undergo charge density wave transitions before developing superconductivity at low temperatures. Here we report the observation of unconventional superconductivity and pair density wave (PDW) in CsV3Sb5 using scanning tunneling microscope/spectroscopy (STM/STS) and Josephson STS. We find that CsV3Sb5 exhibits a V-shaped pairing gap {\\Delta}~0.5 meV and is a strong-coupling superconductor (2{\\Delta}/kBTc~5) that coexists with 4a0 unidirectional and 2a0X2a0 charge order. Remarkably, we discover a 3Q PDW accompanied by bidirectional 4a0/3 spatial modulations of the superconducting gap, coherence peak and gap-depth in the tunneling conductance. We term this novel quantum state a roton-PDW associated with an underlying vortex-antivortex lattice that can account for the observed conductance modulations. Probing the electronic states in the vortex halo in an applied magnetic field, in strong-field that suppresses superconductivity, and in zero-field above Tc reveals that the PDW is a primary state responsible for an emergent pseudogap and intertwined electronic order. Our findings show striking analogies and distinctions to the phenomenology of high-Tc cuprate superconductors, and provide groundwork for understanding the microscopic origin of correlated electronic states and superconductivity in vanadium-based kagome metals.

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.

Critical current density (Jc) is one of the major limiting factors for high field applications of iron-based superconductors. Here, we report that Mn-ions are successfully incorporated into nontoxic superconducting (Li,Fe)OHFeSe films. Remarkably, the Jc is significantly enhanced from 0.03 to 0.32 MA/cm^2 under 33 T, and the vortex pinning force density monotonically increases up to 106 GN/m^3, which is the highest record so far among all iron-based superconductors. Our results demonstrate that Mn incorporation is an effective method to optimize the performance of (Li,Fe)OHFeSe films, offering a promising candidate for high-field applications.

The superconducting film of (Li1-xFex)OHFeSe is reported for the first time. The thin film exhibits a small in-plane crystal mosaic of 0.22 deg, in terms of the FWHM (full-width-at-half-maximum) of x-ray rocking curve, and an excellent out-of-plane orientation by x-ray phi-scan. Its bulk superconducting transition temperature (Tc) of 42.4 K is characterized by both zero electrical resistance and diamagnetization measurements. The upper critical field (Hc2) is estimated to be 79.5 T and 443 T, respectively, for the magnetic field perpendicular and parallel to the ab plane. Moreover, a large critical current density (Jc) of a value over 0.5 MA/cm2 is achieved at ~20 K. Such a (Li1-xFex)OHFeSe film is therefore not only important to the fundamental research for understanding the high-Tc mechanism, but also promising in the field of high-Tc superconductivity application, especially in high-performance electronic devices and large scientific facilities such as superconducting accelerator.

The phenomenon of phase separation into antiferromagnetic (AFM) and superconducting (SC) or normal-state regions has great implication for the origin of high-temperature (high-Tc) superconductivity. However, the occurrence of an intrinsic antiferromagnetism above the Tc of (Li, Fe)OHFeSe superconductor is questioned. Here we report a systematic study on a series of (Li, Fe)OHFeSe single crystal samples with Tc up to ~41 K. We observe an evident drop in the static magnetization at Tafm ~125 K, in some of the SC (Tc < ~38 K, cell parameter c < ~9.27 Å) and non-SC samples. We verify that this AFM signal is intrinsic to (Li, Fe)OHFeSe. Thus, our observations indicate mesoscopic-to-macroscopic coexistence of an AFM state with the normal (below Tafm) or SC (below Tc) state in (Li, Fe)OHFeSe. We explain such coexistence by electronic phase separation, similar to that in high-Tc cuprates and iron arsenides. However, such an AFM signal can be absent in some other samples of (Li, Fe)OHFeSe, particularly it is never observed in the SC samples of Tc > ~38 K, owing to a spatial scale of the phase separation too small for the macroscopic magnetic probe. For this case, we propose a microscopic electronic phase separation. It is suggested that the microscopic static phase separation reaches vanishing point in high-Tc (Li, Fe)OHFeSe, by the occurrence of two-dimensional AFM spin fluctuations below nearly the same temperature as Tafm reported previously for a (Li, Fe)OHFeSe (Tc ~42 K) single crystal. A complete phase diagram is thus established. Our study provides key information of the underlying physics for high-Tc superconductivity.

We report the success in introducing Mn into (Li1-xFex)OHFe1-ySe superconducting crystals by applying two different hydrothermal routes, ion exchange (1-Step) and ion release/introduction (2-Step). The micro-region x-ray diffraction and energy dispersive x-ray spectroscopy analyses indicate that the Mn has been doped into the lattice, and its content in the 1-Step fabricated sample is higher than that in the 2-Step one. Magnetic susceptibility and electric transport properties reveal that Mn doping influences little on the superconducting transition, regardless of 1-Step or 2-Step routes. By contrast, the characteristic temperature, T*, where the negative Hall coefficient reaches its minimum, is significantly reduced by Mn doping. This implies that the reduction of the hole carriers contribution is obviously modified, and hence the hole band might have no direct relationship with the superconductivity in (Li1-xFex)OHFe1-ySe superconductors. Our present hydrothermal methods of ion exchange and ion release/introduction provide an efficient way for elements substitution/doping into (Li1-xFex)OHFe1-ySe superconductors, which will promote the in-depth investigations on the role of multiple electron and hole bands and their interplay with the high-temperature superconductivity in the FeSe-based superconductors.