Electronic Phase Separation in Iron Selenide(Li,Fe)OHFeSe Superconductor System

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-T_c) superconductivity. However, the occurrence of an intrinsic antiferromagnetism above the T_c of(Li,Fe)OHFe Se superconductor is questioned. Here we report a systematic study on a series of(Li,Fe)OHFe Se single crystal samples with T_c up to ～41 K. We observe an evident drop in the static magnetization at T_(afm) ～ 125 K, in some of the SC(T_c 38 K, cell parameter c■9.27 ?) and non-SC samples. We verify that this AFM signal is intrinsic to(Li,Fe)OHFe Se. Thus, our observations indicate mesoscopic-to-macroscopic coexistence of an AFM state with the normal(below T_(afm)) or SC(below T_c) state in(Li,Fe)OHFe Se. We explain such coexistence by electronic phase separation, similar to that in high-T_c cuprates and iron arsenides. However, such an AFM signal can be absent in some other samples of(Li,Fe)OHFe Se, particularly it is never observed in the SC samples of T_c 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. The occurrence of two-dimensional AFM spin fluctuations below nearly the same temperature as T_(afm), reported previously for a(Li,Fe)OHFe Se(T_c ～ 42 K) single crystal, suggests that the microscopic static phase separation reaches vanishing point in high T_c(Li,Fe)OHFe Se. A complete phase diagram is thus established. Our study provides key information of the underlying physics for high-T_c superconductivity.     

Effect of Mn substitution on superconductivity in iron selenide(Li,Fe)OHFeSe single crystals

We synthesize a series of Mn substituted(Li, Fe)OHFeSe superconductor single crystals via a modified ion-exchange method, with the Mn concentration z(the atomic ratio of Mn:Se) ranging from 0 to 0.07. The distribution homogeneity of the Mn element incorporated into the lattice of(Li, Fe)OHFeSe is checked by combined measurements of high-angleannular-dark-field(HAADF) imaging and electron energy-loss spectroscopy(EELS). Interestingly, we find that the superconducting transition temperature T_c and unit cell parameter c of the Mn-doped(Li, Fe)OHFeSe samples display similar V-shaped evolutions with the increasing dopant concentration z. We propose that, with increasing doping level, the Mn dopant first occupies the tetrahedral sites in the(Li, Fe)OH layers before starting to substitute the Fe element in the superconducting Fe Se layers, which accounts for the V-shaped change in cell parameter c. The observed positive correlation between the T_c and lattice parameter c, regardless of the Mn doping level z, indicates that a larger interlayer separation, or a weaker interlayer coupling, is essential for the high-T_c superconductivity in(Li, Fe)OHFeSe. This agrees with our previous observations on powder, single crystal, and film samples of(Li, Fe)OHFeSe superconductors.     

Distinction between critical current effects and intrinsic anomalies in the point-contact Andreev reflection spectra of unconventional superconductors

In this work,we discuss the origin of several anomalies present in the point-contact Andreev reflection spectra of(Li_(1-x)Fe_x)OHFeSe,LiTi_2O_4,and La_(2-x)Ce_xCuO_4.While these features are similar to those stemming from intrinsic superconducting properties,such as Andreev reflection,electron-boson coupling,multigap superconductivity,d-wave and p-wave pairing symmetry,they cannot be accounted for by the modified Blonder–Tinkham–Klapwijk(BTK) model,but require to consider critical current effects arising from the junction geometry.Our results point to the importance of tracking the evolution of the dips and peaks in the differential conductance as a function of the bias voltage,in order to correctly deduce the properties of the superconducting state.     

Synthesis of large FeSe superconductor crystals via ion release/introduction and property characterization

Large superconducting Fe Se crystals of(001) orientation have been prepared via a hydrothermal ion release/introduction route for the first time. The hydrothermally derived Fe Se crystals are up to 10 mm×5 mm×0.3 mm in dimension. The pure tetragonal FeSe phase has been confirmed by x-ray diffraction(XRD) and the composition determined by both inductively coupled plasma atomic emission spectroscopy(ICP-AES) and energy dispersive x-ray spectroscopy(EDX). The superconducting transition of the Fe Se samples has been characterized by magnetic and transport measurements. The zero-temperature upper critical field H_(c2) is calculated to be 13.2–16.7 T from a two-band model. The normal-state cooperative paramagnetism is found to be predominated by strong spin frustrations below the characteristic temperature T_(sn), where the Ising spin nematicity has been discerned in the FeSe superconductor crystals as reported elsewhere.     

Doping Mn into(Li_(1-x)Fe_x)OHFe_(1-y)Se superconducting crystals via ion-exchange and ion-release/introduction syntheses

We report the success in introducing Mn into(Li_(1-_x)Fe_x)OHFe_(1-y) Se superconducting crystals by applying two different hydrothermal routes, ion e_xchange(1-step) and ion release/introduction(2-step). The micro-region _x-ray diffraction and energy dispersive _x-ray spectroscopy analyses indicate that 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*, at which the negative Hall coefficient reaches its minimum, is significantly reduced by Mn doping.This implies that the hole carriers contribution is obviously modified, and hence the hole band might have no direct relationship with the superconductivity in(Li_(1-_x)Fe_x)OHFe_(1-y) Se superconductors. Our present hydrothermal methods of ion e_xchange and ion release/introduction provide an efficient way for elements substitution/doping into(Li_(1-_x)Fe_x)OHFe_(1-y) Se 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.     

铁硒基超导研究新进展:高质量(Li,Fe)OHFeSe单晶薄膜

单晶薄膜形态的高温超导材料对于相关基础科学研究和应用开发都极为重要.多带的铁基高温超导体往往呈现丰富的物理现象,并具有较高的超导临界参数.特别是近年发现的插层（Li,Fe）OHFeSe超导体,无论对高温超导机理还是应用研究而言,都日益受到重视,已成为铁基家族中重要的典型材料.但是,该化合物含有OH键,加热易分解.因此,现有的常规高温成膜技术均不适用于生长该薄膜材料.为解决这一生长难题,我们最近发明了基体辅助水热外延生长法,实现了超导薄膜制备技术上的突破.本文简要介绍用此软化学成膜技术首次成功制备出（Li,Fe）OHFeSe单晶薄膜.该薄膜材料具有优良的结晶质量和较高的超导临界参数,特别是其高的临界电流密度和上临界场对应用开发有实际价值.因此,（Li,Fe）OHFeSe超导单晶薄膜的成功合成,为机理研究和应用开发分别提供了重要的实验载体和备选材料.另外,该薄膜技术也有望应用于其他功能材料的探索与合成,尤其是对常规手段难以获取的材料更具重大价值.     

插层FeSe高温超导体的高压研究进展

通过对FeSe进行化学插层可以将其超导转变温度（T_c）从约8 K提高到40 K以上,实现高温超导电性.最近,我们对两种插层FeSe高温超导材料（Li_0.84Fe_0.16）OHFe_0.98Se和Li_0.36（NH₃）_yFe₂Se₂开展了高压调控研究,发现压力会首先抑制高温超导相（称为SC-I相）,然后在临界压力P_c以上诱导出第二个高温超导相（称为SC-Ⅱ相）,呈现出双拱形T-P超导相图.这两个体系的P_c分别约为5和2 GPa,两个体系SC-Ⅱ相的最高T_c分别可以达到约52和55 K,比相应SC-I相的初始T_c提高了10 K.对（Li_0.84Fe_0.16）OHFe_0.98Se的正常态电输运性质分析表明,SC-I和SC-Ⅱ相的正常态分别具有费米液体和非费米液体行为,意味着这两个超导相可能存在显著差异.此外,还发现这两个体系的SC-Ⅱ相的T_c与霍尔系数倒数1/R_H（∝载流子浓度n_e）具有很好的线性依赖关系.对（Li_0.84Fe_0.16）OHFe_0.98Se的高压X射线衍射测量排除了其在10 GPa以内发生结构相变的可能,因此P_c以上SC-Ⅱ相的出现和载流子浓度的增加很可能起源于压力导致的费米面重构.