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FeSe$_{1-x}$S$_{x}$ superconductors are commonly considered layered van der Waals materials with negligible inter-layer coupling. Here, using inelastic neutron scattering to study spin excitations in single-crystal samples, we reveal that the magnetic coupling between adjacent Fe layers is not only significant, as it affects excitations up to \textcolor{black}{15} meV, but also ferromagnetic in nature, making the system different from most unconventional superconductors including iron pnictides. Our observation provides a new standpoint to understand the absence of magnetic order in FeSe$_{1-x}$S$_{x}$. Since intercalating between the Fe layers is known to enhance superconductivity and suppress the inter-layer coupling, superconductivity appears to be a more robust phenomenon in the two-dimensional limit than antiferromagnetic order.

A series of tetragonal Fe$_{1-x}$Co${_x}$Se single crystals with a complete Co doping range (0$\leq$x$\leq$0.52) up to its solid solubility limit in FeSe have been grown by an eutectic AlCl${_3}$/KCl molten salt method. The typical lateral size of as-grown Fe$_{1-x}$Co${_x}$Se single crystals is 1$-$5 mm. The chemical composition and homogeneity of the crystals was examined by both inductively coupled plasma atomic emission spectroscopy and energy dispersive spectrometer. X-ray diffraction analysis demonstrates that the crystal lattice parameters $a$ and $c$ are both linearly decreased with increasing Co doping level x. In the whole doping range, all the samples show metallic behaviour in contrast to a metal insulator transition of Cu-doped FeSe according to the resistivity measurements

An eutectic AlCl$_3$/KCl molten salt method in a horizontal configuration was employed to grow millimeter-sized and composition homogeneous CuFeSe$_2$ single crystals due to the continuous growth process in a temperature gradient induced solution convection. The typical as-grown CuFeSe$_2$ single crystals in cubic forms are nearly 1.6$\times$1.2$\times$1.0 mm3 in size. The chemical composition and homogeneity of the crystals was examined by both inductively coupled plasma atomic emission spectroscopy and energy dispersive spectrometer with Cu:Fe:Se = 0.96:1.00:1.99 consistent with the stoichiometric composition of CuFeSe$_2$. The magnetic measurements suggest a ferrimagnetic or weak ferromagnetic transition below T$_C$ = 146 K and the resistivity reveals a semiconducting behavior and an abrupt increase below T$_C$.

There are few inelastic neutron scattering (INS) reports on the superconducting single crystals of FeAs-1111 system, even though it was first discovered in 2008, due to the extreme difficulty in large single crystal growth. In this paper, we have studied the low-energy spin excitations in the optimally electron-doped CaFe$_{0.88}$Co$_{0.12}$AsF single crystals with $T_\mathrm{c}$ = 21 K by INS. The resonance energy of the superconducting spin resonant mode with $E_\mathrm{r}$ = 12 meV amounts to 6.6 $k_\mathrm{B}$$T_\mathrm{c}$, which constitutes the largest $E_\mathrm{r}$/$k_\mathrm{B}$$T_\mathrm{c}$ ratio among iron-based superconductors reported to date. The large ratio implies a strong coupling between conduction electrons and magnetic excitations in CaFe$_{0.88}$Co$_{0.12}$AsF. The resonance possesses a magnonlike upward dispersion along transverse direction due to the anisotropy of spin-spin correlation length within $ab$ plane in the normal-state, which points to a spin fluctuation mediated sign-reversed ${s}\mathbf\pm$ wave pairing in CaFe$_{0.88}$Co$_{0.12}$AsF.

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.

An unaddressed challenge in multi-agent coordination is to enable AI agents to exploit the semantic relationships between the features of actions and the features of observations. Humans take advantage of these relationships in highly intuitive ways. For instance, in the absence of a shared language, we might point to the object we desire or hold up our fingers to indicate how many objects we want. To address this challenge, we investigate the effect of network architecture on the propensity of learning algorithms to exploit these semantic relationships. Across a procedurally generated coordination task, we find that attention-based architectures that jointly process a featurized representation of observations and actions have a better inductive bias for learning intuitive policies. Through fine-grained evaluation and scenario analysis, we show that the resulting policies are human-interpretable. Moreover, such agents coordinate with people without training on any human data., Comment: ICML 2023

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 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

Here we establish a combined electronic phase diagram of isoelectronic FeSe1-xSx (0.19 > x > 0.0) and FeSe1-yTey (0.04 < y < 1.0) single crystals. The FeSe1-yTey crystals with y = 0.04 - 0.30 are grown by a hydrothermal ion-deintercalation (HID) method. Based on combined experiments of the specific heat, electrical transport, and angle-resolved photoemission spectroscopy, no signature of the tetragonal-symmetry-broken transition to orthorhombic (nematic) phase is observed in the HID FeSe1-yTey samples, as compared with the FeSe1-xSx samples showing this transition at Ts. A ubiquitous dip-like temperature dependence of the Hall coefficient is observed around a characteristic temperature T* in the tetragonal regimes, which is well above the superconducting transition. More importantly, we find that the superconducting transition temperature Tc is positively correlated with the Hall-dip temperature T* across the FeSe1-xSx and FeSe1-yTey systems, suggesting that the tetragonal background is a fundamental host for the superconductivity., Comment: 18 pages, 5 figures

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 {\AA}) 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., Comment: 13 pages, 5 figures

Chemical substitution during growth is a well-established method to manipulate electronic states of quantum materials, and leads to rich spectra of phase diagrams in cuprate and iron-based superconductors. Here we report a novel and generic strategy to achieve nonvolatile electron doping in series of (i.e. 11 and 122 structures) Fe-based superconductors by ionic liquid gating induced protonation at room temperature. Accumulation of protons in bulk compounds induces superconductivity in the parent compounds, and enhances the Tc largely in some superconducting ones. Furthermore, the existence of proton in the lattice enables the first proton nuclear magnetic resonance (NMR) study to probe directly superconductivity. Using FeS as a model system, our NMR study reveals an emergent high-Tc phase with no coherence peak which is hard to measure by NMR with other isotopes. This novel electric-field-induced proton evolution opens up an avenue for manipulation of competing electronic states (e.g. Mott insulators), and may provide an innovative way for a broad perspective of NMR measurements with greatly enhanced detecting resolution., Comment: 11 pages, 4 figures, published, http://engine.scichina.com/publisher/scp/journal/SB/63/1/10.1016/j.scib.2017.12.009?slug=full text

We report an inelastic neutron scattering study of single crystals of (Li$_{0.8}$Fe$_{0.2}$)ODFeSe. Temperature-dependent low-energy spin excitations are observed near $\mathbf{Q}=$ (0.5, 0.27, 0.5) and equivalent wave vectors symmetrically surrounding $\mathbf{Q}=$ (0.5, 0.5, 0.5) in the 1-Fe Brillouin zone, consistent with a Fermi-surface-nesting description. The excitations are broadly distributed in energy, ranging from 16 to 35 meV. Upon cooling below the superconducting critical temperature ($T_\mathrm{c}$), magnetic response below twice the superconducting gap $2\Delta_\mathrm{SC}$ exhibits an abrupt enhancement, consistent with the notion of spin resonance, whereas the response at higher energies increases more gradually with only a weak anomaly at $T_\mathrm{c}$. Our results suggest that (Li$_{0.8}$Fe$_{0.2}$)ODFeSe might be on the verge of a crossover between different Cooper-pairing channels with distinct symmetries., Comment: 5 pages, 4 figures

In most existing theories for iron-based superconductors, spin-orbit coupling (SOC) has been assumed insignificant. Even though recent experiments have revealed an influence of SOC on the electronic band structure, whether SOC fundamentally affects magnetism and superconductivity remains an open question. Here we use spin-polarised inelastic neutron scattering to show that collective low-energy spin fluctuations in the orthorhombic (or "nematic") phase of FeSe possess nearly no in-plane component. Such spin-space anisotropy can only be caused by SOC. It is present over an energy range greater than the superconducting gap 2$\Delta _\mathrm{sc}$ and gets fully inherited in the superconducting state, resulting in a distinct $c$-axis polarised "spin resonance". Our result demonstrates the importance of SOC in defining the low-energy spin excitations in FeSe, which helps to elucidate the nearby magnetic instabilities and the debated interplay between spin and orbital degrees of freedom. The prominent role of SOC also implies a possible unusual nature of the superconducting state.

Elucidating the microscopic origin of nematic order in iron-based superconducting materials is important because the interactions that drive nematic order may also mediate the Cooper pairing. Nematic order breaks fourfold rotational symmetry in the iron plane, which is believed to be driven by either orbital or spin degrees of freedom. However, as the nematic phase often develops at a temperature just above or coincides with a stripe magnetic phase transition, experimentally determining the dominant driving force of nematic order is difficult. Here, we use neutron scattering to study structurally the simplest iron-based superconductor FeSe, which displays a nematic (orthorhombic) phase transition at $T_s=90$ K, but does not order antiferromagnetically. Our data reveal substantial stripe spin fluctuations, which are coupled with orthorhombicity and are enhanced abruptly on cooling to below $T_s$. Moreover, a sharp spin resonance develops in the superconducting state, whose energy (~4 meV) is consistent with an electron boson coupling mode revealed by scanning tunneling spectroscopy, thereby suggesting a spin fluctuation-mediated sign-changing pairing symmetry. By normalizing the dynamic susceptibility into absolute units, we show that the magnetic spectral weight in FeSe is comparable to that of the iron arsenides. Our findings support recent theoretical proposals that both nematicity and superconductivity are driven by spin fluctuations., Comment: 19 pages, 8 figures

A large and high-quality single crystal (Li0.84Fe0.16)OHFe0.98Se, the optimal superconductor of newly reported (Li1-xFex)OHFe1-ySe system, has been successfully synthesized via a hydrothermal ion-exchange technique. The superconducting transition temperature (Tc) of 42 K is determined by magnetic susceptibility and electric resistivity measurements, and the zero-temperature upper critical magnetic fields are evaluated as 79 and 313 Tesla for the field along the c-axis and the ab-plane, respectively. The ratio of out-of-plane to in-plane electric resistivity,\r{ho}c/\r{ho}ab, is found to increases with decreasing temperature and to reach a high value of 2500 at 50 K, with an evident kink occurring at a characteristic temperature T*=120 K. The negative in-plane Hall coefficient indicates that electron carriers dominate in the charge transport, and the hole contribution is significantly reduced as the temperature is lowered to approach T*. From T* down to Tc, we observe the linear temperature dependences of the in-plane electric resistivity and the magnetic susceptibility for the FeSe layers. Our findings thus reveal that the normal state of (Li0.84Fe0.16)OHFe0.98Se becomes highly two-dimensional and anomalous prior to the superconducting transition, providing a new insight into the mechanism of high-Tc superconductivity., Comment: 11 pages, 4 figures, supplementary information is not uploaded

A flux-free solution to the growth of large and composition homogeneous superconducting FeSe crystal is reported for the first time, which is based on the traveling-solvent floating-zone technique. The size of the crystal samples prepared by this approach is up to 15x6x2 mm3, being far bigger than previously reported in all dimensions, and the main phase of the crystals is of a single preferred orientation along the tetragonal (101) plane. X-ray diffraction analysis identifies the main phase to be the superconducting tetragonal \b{eta}-FeSe. The superconducting transition temperature (TC) is determined to be 9.4 K by AC magnetic susceptibility and electronic transport measurements. A nearly perfect diamagnetic shielding of -97% is observed, indicating a bulk superconductivity in the crystal sample., Comment: 14 pages, 5 figures