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High-temperature superconductivity and a wide variety of exotic superconducting states discovered in FeSe-based materials have been at the frontier of research on condensed matter physics over the past decade. Unique properties originating from the multiband electronic structure, strongly orbital-dependent phenomena, extremely small Fermi energy, electronic nematicity, and topological aspects give rise to many distinct and fascinating superconducting states. Here, we provide an overview of our current understanding of the superconductivity of {it bulk} FeSe-based materials, focusing on FeSe and the isovalent substituted FeSe$_{1-x}$S$_{x}$ and FeSe$_{1-x}$Te$_{x}$. We discuss the highly nontrivial superconducting properties in FeSe, including extremely anisotropic pairing states, crossover phenomena from Bardeen--Cooper--Schrieffer (BCS) to Bose--Einstein condensation (BEC) states, a novel field-induced superconducting phase, and broken time-reversal symmetry. We also discuss the evolution of the superconducting gap function with sulfur and tellurium doping, paying particular attention to the impact of quantum critical nematic fluctuations and the topological superconductivity. FeSe-based materials provide an excellent playground to study various exotic superconducting states.
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A general feature of unconventional superconductors is the existence of a superconducting dome in the phase diagram as a function of carrier concentration. For the simplest iron-based superconductor FeSe (with transition temperature Tc ~ 8 K), its Tc can be greatly enhanced by doping electrons via many routes, even up to 65 K in monolayer FeSe/SiTiO3. However, a clear phase diagram with carrier concentration for FeSe-derived superconductors is still lacking. Here, we report the observation of a series of discrete superconducting phases in FeSe thin flakes by continuously tuning carrier concentration through the intercalation of Li and Na ions with a solid ionic gating technique. Such discrete superconducting phases are robust against the substitution of Se by 20% S, but are vulnerable to the substitution of Fe by 2% Cu, highlighting the importance of the iron site being intact. A complete superconducting phase diagram for FeSe-derivatives is given, which is distinct from other unconventional superconductors.
Superconductivity arises from two distinct quantum phenomena: electron pairing and long-range phase coherence. In conventional superconductors, the two quantum phenomena generally take place simultaneously, while the electron pairing occurs at higher temperature than the long-range phase coherence in the underdoped high-Tc cuprate superconductors. Recently, whether electron pairing is also prior to long-range phase coherence in single-layer FeSe film on SrTiO3 substrate is under debate. Here, by measuring Knight shift and nuclear spin-lattice relaxation rate, we unambiguously reveal a pseudogap behavior below Tp ~ 60 K in two layered FeSe-based superconductors with quasi-two-dimension. In the pseudogap regime, a weak diamagnetic signal and a remarkable Nernst effect are also observed, which indicate that the observed pseudogap behavior is related to superconducting fluctuations. These works confirm that strong phase fluctuation is an important character in the two-dimensional iron-based superconductors as widely observed in high-Tc cuprate superconductors.
Topological insulators and semimetals as well as unconventional iron-based superconductors have attracted major recent attention in condensed matter physics. Previously, however, little overlap has been identified between these two vibrant fields, even though the principal combination of topological bands and superconductivity promises exotic unprecedented avenues of superconducting states and Majorana bound states (MBSs), the central building block for topological quantum computation. Along with progressing laser-based spin-resolved and angle-resolved photoemission spectroscopy (ARPES) towards high energy and momentum resolution, we have resolved topological insulator (TI) and topological Dirac semimetal (TDS) bands near the Fermi level ($E_{text{F}}$) in the iron-based superconductors Li(Fe,Co)As and Fe(Te,Se), respectively. The TI and TDS bands can be individually tuned to locate close to $E_{text{F}}$ by carrier doping, allowing to potentially access a plethora of different superconducting topological states in the same material. Our results reveal the generic coexistence of superconductivity and multiple topological states in iron-based superconductors, rendering these materials a promising platform for high-$T_{text{c}}$ topological superconductivity.
The importance of the spin-orbit coupling (SOC) effect in Fe-based superconductors (FeSCs) has recently been under hot debate. Considering the Hunds coupling-induced electronic correlation, the understanding of the role of SOC in FeSCs is not trivial and is still elusive. Here, through a comprehensive study of 77Se and 57Fe nuclear magnetic resonance, a nontrivial SOC effect is revealed in the nematic state of FeSe. First, the orbital-dependent spin susceptibility, determined by the anisotropy of the 57Fe Knight shift, indicates a predominant role from the 3dxy orbital, which suggests the coexistence of local and itinerant spin degrees of freedom (d.o.f.) in the FeSe. Then, we reconfirm that the orbital reconstruction below the nematic transition temperature (Tnem ~ 90 K) happens not only on the 3dxz and 3dyz orbitals but also on the 3dxy orbital, which is beyond a trivial ferro-orbital order picture. Moreover, our results also indicate the development of a coherent coupling between the local and itinerant spin d.o.f. below Tnem, which is ascribed to a Hunds coupling-induced electronic crossover on the 3dxy orbital. Finally, due to a nontrivial SOC effect, sizable in-plane anisotropy of the spin susceptibility emerges in the nematic state, suggesting a spin-orbital-intertwined nematicity rather than simply spin- or orbital-driven nematicity}. The present work not only reveals a nontrivial SOC effect in the nematic state but also sheds light on the mechanism of nematic transition in FeSe.
We present a comprehensive study of the evolution of the nematic electronic structure of FeSe using high resolution angle-resolved photoemission spectroscopy (ARPES), quantum oscillations in the normal state and elastoresistance measurements. Our high resolution ARPES allows us to track the Fermi surface deformation from four-fold to two-fold symmetry across the structural transition at ~87 K which is stabilized as a result of the dramatic splitting of bands associated with dxz and dyz character. The low temperature Fermi surface is that a compensated metal consisting of one hole and two electron bands and is fully determined by combining the knowledge from ARPES and quantum oscillations. A manifestation of the nematic state is the significant increase in the nematic susceptibility as approaching the structural transition that we detect from our elastoresistance measurements on FeSe. The dramatic changes in electronic structure cannot be explained by the small lattice effects and, in the absence of magnetic fluctuations above the structural transition, points clearly towards an electronically driven transition in FeSe stabilized by orbital-charge ordering.
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