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Register a new userRole of nematicity in controlling spin fluctuations and superconducting Tc in bulk FeSe
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Bulk FeSe superconducts inside a nematic phase, that sets in through an orthorhombic distortion of the high temperature tetragonal phase. Bulk non-alloy tetragonal superconducting FeSe does not exist as yet. This raises the question whether nematicity is fundamental to superconductivity. We employ an advanced ab-initio ability and show that bulk tetragonal FeSe can, in principle, superconduct at almost the same Tc as the orthorhombic phase had that been the ground state. Further, we perform rigorous benchmarking of our theoretical spin susceptibilities against experimentally observed data over all energies and relevant momentum direction. We show that susceptibilities computed in both the tetragonal and orthorhombic phases already have the correct momentum structure at all energies, but not the desired intensity. The enhanced nematicity that simulates the correct spin fluctuation intensity can only lead to a maximum 10-15% increment in the superconducting Tc . Our results suggest while nematicity may be intrinsic property of the bulk FeSe, is not the primary force driving the superconducting pairing.
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The interplay of orbital and spin degrees of freedom is the fundamental characteristic in numerous condensed matter phenomena, including high temperature superconductivity, quantum spin liquids, and topological semimetals. In iron-based superconductors (FeSCs), this causes superconductivity to emerge in the vicinity of two other instabilities: nematic and magnetic. Unveiling the mutual relationship among nematic order, spin fluctuations, and superconductivity has been a major challenge for research in FeSCs, but it is still controversial. Here, by carrying out 77Se nuclear magnetic resonance (NMR) measurements on FeSe single crystals, doped by cobalt and sulfur that serve as control parameters, we demonstrate that the superconducting transition temperature Tc increases in proportion to the strength of spin fluctuations, while it is independent of the nematic transition temperature Tnem. Our observation therefore directly implies that superconductivity in FeSe is essentially driven by spin fluctuations in the intermediate coupling regime, while nematic fluctuations have a marginal impact on Tc.
The mechanism behind the nematicity of FeSe is not known. Through elastoresitivity measurements it has been shown to be an electronic instability. However, so far measurements have extended only to small strains, where the response is linear. Here, we apply large elastic strains to FeSe, and perform two types of measurements. (1) Using applied strain to control twinning, the nematic resistive anisotropy at temperatures below the nematic transition temperature Ts is determined. (2) Resistive anisotropy is measured as nematicity is induced through applied strain at fixed temperature above Ts. In both cases, as nematicity strengthens the resistive anisotropy peaks about about 7%, then decreases. Below ~40 K, the nematic resistive anisotropy changes sign. We discuss possible implications of this behaviour for theories of nematicity. We report in addition: (1) Under experimentally accessible conditions with bulk crystals, stress, rather than strain, is the conjugate field to the nematicity of FeSe. (2) At low temperatures the twin boundary resistance is ~10% of the sample resistance, and must be properly subtracted to extract intrinsic resistivities. (3) Biaxial inplane compression increases both in-plane resistivity and the superconducting critical temperature Tc, consistent with a strong role of the yz orbital in the electronic correlations.
Electronic nematicity is an important order in most iron-based superconductors, and FeSe represents a unique example, in which nematicity disentangles from spin ordering. It is commonly perceived that this property arises from strong electronic correlation, which can not be properly captured by density functional theory (DFT). Here, we show that by properly considering the paramagnetic condition and carefully searching the energy landscape with symmetry-preconditioned wavefunctions, two nematic solutions stand out at either the DFT+$U$ or hybrid functional level, both of which are lower in energy than the symmetric solution. The ground-state band structure and Fermi surface can be well compared with the recent experimental results. Symmetry analysis assigns these two new solutions to the $B_{1g}$ and $E_u$ irreducible representations of the D$_{4h}$ point group. While the $B_{1g}$ Ising nematicity has been widely discussed in the context of vestigial stripe antiferromagnetic order, the two-component $E_u$ vector nematicity is beyond previous theoretical discussion. Distinct from the $B_{1g}$ order, the $E_u$ order features mixing of the Fe $d$-orbitals and inversion symmetry breaking, which lead to striking experimental consequences, e.g. missing of an electron pocket.
The discovery of enhanced superconductivity (SC) in FeSe films grown on SrTiO3 (FeSe/STO) has revitalized the field of Fe-based superconductors. In the ultrathin limit, the superconducting transition temperature Tc is increased by almost an order of magnitude, raising new questions on the pairing mechanism. As in other unconventional superconductors, antiferromagnetic spin fluctuations have been proposed as a candidate to mediate SC in this system. Thus, it is essential to study the evolution of the spin dynamics of FeSe in the ultrathin limit to elucidate their relationship with superconductivity. Here, we investigate and compare the spin excitations in bulk and monolayer FeSe grown on STO using high-resolution resonant inelastic x-ray scattering (RIXS) and quantum Monte Carlo (QMC) calculations. Despite the absence of long-range magnetic order, bulk FeSe displays dispersive magnetic excitations reminiscent of other Fe-pnictides. Conversely, the spin excitations in FeSe/STO are gapped, dispersionless, and significantly hardened relative to the bulk counterpart. By comparing our RIXS results with simulations of a bilayer Hubbard model, we connect the evolution of the spin excitations to the Fermiology of the two systems. The present study reveals a remarkable reconfiguration of spin excitations in FeSe/STO, which is essential to understand the role of spin fluctuations in the pairing mechanism.
The large anisotropy in the electronic properties across a structural transition in several correlated systems has been identified as the key manifestation of electronic nematic order, breaking rotational symmetry. In this context, FeSe is attracting tremendous interest, since electronic nematicity develops over a wide range of temperatures, allowing accurate experimental investigation. Here we combine angle-resolved photoemission spectroscopy and theoretical calculations based on a realistic multi-orbital model to unveil the microscopic mechanism responsible for the evolution of the electronic structure of FeSe across the nematic transition. We show that the self-energy corrections due to the exchange of spin fluctuations between hole and electron pockets are responsible for an orbital-dependent shrinking of the Fermi Surface that affects mainly the $xz/yz$ parts of the Fermi surface. This result is consistent with our experimental observation of the Fermi Surface in the high-temperature tetragonal phase, that includes the $xy$ electron sheet that was not clearly resolved before. In the low-temperature nematic phase, we experimentally confirm the appearance of a large ($sim$ 50meV) $xz/yz$ splittings. It can be well reproduced in our model by assuming a moderate splitting between spin fluctuations along the $x$ and $y$ crystallographic directions. Our mechanism shows how the full entanglement between orbital and spin degrees of freedom can make a spin-driven nematic transition equivalent to an effective orbital order.
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