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Following the discovery of the potentially very high temperature superconductivity in monolayer FeSe we investigate the doping effect of Se vacancies in these materials. We find that Se vacancies pull a vacancy centered orbital below the Fermi energy that absorbs most of the doped electrons. Furthermore we find that the disorder induced broadening causes an effective hole doping. The surprising net result is that in terms of the band structure Se vacancies behave like hole dopants rather than electron dopants. Our results exclude Se vacancies as the origin of the large electron pockets measured by angle resolved photoemission spectroscopy.
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We investigate the currently debated issue concerning whether transition metal substitutions dope carriers in iron based superconductors. From first-principles calculations of the configuration-averaged spectral function of BaFe$_2$As$_2$ with disordered Co/Zn substitutions of Fe, important doping effects are found beyond merely changing the carrier density. While the chemical potential shifts suggest doping of a large amount of carriers, a reduction of the coherent carrier density is found due to the loss of spectral weight. Therefore, none of the change in the Fermi surface, density of states, or charge distribution can be solely used for counting doped coherent carriers, let alone presenting the full effects of the disordered substitutions. Our study highlights the necessity of including disorder effects in the studies of doped materials in general.
The discovery of high-temperature (Tc) superconductivity in monolayer FeSe on SrTiO3 raised a fundamental question whether high Tc is commonly realized in monolayer iron-based superconductors. Tetragonal FeS is a key material to resolve this issue because bulk FeS is a superconductor with Tc comparable to that of isostructural FeSe. However, difficulty in synthesizing tetragonal monolayer FeS due to its metastable nature has hindered further investigations. Here we report elucidation of band structure of monolayer FeS on SrTiO3, enabled by a unique combination of in-situ topotactic reaction and molecular-beam epitaxy. Our angle-resolved photoemission spectroscopy on FeS and FeSe revealed marked similarities in the electronic structure, such as heavy electron doping and interfacial electron-phonon coupling, both of which have been regarded as possible sources of high Tc in FeSe. However, surprisingly, high-Tc superconductivity is absent in monolayer FeS. This is linked to the weak superconducting pairing in electron-doped multilayer FeS in which the interfacial effects are absent. Our results strongly suggest that the cross-interface electron-phonon coupling enhances Tc only when it cooperates with the pairing interaction inherent to the superconducting layer. This finding provides a key insight to explore new heterointerface high-Tc superconductors.
Fermi surface topology and pairing symmetry are two pivotal characteristics of a superconductor. Superconductivity in one monolayer (1ML) FeSe thin film has attracted great interest recently due to its intriguing interfacial properties and possibly high superconducting transition temperature (Tc) over 77 K. Here, we report high-resolution measurements of the Fermi surface and superconducting gaps in 1ML FeSe using angle-resolved photoemission spectroscopy (ARPES). Two ellipse-like electron pockets are clearly resolved overlapping with each other at the Brillouin zone corner. The superconducting gap is nodeless but moderately anisotropic, which put strong constraints on determining the pairing symmetry. The gap maxima locate along the major axis of ellipse, which cannot be explained by a single d-wave, extended s-wave, or s$pm$ gap function. Four gap minima are observed at the intersection of electron pockets suggesting the existence of either a sign change or orbital-dependent pairing in 1ML FeSe.
Monolayer FeSe on SrTiO$_3$ superconducts with reported $T_mathrm{c}$ as high as 100 K, but the dramatic interfacial $T_mathrm{c}$ enhancement remains poorly understood. Oxygen vacancies in SrTiO$_3$ are known to enhance the interfacial electron doping, electron-phonon coupling, and superconducting gap, but the detailed mechanism is unclear. Here we apply scanning transmission electron microscopy (STEM) and electron energy loss spectroscopy (EELS) to FeSe/SrTiO$_3$ to image the diffusion of selenium into SrTiO$_3$ to an unexpected depth of several unit cells, consistent with the simultaneously observed depth profile of oxygen vacancies. Our density functional theory (DFT) calculations support the crucial role of oxygen vacancies in facilitating the thermally driven Se diffusion. In contrast to excess Se in the FeSe monolayer or FeSe/SrTiO$_3$ interface that is typically removed during post-growth annealing, the diffused Se remains in the top few unit cells of the SrTiO$_3$ bulk after the extended post-growth annealing that is necessary to achieve superconductivity. Thus the unexpected Se in SrTiO$_3$ may contribute to the interfacial electron doping and electron-phonon coupling that enhance $T_mathrm{c}$, suggesting another important role for oxygen vacancies as facilitators of Se diffusion.
Monolayer FeSe exhibits the highest transition temperature among the iron based superconductors and appears to be fully gapped, seemingly consistent with $s$-wave superconductivity. Here, we develop a theory for the superconductivity based on coupling to fluctuations of checkerboard magnetic order (which has the same translation symmetry as the lattice). The electronic states are described by a symmetry based ${bf k}cdot {bf p}$-like theory and naturally account for the states observed by angle resolved photoemission spectroscopy. We show that a prediction of this theory is that the resultant superconducting state is a fully gapped, nodeless, $d$-wave state. This state, which would usually have nodes, stays nodeless because, as seen experimentally, the relevant spin-orbit coupling term has an energy scale smaller than the superconducting gap.
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