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Register a new userAntiferromagnetic order in epitaxial FeSe films on SrTiO3
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Single monolayer FeSe film grown on Nb-doped SrTiO$_3$(001) substrate shows the highest superconducting transition temperature (T$_C$ $sim$ 100 K) among the iron-based superconductors (iron-pnictide), while T$_C$ of bulk FeSe is only $sim$ 8 K. Antiferromagnetic spin fluctuations were believed to be crucial in iron-pnictides, which has inspired several proposals to understand the FeSe/SrTiO$_3$ system. Although bulk FeSe does not show the antiferromagnetic order, calculations suggest that the parent FeSe/SrTiO$_3$ films are AFM. Experimentally, due to lacking of direct probe, the magnetic state of FeSe/SrTiO$_3$ films remains mysterious. Here, we report the direct evidences of the antiferromagnetic order in the parent FeSe/SrTiO$_3$ films by the magnetic exchange bias effect measurements. The phase transition temperature is $geq$ 140 K for single monolayer film. The AFM order disappears after electron doping.
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Cryogenic scanning tunneling microscopy is employed to investigate the stoichiometry and defects of epitaxial FeSe thin films on SrTiO3(001) substrates under various post-growth annealing conditions. Low-temperature annealing with an excess supply of Se leads to formation of Fe vacancies and superstructures, accompanied by a superconductivity (metal)-to-insulator transition in FeSe films. By contrast, high-temperature annealing could eliminate the Fe vacancies and superstructures, and thus recover the high-temperature superconducting phase of monolayer FeSe films. We also observe multilayer FeSe during low-temperature annealing, which is revealed to link with Fe vacancy formation and adatom migration. Our results document very special roles of film stoichiometry and help unravel several controversies in the properties of monolayer FeSe films.
The accurate theoretical description of the underlying electronic structures is essential for understanding the superconducting mechanism of iron-based superconductors. Compared to bulk FeSe, the superconducting single-layer FeSe/SrTiO3 films exhibit a distinct electronic structure consisting of only electron Fermi pockets, due to the formation of a new band gap at the Brillouin zone (BZ) corners and an indirect band gap between the BZ center and corners. Although intensive studies have been carried out, the origin of such a distinct electronic structure and its connection to bulk FeSe remain unclear. Here we report a systematic study on the temperature evolution of the electronic structure in single-layer FeSe/SrTiO3 films by angle-resolved photoemission spectroscopy. A temperature-induced electronic phase transition was clearly observed at 200 K, above which the electronic structure of single-layer FeSe/SrTiO3 films restored to that of bulk FeSe, characterized by the closing of the new band gap and the vanishing of the indirect band gap. Moreover, the interfacial charge transfer effect induced band shift of ~ 60 meV was determined for the first time. These observations not only show the first direct evidence that the electronic structure of single-layer FeSe/SrTiO3 films originates from bulk FeSe through a combined effect of an electronic phase transition and an interfacial charge transfer, but also provide a quantitative basis for theoretical models in describing the electronic structure and understanding the superconducting mechanism in single-layer FeSe/SrTiO3 films.
Charge transfer and electron-phonon coupling (EPC) are proposed to be two important constituents associated with enhanced superconductivity in the single unit cell FeSe films on oxide surfaces. Using high-resolution electron energy loss spectroscopy combined with first-principles calculations, we have explored the lattice dynamics of ultrathin FeSe films grown on SrTiO3. We show that, despite the significant effect from the substrate on the electronic structure and superconductivity of the system, the FeSe phonons in the films are unaffected. The energy dispersion and linewidth associated with the Fe- and Se-derived vibrational modes are thickness- and temperature-independent. Theoretical calculations indicate the crucial role of antiferromagnetic correlation in FeSe to reproduce the experimental phonon dispersion. Importantly, the only detectable change due to the growth of FeSe films is the broadening of the Fuchs-Kliewer (F-K) phonons associated with the lattice vibrations of SrTiO$_3$(001) substrate. If EPC plays any role in the enhancement of film superconductivity, it must be the interfacial coupling between the electrons in FeSe film and the F-K phonons from substrate rather than the phonons of FeSe.
The intriguing role of nematicity in iron-based superconductors, defined as broken rotational symmetry below a characteristic temperature, is an intensely investigated contemporary subject. Nematicity is closely connected to the structural transition, however, it is highly doubtful that the lattice degree of freedom is responsible for its formation, given the accumulating evidence for the observed large anisotropy. Here we combine molecular beam epitaxy, angle-resolved photoemission spectroscopy and scanning tunneling microscopy together to study the nematicity in multilayer FeSe films on SrTiO3. Our results demonstrate direct connection between electronic anisotropy in momentum space and standing waves in real space at atomic scale. The lifting of orbital degeneracy of dxz/dyz bands gives rise to a pair of Dirac cone structures near the zone corner, which causes energy-independent unidirectional interference fringes, observed in real space as standing waves by scattering electrons off C2 domain walls and Se-defects. On the other hand, the formation of C2 nematic domain walls unexpectedly shows no correlation with lattice strain pattern, which is induced by the lattice mismatch between the film and substrate. Our results establish a clean case that the nematicity is driven by electronic rather than lattice degrees of freedom in FeSe films.
We report measurements of resistance and ac magnetic susceptibility on FeSe single crystals under high pressure up to 27.2 kbar. The structural phase transition is quickly suppressed with pressure, and the associated anomaly is not seen above $sim$18 kbar. The superconducting transition temperature evolves nonmonotonically with pressure, showing a minimum at $sim12$ kbar. We find another anomaly at 21.2 K at 11.6 kbar. This anomaly most likely corresponds to the antiferromagnetic phase transition found in $mu$SR measurements [M. Bendele textit{et al.}, Phys. Rev. Lett. textbf{104}, 087003 (2010)]. The antiferromagnetic and superconducting transition temperatures both increase with pressure up to $sim25$ kbar and then level off. The width of the superconducting transition anomalously broadens in the pressure range where the antiferromagnetism coexists.
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