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تسجيل مستخدم جديدStoichiometry and defect superstructures in epitaxial FeSe films on SrTiO3
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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.
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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. Antif
erromagnetic 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.
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.
Synthesis of monolayer FeSe on SrTiO3, with greatly enhanced superconductivity compared to bulk FeSe, remains difficult. Lengthy annealing within a certain temperature window is always required to achieve superconducting samples as reported by differ
ent groups around the world, but the mechanism of annealing in inducing superconductivity has not been elucidated. We grow FeSe films on SrTiO3 by molecular beam epitaxy and adjust the stoichiometry by depositing additional small amounts of Fe atoms. The monolayer films become superconducting after the Fe deposition without any annealing, and show similar superconducting transition temperatures as those of the annealed films in transport measurements. We also demonstrate on the 5-unit-cell films that the FeSe multilayer can be reversibly tuned between the non-superconducting $sqrt{5} times sqrt{5}$ phase with Fe-vacancies and superconducting $1 times 1$ phase. Our results reveal that the traditional anneal process in essence removes Fe vacancies and the additional Fe deposition serves as a more efficient way to achieve superconductivity. This work highlights the significance of stoichiometry in the superconductivity of FeSe thin films and provides an easy path for superconducting samples.
In high temperature cuprate superconductors, it is now generally agreed that the parent compound is a Mott insulator and superconductivity is realized by doping the antiferromagnetic Mott insulator. In the iron-based superconductors, however, the par
ent compound is mostly antiferromagnetic metal, raising a debate on whether an appropriate starting point should go with an itinerant picture or a localized picture. It has been proposed theoretically that the parent compound of the iron-based superconductors may be on the verge of a Mott insulator, but so far no clear experimental evidence of doping-induced Mott transition has been available. Here we report an electronic evidence of an insulator-superconductor transition observed in the single-layer FeSe films grown on the SrTiO3 substrate. By taking angle-resolved photoemission measurements on the electronic structure and energy gap, we have identified a clear evolution of an insulator to a superconductor with the increasing doping. This observation represents the first example of an insulator-superconductor transition via doping observed in the iron-based superconductors. It indicates that the parent compound of the iron-based superconductors is in proximity of a Mott insulator and strong electron correlation should be considered in describing the iron-based superconductors.
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