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Register a new userLattice Dynamics of Ultrathin FeSe Films on SrTiO3
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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.
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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.
Among the recently discovered iron-based superconductors, ultrathin films of FeSe grown on SrTiO3 substrates have uniquely evolved into a high superconducting-transition-temperature (TC) material. The mechanisms for the high-TC superconductivity are ongoing debate mainly with the superconducting gap characterized with in-situ analysis for FeSe films grown by bottom-up molecular-beam epitaxy. Here, we demonstrate the alternative access to investigate the high-TC superconductivity in ultrathin FeSe with top-down electrochemical etching technique in three-terminal transistor configuration. In addition to the high-TC FeSe on SrTiO3, the electrochemically etched ultrathin FeSe transistor on MgO also exhibits superconductivity around 40 K, implying that the application of electric-field effectively contributes to the high-TC superconductivity in ultrathin FeSe regardless of substrate material. Moreover, the observable critical thickness for the high-TC superconductivity is expanded up to 10-unit-cells under applying electric-field and the insulator-superconductor transition is electrostatically controlled. The present demonstration implies that the electric-field effect on both conduction and valence bands plays a crucial role for inducing high-TC superconductivity in FeSe.
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.
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 parent 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.
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.
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