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Register a new userElectric-field-induced superconductivity in electrochemically-etched ultrathin FeSe films on SrTiO3 and MgO
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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.
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In this study, we investigated the gate voltage dependence of $T_{mathrm c}$ in electrochemically etched FeSe films with an electric-double layer transistor structure. The $T_{mathrm c}^{mathrm {zero}}$ value of the etched FeSe films with a lower gate voltage ($V_{mathrm g}$ = 2.5 and 3.3 V) reaches 46 K, which is the highest value among almost all reported values from the resistivity measurements except for the data by Ge et al. This enhanced $T_{mathrm c}$ remains unchanged even after the discharge process, unlike the results for electrostatic doping without an etching process. Our results suggest that the origin of the increase in $T_{mathrm c}$ is not electrostatic doping but rather the electrochemical reaction at the surface of an etched 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.
Searching for superconducting materials with high transition temperature (TC) is one of the most exciting and challenging fields in physics and materials science. Although superconductivity has been discovered for more than 100 years, the copper oxides are so far the only materials with TC above 77 K, the liquid nitrogen boiling point. Here we report an interface engineering method for dramatically raising the TC of superconducting films. We find that one unit-cell (UC) thick films of FeSe grown on SrTiO3 (STO) substrates by molecular beam epitaxy (MBE) show signatures of superconducting transition above 50 K by transport measurement. A superconducting gap as large as 20 meV of the 1 UC films observed by scanning tunneling microcopy (STM) suggests that the superconductivity could occur above 77 K. The occurrence of superconductivity is further supported by the presence of superconducting vortices under magnetic field. Our work not only demonstrates a powerful way for finding new superconductors and for raising TC, but also provides a well-defined platform for systematic study of the mechanism of unconventional superconductivity by using different superconducting materials and substrates.
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.
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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