No Arabic abstract
In many unconventional superconductors, the presence of a pseudogap - a suppression in the electronic density of states extending above the critical temperature - has been a long-standing mystery. Here, we employ combined textit{in situ} electrical transport and angle-resolved photoemission spectroscopy (ARPES) measurements to reveal an unprecedentedly large pseudogap regime in single-layer FeSe/SrTiO$_3$, an interfacial superconductor where incoherent Cooper pairs are initially formed above $T_{Delta}$ $approx$ 60 K, but where a zero resistance state is only achieved below $T_{0}$ $<$ 30 K. We show that this behavior is accompanied by distinct transport signatures of two-dimensional phase fluctuating superconductivity, suggesting a mixed vortex state hosting incoherent Cooper pairs which persist well above the maximum clean limit $T_{c}$ of $approx$ 40 K. Our work establishes the critical role of reduced dimensionality in driving the complex interplay between Cooper pairing and phase coherence in two-dimensional high-$T_c$ superconductors, providing a paradigm for understanding and engineering higher-$T_{c}$ interfacial superconductors.
Single-layer FeSe films grown on the SrTiO3 substrate (FeSe/STO) have attracted much attention because of their possible record-high superconducting critical temperature Tc and distinct electronic structures in iron-based superconductors. However, it has been under debate on how high its Tc can really reach due to the inconsistency of the results obtained from the transport, magnetic and spectroscopic measurements. Here we report spectroscopic evidence of superconductivity pairing at 83 K in single-layer FeSe/STO films. By preparing high-quality single-layer FeSe/STO films, we observe for the first time strong superconductivity-induced Bogoliubov back-bending bands that extend to rather high binding energy ~100 meV by high-resolution angle-resolved photoemission measurements. The Bogoliubov back-bending band provides a new definitive benchmark of superconductivity pairing that is directly observed up to 83 K in the single-layer FeSe/STO films. Moreover, we find that the superconductivity pairing state can be further divided into two temperature regions of 64-83 K and below 64 K. We propose the 64-83 K region may be attributed to superconductivity fluctuation while the region below 64 K corresponds to the realization of long-range superconducting phase coherence. These results indicate that either Tc as high as 83 K is achievable in iron-based superconductors, or there is a pseudogap formation from superconductivity fluctuation in single-layer FeSe/STO films.
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.
Single-layer FeSe films with extremely expanded in-plane lattice constant of 3.99A are fabricated by epitaxially growing FeSe/Nb:SrTiO3/KTaO3 heterostructures, and studied by in situ angle-resolved photoemission spectroscopy. Two elliptical electron pockets at the Brillion zone corner are resolved with negligible hybridization between them, indicating the symmetry of the low energy electronic structure remains intact as a free-standing single-layer FeSe, although it is on a substrate. The superconducting gap closes at a record high temperature of 70K for the iron based superconductors. Intriguingly, the superconducting gap distribution is anisotropic but nodeless around the electron pockets, with minima at the crossings of the two pockets. Our results put strong constraints on the current theories, and support the coexistence of both even and odd parity spin-singlet pairing channels as classified by the lattice symmetry.
The latest discovery of possible high temperature superconductivity in the single-layer FeSe film grown on a SrTiO3 substrate, together with the observation of its unique electronic structure and nodeless superconducting gap, has generated much attention. Initial work also found that, while the single-layer FeSe/SrTiO3 film exhibits a clear signature of superconductivity, the double-layer FeSe/SrTiO3 film shows an insulating behavior. Such a dramatic difference between the single-layer and double-layer FeSe/SrTiO3 films is surprising and the underlying origin remains unclear. Here we report our comparative study between the single-layer and double-layer FeSe/SrTiO3 films by performing a systematic angle-resolved photoemission study on the samples annealed in vacuum. We find that, like the single-layer FeSe/SrTiO3 film, the as-prepared double-layer FeSe/SrTiO3 film is insulating and possibly magnetic, thus establishing a universal existence of the magnetic phase in the FeSe/SrTiO3 films. In particular, the double-layer FeSe/SrTiO3 film shows a quite different doping behavior from the single-layer film in that it is hard to get doped and remains in the insulating state under an extensive annealing condition. The difference originates from the much reduced doping efficiency in the bottom FeSe layer of the double-layer FeSe/SrTiO3 film from the FeSe-SrTiO3 interface. These observations provide key insights in understanding the origin of superconductivity and the doping mechanism in the FeSe/SrTiO3 films. The property disparity between the single-layer and double-layer FeSe/SrTiO3 films may facilitate to fabricate electronic devices by making superconducting and insulating components on the same substrate under the same condition.
Superconductivity arises from two distinct quantum phenomena: electron pairing and long-range phase coherence. In conventional superconductors, the two quantum phenomena generally take place simultaneously, while the electron pairing occurs at higher temperature than the long-range phase coherence in the underdoped high-Tc cuprate superconductors. Recently, whether electron pairing is also prior to long-range phase coherence in single-layer FeSe film on SrTiO3 substrate is under debate. Here, by measuring Knight shift and nuclear spin-lattice relaxation rate, we unambiguously reveal a pseudogap behavior below Tp ~ 60 K in two layered FeSe-based superconductors with quasi-two-dimension. In the pseudogap regime, a weak diamagnetic signal and a remarkable Nernst effect are also observed, which indicate that the observed pseudogap behavior is related to superconducting fluctuations. These works confirm that strong phase fluctuation is an important character in the two-dimensional iron-based superconductors as widely observed in high-Tc cuprate superconductors.