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. However, it has been under debate on how high its Tc can really reach due to the inconsistency of the results from different 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 strong superconductivity-induced Bogoliubov back-bending bands that extend to rather high binding energy ~ 100 meV by high-resolution angle-resolved photoemission measurements. They provide a new definitive benchmark of superconductivity pairing that is directly observed up to 83 K. Moreover, we find that the pairing state can be further divided into two temperature regions. These results indicate that either Tc as high as 83 K is achievable, or there is a pseudogap formation from superconductivity fluctuation in single-layer FeSe/STO films. How high the superconducting transition temperature can reach in single layer FeSe/SrTiO3 films has been under debate. Here, the authors use Bogoliubov back-bending bands as a benchmark and demonstrate that superconductivity pairing can be realized up to 83 K in this system.

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Spectroscopic evidence of superconductivity pairing at 83 K in single-layer FeSe/SrTiO 3 films.

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.

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Spectroscopic Evidence of Superconductivity Pairing at 83 K in Single-Layer FeSe/SrTiO3 Films.

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.

Incoherent Cooper pairing and pseudogap behavior in single-layer FeSe/SrTiO$_3$

Liquid-phase exfoliation can be developed for the large-scale production of two-dimensional materials for photonic applications. Although atomically thin 2D transition metal dichalcogenides (TMDs) ...

High-Yield Exfoliation of Monolayer 1T'-MoTe2 as Saturable Absorber for Ultrafast Photonics.

Enormous enhancement of superconducting pairing temperature (Tg) to 65 K in FeSe/SrTiO3 has made it a spotlight. Despite the effort of interfacial engineering, FeSe interfaced with TiOx remains the unique case in hosting high Tg, hindering a decisive understanding on the general mechanism and ways to further improving Tg. Here we constructed a new high-Tg interface, single-layer FeSe interfaced with FeOx-terminated LaFeO3. Large superconducting gap and diamagnetic response evidence that the superconducting pairing can emerge near 80 K, highest amongst all-known interfacial superconductors. Combining various techniques, we reveal interfacial charge transfer and strong interfacial electron-phonon coupling (EPC) in FeSe/LaFeO3, showing that the cooperative pairing mechanism works beyond FeSe-TiOx. Intriguingly, the stronger interfacial EPC than that in FeSe/SrTiO3 is likely induced by the stronger interfacial bonding in FeSe/LaFeO3, and can explain the higher Tg according to recent theoretical calculations, pointing out a workable route in designing new interfaces to achieve higher Tg. An enhanced superconducting pairing temperature (Tg) has only been observed in single-layer FeSe interfaced with TiOx system. Here, the authors construct a new interface composed of single-layer FeSe interfaced with LaFeO3 showing a highest Tg of 80 K among all-known interfacial superconductors.

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High temperature superconductivity at FeSe/LaFeO 3 interface

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 in the underdoped high- ${T}_{c}$ cuprate superconductors, the electron pairing occurs at higher temperature than the long-range phase coherence. Recently, whether electron pairing is also prior to long-range phase coherence in single-layer FeSe film on ${\mathrm{SrTiO}}_{3}$ substrate is under debate. Here, by measuring Knight shift and nuclear spin-lattice relaxation rate, we unambiguously reveal a pseudogap behavior below ${T}_{p}\ensuremath{\sim}60\text{ }\text{ }\mathrm{K}$ in two kinds of layered FeSe-based superconductors with quasi2D nature. In the pseudogap regime, a weak diamagnetic signal and a remarkable Nernst effect are also observed, which indicates that the observed pseudogap behavior is related to superconducting fluctuations. These works confirm that strong phase fluctuation is an important character in the 2D iron-based superconductors as widely observed in high-${T}_{c}$ cuprate superconductors.

M. Z. Shi

Papers

Preformed Cooper Pairs in Layered FeSe-Based Superconductors.