Interfacial mode coupling as the origin of the enhancement of Tc in FeSe films on SrTiO3
J. J. Lee, F. T. Schmitt, R. G. Moore, S. Johnston, Y. -T. Cui, W. Li, M. Yi, Z. K. Liu, M. Hashimoto, Y. Zhang, D. H. Lu, T. P. Devereaux, D. -H. Lee, Z. -X. Shen
Single unit cell films of iron selenide (1UC FeSe) grown on SrTiO3 (STO) substrates have recently shown superconducting energy gaps opening at temperatures close to the boiling point of liquid nitrogen (77 K), a record for iron-based superconductors. Towards understanding why Cooper pairs form at such high temperatures, a primary question to address is the role, if any, of the STO substrate. Here, we report high resolution angle resolved photoemission spectroscopy (ARPES) results which reveal an unexpected and unique characteristic of the 1UC FeSe/STO system: shake-off bands suggesting the presence of bosonic modes, most likely oxygen optical phonons in STO, which couple to the FeSe electrons with only small momentum transfer. Such coupling has the unusual benefit of helping superconductivity in most channels, including those mediated by spin fluctuations. Our calculations suggest such coupling is responsible for raising the superconducting gap opening temperature in 1UC FeSe/STO. This discovery suggests a pathway to engineer high temperature superconductors.
Monolayer FeSe grown on SrTiO$_3$ provides a new playground for high-Tc superconductivity. A recent study shows the importance of stripy instability for superconductivity enhancement in FeSe/SrTiO3. However, it is still under debate whether such a stripe phase is ubiquitously bound to the interfacial superconductivity. Here, we report on molecular beam epitaxy growth and low-temperature scanning tunneling microscopy study of FeSe films on BaTiO$_3$(001). We find that the stripe phase is more prominent in FeSe/BaTiO$_3$. Long-range stripes exist in bilayer and triple-layer FeSe films at 4 K and…
We examine the impact of interfacial phonons on the superconducting state of FeSe/SrTiO$_3$ developing a material's specific multiband, full bandwidth, and anisotropic Eliashberg theory for this system. Our self-consistent calculations highlight the importance of the interfacial electron-phonon interaction, which is hidden behind the seemingly weak-coupling constant λ$_m$ = 0.4, in mediating the high T$_c$, and explain other puzzling experimental observations, such as the s-wave symmetry and replica bands. We discover that the formation of replica bands has a T$_c$ decreasing effect that is ne…
The strong fascination exerted by the binary compound of FeSe demands reliable engineering protocols and more effective approaches towards inducing superconductivity in FeSe thin films. Our study addresses the peculiarities in pulsed laser deposition which determine FeSe thin film growth and focuses on the film/substrate interface, the tendency for domain matching epitaxial growth but also the disadvantage of chemical heterogeneity. We propose that homogenization of the substrate surface improves the control of stoichiometry, texture, and nanostrain in a way that favors superconductivity even …
Thickness dependence of superconductivity and superconductor-insulator transition in ultrathin FeSe films on SrTiO3(001) substrate
SrTiO 3（001）（STO）衬底上单胞FeSe薄膜的界面增强高温超导性是近年来凝聚态物理和材料科学研究的热点。本文利用非原位输运测量方法研究了STO衬底上不同厚度的FeSe超薄膜的超导电性。我们发现，开始超导转变温度（Tc）随FeSe薄膜厚度的增加而降低，这是在传统的超导薄膜中通常观察到的行为相反。通过对5 μ C FeSe薄膜的系统后退火，我们观察到了绝缘体到超导体的转变，根据相应的霍尔测量，在低温下伴随着占主导地位的载流子从空穴到电子的符号变化。
We prepared single unit cell FeSe films on GaO$_{2-δ}$ terminated perovskite NdGaO$_{3}$(110) substrates and performed ex situ transport and scanning transmission electron microscopy measurements on the FeTe protected films. Our experimental measurements showed that the single unit cell FeSe films interfaced with GaO$_{2-δ}$ layer are electron doped via interface charge transfer. Most importantly, this type of heterostructure can host interface enhanced superconductivity with an onset temperature of about 28 K, which is much higher than the value of 8 K in bulk FeSe. Our work indicates that Fe…
We investigated chemical pressure effects in electron-doped (e-doped) FeSe by fabricating an electric-double-layer structure with single crystalline FeSe films on LaAlO$_3$ with Se substituted by isovalent Te and S. Our method enables transport measurements of e-doped FeSe. Electron doping by applying gate voltage of 5 V increases $T_{\mathrm c}$ of the FeSe$_{1-x}$Te$_x$ and FeSe$_{1-y}$S$_y$ films with $0 \leq x \leq 0.4$ and $0 \leq y \leq 0.25$, while the e-doped $x=0.5$ film showed lower $T_{\mathrm c}$ than that of the undoped one. Both positive and chemical pressure suppress $T_{\mathrm…
We report the successful growth of epitaxial thin films of FeSe$_{1-x}$S$_x$ with $x \leq 0.43$ via pulsed laser deposition. As S content increases, the nematic transition temperature, $T_{\mathrm s}$, decreases systematically and the superconducting transition temperature, $T_{\mathrm c}$, shows a gradual decrease even when $x$ exceeds the nematic end point (NEP), similar to bulk samples. A new kink anomaly was observed in the $ρ$-$T$ curves for films with large $x$, which is likely due to a magnetic transition. The obtained phase diagram of FeSe$_{1-x}$S$_x$ thin films is in contrast to that…
Superconducting FeSe films were electrochemically deposited on rolling-assisted biaxially textured substrate (RABiTS) tape. We observed zero resistivity in the as-electrodeposited FeSe film prepared on the RABiTS when the appropriate voltage was applied while it was dipped into the solution. When the RABiTS tape was dipped in the solution without applying voltage, a thin Se film was deposited on the substrate. The compositional ratio of the FeSe film got closer to the stoichiometric ratio with decreasing the dipping time before applying voltage.
The observation of substantially enhanced superconductivity of single-layer FeSe films on SrTiO3 has stimulated intensive research interest. At present, conclusive experimental data on the corresponding electron-boson interaction is still missing. Here we use inelastic electron scattering spectroscopy and angle resolved photoemission spectroscopy to show that the electrons in these systems are dressed by the strongly polarized lattice distortions of the SrTiO3, and the indispensable non-adiabatic nature of such a coupling leads to the formation of dynamic interfacial polarons. Furthermore, the…
Superconducting fluctuations in FeSe$_{0.5}$Te$_{0.5}$ thin films probed via microwave spectroscopy
我们研究了FeSe $_{0.5}$ Te $_{0.5}$在CaF $_2$上外延薄膜在超导转变附近的微波电导率谱。随着薄膜厚度的增加，我们观察到了超导涨落的临界行为，并出现了从二维到三维的空间交叉。由标度参数的温度依赖性，我们得出FeSe $_{0.5}$ Te $_{0.5}$超导转变的普适类是3D-XY模型。超导波动的起始温度的下限，Tonset，由我们的测量确定的是1.1 Tc，这表明FeSe $_{0.5}$ Te $_{0.5}$的超导波动至少与最佳和过掺杂的铜酸盐一样大。
Structural and electronic properties of ultrathin FeSe films grown on Bi$_2$Se$_3$(0001) studied by STM/STS
本文报道了在Bi $_2$ Se $_3$（0001）衬底上生长的单晶胞和双晶胞高FeSe薄膜的扫描隧道显微镜和光谱学（STM/STS）研究。在我们的薄膜中，我们发现FeSe的四方相和沿Se-Se键方向取向的哑铃形缺陷。此外，我们观察到条纹莫尔图案的周期性（$7.3\pm 0.1$）nm之间的失配FeSe晶格和Bi $_2$ Se $_3$晶格产生的。在6.5 K下，在一个和两个UC厚的FeSe岛表面上测量的隧道谱中，我们没有发现任何超导能隙的特征。光谱，而不是显示出一个不对称的行为和有限的状态密度在费米能级（$E_F$）类似于在正常状态的散装FeSe。
Our recent year's studies of the prototypal FeSe and molecule-intercalated (Li,Fe)OHFeSe superconductor systems are briefly reviewed here, with emphasis on experimental observations of the link between the superconductivity and normal-state electronic property in the single crystals and films. These samples were successfully synthesized by our recently developed soft-chemical hydrothermal methods, which are also briefly described. Particularly in the Mn-doped high-Tc (Li,Fe)OHFeSe film, a strong enhancement of the superconducting critical current density was achieved, which is promising for pr…
Universal Substrate Effect on the Superconductivity of FeSe Monolayer Films
为了阐明单层（1 ML）FeSe在SrTiO $_3$（STO）上的$T_c$增强的机制，我们在金红石TiO $_2$的矩形（100）面上生长了高应变的1 ML FeSe，并在63 K的$T_c$下观察到了复制带和超导电性的共存。从该系统与STO（001）上的1 ML FeSe之间的相似的$T_c$，我们得出结论，在这些系统中，应变和介电常数可能对增强的$T_c$不重要。一个系统的比较1 ML FeSe的TiO $_2$与其他系统中的FeSe家庭表明，虽然单独的电荷转移可以提高$T_c$，它只是与界面的电子-声子耦合，$T_c$可以增加到在STO上的1 ML FeSe的水平。
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 resu…
Determination of the pairing symmetry in monolayer FeSe films on SrTiO3 is a requisite for understanding the high superconducting transition temperature in this system, which has attracted intense theoretical and experimental studies but remains controversial. Here, by introducing several types of point defects in FeSe monolayer films, we conduct a systematic investigation on the impurity-induced electronic states by spatially resolved scanning tunneling spectroscopy. Ranging from surface adsorption, chemical substitution to intrinsic structural modification, these defects generate a variety o…
In this study, we fabricate 5-30-nm-thick films of FeSe/STO using pulsed laser deposition (PLD). The grown films exhibit superconductivity with an onset $T_{\mathrm{c}}$ that is much higher than that of bulk FeSe under ambient pressure. The observed $T_{\mathrm{c}}$ values are exceptionally high in terms of the strain vs. $T_{\mathrm{c}}$ relationship of the same material established so far. Furthermore, $T_{\mathrm{c}}$ increases as the film thickness decreases, except for films thinner than 10 nm. This thickness dependence of $T_{\mathrm{c}}$ is in good agreement with the results reported fo…
Interface charge transfer and electron-phonon coupling have been suggested to play a crucial role in the recently discovered high-temperature superconductivity of single unit-cell FeSe films on SrTiO3. However, their origin remains elusive. Here, using ultraviolet photoemission spectroscopy (UPS) and element-sensitive X-ray photoemission spectroscopy (XPS), we identify the strengthened Ti-O bond that contributes to the interface enhanced electron-phonon coupling and unveil the band bending at the FeSe/SrTiO3 interface that leads to the charge transfer from SrTiO3 to FeSe films. We also observe…
We performed systematic studies on the transport properties of FeSe thin films with controlled degrees of in-plane lattice strain, including both tensile and compressive strains. The superconducting transition temperature, $T_{\mathrm c}$, increases up to 12 K for films with compressive strain while the superconductivity disappears for films with large tensile strains. On the other hand, the structural (nematic) transition temperature, $T_{\mathrm s}$, slightly decreases as the in-plane strain is more compressive. This suggests that the structural transition can be extinguished by a smaller am…
Muon spin rotation/relaxation measurements were performed to investigate magnetic properties of FeSe$_{1-x}$S$_x$ thin films on LaAlO$_3$. A drastic decrease of the initial asymmetry was observed together with the peak structure in the temperature dependence of the relaxation rate of muon spins almost at the same temperature where kink anomalies were observed in the temperature dependent resistivity. With increasing S content, the anomaly temperature increased and the magnetic fluctuations at the lowest temperature were suppressed. These results show that the S substitution induces magnetism a…
The observation of replica bands by angle-resolved photoemission spectroscopy has ignited interest in the study of electron-phonon coupling at low carrier densities, particularly in monolayer FeSe/SrTiO$_3$, where the appearance of replica bands has motivated theoretical work suggesting that the interfacial coupling of electrons in the FeSe layer to optical phonons in the SrTiO$_3$ substrate might contribute to the enhanced superconducting pairing temperature. Alternatively, it has also been recently proposed that such replica bands might instead originate from extrinsic final state losses ass…
Suppression of phase separation and giant enhancement of superconducting transition temperature in FeSe$_{1-x}$Te$_{x}$ thin films
我们证明了成功的制造与$0 \le x \le 1$的FeSe $_{1-x}$ Te $_{x}$薄膜的CaF $_2$衬底上，包括区域的$0.1 \le x \le 0.4$，这是众所周知的“相分离区”，通过脉冲激光沉积，这是一种非平衡的方法。在由此产生的薄膜中，我们观察到一个巨大的增强的超导转变温度，$T_\mathrm{c}$，在该区域的$0.1 \le x \le 0.4$：最大值达到23 K，这是大约1.5倍大的散装样品的FeSe $_{1-x}$ Te $_{x}$报告的值。我们提出了一个完整的相图FeSe $_{1-x}$ Te $_{x}$薄膜。令人惊讶的是，在$0.1<x<0.2$处观察到$T_\mathrm{c}$的突然抑制，而对于$0.2 \le x < 1$，$T_\mathrm{c}$随着$x$的降低而增加。也就是说，在$x=0-0.1$和$x \ge 0.2$中实现的超导性之间存在明显的差异。为了获得具有高$T_\mathrm{c}$的FeSe $_{1-x}$ Te $_{x}$薄膜，发现Te含量$x$和面内晶格应变的控制是关键因素。
Systematic Comparison of Eight Substrates in the Growth of FeSe$_{0.5}$Te$_{0.5}$ Superconducting Thin Films
本文研究了在八种不同衬底上生长的FeSe $_{0.5}$ Te $_{0.5}$薄膜的晶体结构和超导性质。超导性与晶格失配无关，而是与面内取向程度和晶格参数比$c/a$相关。在MgO和LaAlOPDMATHABMO（$T_\mathrm{c}^\mathrm{zero}$为9.5 K）上的薄膜中观察到最好的超导性能。TEM观察表明，在衬底表面的非晶类层的存在或不存在起着关键作用，在确定的结构和超导性能的生长薄膜。
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 different 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 …
We performed terahertz magneto-optical spectroscopy of FeSe thin film to elucidate the charge carrier dynamics. The measured diagonal (longitudinal) and off-diagonal (Hall) conductivity spectra are well reproduced by two-carrier Drude model, from which the carrier densities, scattering times and effective masses of electron and hole carriers are determined in a wide range of temperature. The hole density decreases below the structural transition temperature while electron density increases, which is attributed to the band structure modification in the electronic nematic phase. The scattering t…
