典型的 BCS 超导体在实空间中微观上是均匀的，受具有高超流密度相位刚度的相干 Cooper 对支配，并以相干长度为特征。然而，在时间反演或平移不变性破缺的驱动下，超导序参量可能形成周期性振荡。迄今为止，这类调制序是各材料体系所特有的，其周期远大于晶格常数。这里，我们报道在单层 FeSe/SrTiO3 薄膜中直接观测到均匀的晶格尺度配对密度波（PDW），它由晶体对称性破缺的特殊界面结构所强制产生。我们的光谱成像扫描隧道显微镜揭示了单个晶胞内 Cooper 配对能隙的空间调制，且该调制取决于不等价原子位点。通过使用超导针尖测量 Josephson 电流，超流密度显著的周期性变化被可视化，表明相位刚度在实空间中发生振荡。这种晶格尺度超导调制与更大长度尺度的 PDW 序共存，表明配对强度和相位刚度均存在晶格尺度变化。我们的发现为关联电子体系中准粒子性质的相互交织密度波序提供了新见解，并推动未来对二维极限下非传统配对相互作用和相位刚度的研究。
英文摘要：
Typical BCS superconductors are microscopically homogeneous in real space governed by the coherent Cooper pairs with high phase stiffness of superfluid density, which is characterized by a coherence length. However, a periodic oscillation of superconducting order parameter may develop driven by breaking the time-reversal or translational invariance. To date, such modulated orders were specific to each material systems, with a periodicity much larger than the lattice constant. Here we report the direct observation of a uniform lattice-scale pair density wave (PDW) in single-layer FeSe/SrTiO3 films, enforced by peculiar interfacial structure of crystal symmetries breaking. Our spectroscopic imaging scanning tunneling microscopy unravels a spatial modulation of Cooper-pairing gap within a single unit-cell, depending on inequivalent atomic sites. Prominent periodic variation of superfluid density is visualized via Josephson current by a superconducting tip, indicating a real-space oscillation of phase stiffness. Such a lattice-scale superconducting modulation, which coexists with a larger length scale of PDW order, indicates the lattice-scale variation of both pairing strength and phase stiffness. Our findings provide new insights into the intertwined density-wave orders of quasiparticle character in correlated electronic systems, and provoke future studies on the unconventional pairing interaction and phase stiffness in the two-dimensional limit.
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 ou…
The discovery of high temperature superconductivity in FeSe films on SrTiO3 substrate has inspired great experimental and theoretical interests. First-principles density functional theory calculations, which have played an important role in the study of bulk iron-based superconductors, also participate in the investigation of interfacial superconductivity. In this article, we review the calculation results on the electronic and magnetic structures of FeSe epitaxial films, emphasizing on the interplay between different degrees of freedom, such as charge, spin, and lattice vibrations. Furthermor…
The single-layer FeSe/SrTiO3 (FeSe/STO) films have attracted much attention because of their simple crystal structure, distinct electronic structure and record high superconducting transition temperature (Tc). The origin of the dramatic Tc enhancement in single-layer FeSe/STO films and the dichotomy of superconductivity between single-layer and multiple-layer FeSe/STO films are still under debate. Here we report a comprehensive high resolution angle-resolved photoemission spectroscopy and scanning tunneling microscopy/spectroscopy measurements on the electronic structure evolution with doping …
The single-layer FeSe films grown on SrTiO3 (STO) substrates have attracted much attention because of its record high superconducting critical temperature (Tc). It is usually believed that the composition of the epitaxially grown single-layer FeSe/STO films is stoichiometric, i.e., the ratio of Fe and Se is 1:1. Here we report the identification of a large amount of excess Fe in the superconducting single-layer FeSe/STO films. By depositing Se onto the superconducting single-layer FeSe/STO films, we find by in situ scanning tunneling microscopy (STM) the formation of the second-layer FeSe isla…
The electronic structure of FeSe thin films grown on SrTiO3 substrate is studied by angle-resolved photoemission spectroscopy (ARPES). We reveal the existence of Dirac cone band dispersions in FeSe thin films thicker than 1 Unit Cell below the nematic transition temperature, whose apex are located -10 meV below Fermi energy. The evolution of Dirac cone electronic structure for FeSe thin films as function of temperature, thickness and cobalt doping is systematically studied. The Dirac cones are found to be coexisted with the nematicity in FeSe, disappear when nematicity is suppressed. Our resul…
The exact mechanism responsible for the tenfold enhancement of superconducting transition temperature (Tc) in a monolayer iron selenide (FeSe) on SrTiO3(STO) substrate over that of bulk FeSe, is an open issue. We present here a coordinated study of electrical transport and low temperature electron energy-loss spectroscopy (EELS) measurements on FeSe/STO films of various thicknesses. Our EELS mapping across the FeSe/STO interface shows direct evidence of band-bending caused by electrons transferred from STO to FeSe layer. The transferred electrons were found to accumulate only within the first …
The record of superconducting transition temperature(Tc) has long been 56K for the iron-based high temperature superconductors(Fe-HTS's). Recently, in single layer FeSe films grown on SrTiO3 substrate, signs for a new 65K Tc record are reported. Here with in-situ photoemission measurements, we substantiate the presence of the spin density wave(SDW) in FeSe films, a key ingredient of Fe-HTS that was missed in FeSe before, which weakens with increased thickness or reduced strain. We demonstrate that the superconductivity occurs when the electrons transferred from the oxygen-vacant substrate supp…
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 st…
Various Fe-vacancy orders have been reported in tetragonal Fe1-xSe single crystals and nanowires/nanosheets, which are similar to those found in alkali metal intercalated A1-xFe2-ySe2 superconductors. Here we report the in-situ angle-resolved photoemission spectroscopy study of Fe-vacancy disordered and ordered phases in FeSe multi-layer thin films grown by molecular beam epitaxy. Low temperature annealed FeSe films are identified to be Fe-vacancy disordered phase and electron doped. Further long-time low temperature anneal can change the Fe-vacancy disordered phase to ordered phase, which is …
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 Fe…
We report on the observation of high-temperature ($T_\textrm{c}$) superconductivity and magnetic vortices in single-unit-cell FeSe films on anatase TiO$_2$(001) substrate by using scanning tunneling microscopy. A systematic study and engineering of interfacial properties has clarified the essential roles of substrate in realizing the high-$T_\textrm{c}$ superconductivity, probably via interface-induced electron-phonon coupling enhancement and charge transfer. By visualizing and tuning the oxygen vacancies at the interface, we find their very limited effect on the superconductivity, which exclu…
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 …
We have studied the effect of tensile strain on the superconductivity in FeSe films. 50 nm, 100 nm, and 200 nm FeSe films were grown on MgO, SrTiO$_3$, and LaAlO$_3$ substrates by using a pulsed laser deposition technique. X-ray diffraction analysis showed that the tetragonal phase is dominant in all of our FeSe films. The 50 nm FeSe films on MgO and SrTiO$_3$ are under tensile strain, while the 50 nm FeSe film on LaAlO$_3$ and the other thick FeSe films are unstrained. Superconducting transitions have been observed in unstrained FeSe films with T$_{onset}$ $\approx$ 8 K, which is close to the…
Hexagonal FeSe thin films were grown on SrTiO3 substrates and the temperature and thickness dependence of their electronic structures were studied. The hexagonal FeSe is found to be metallic and electron doped, whose Fermi surface consists of six elliptical electron pockets. With decreased temperature, parts of the bands shift downward to high binding energy while some bands shift upwards to EF. The shifts of these bands begin around 300 K and saturate at low temperature, indicating a magnetic phase transition temperature of about 300 K. With increased film thickness, the Fermi surface topolog…
The effects of electron doping and phonon vibrations on the magnetic properties of monolayer and bilayer FeSe epitaxial films on SrTiO$_3$ have been studied, respectively, using first-principles calculations with van der Waals correction. For monolayer FeSe epitaxial film, the combined effect of electron doping and phonon vibrations readily leads to magnetic frustration between the collinear antiferromagnetic state and the checkerboard antiferromagnetic Néel state. For bilayer FeSe epitaxial film, such magnetic frustration is much more easily induced by electron doping in its bottom layer than…
We report the Meissner effect studies on an FeSe thin film grown on Nb doped SrTiO3 substrate by molecular beam epitaxy. Two-coil mutual inductance measurement clearly demonstrates the onset of diamagnetic screening at 65 K, which is consistent with the gap opening temperature determined by previous angle resolved photoemission spectroscopy results. The applied magnetic field causes a broadening of the superconducting transition near the onset temperature, which is the typical behavior for quasi-two-dimensional superconductors. Our results provide direct evidence that FeSe thin film grown on N…
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…
We report the synthesis of tetragonal $\mathrm{FeS}_x\mathrm{Se}_{1-x}$ films ($x \leq 0.78$) by pulsed-laser deposition. To fabricate the tetragonal alloy films with tetragonal FeSe and hexagonal FeS targets, we adopted an alternate deposition technique with FeSe buffer layer on MgO(001). The overall film composition is controlled by the thickness ratio of FeS / FeSe layers. The out-of-plane lattice parameter of the films follows Vegard's law, demonstrating homogeneous alloying by inter-diffusion. The sulfur solid solubility reaches $x = 0.78$ in the $\mathrm{FeS}_x\mathrm{Se}_{1-x}$ films, w…
The films of FeSe on substrates have attracted attention because of their unusually high-temperature (Tc) superconducting properties whose origins continue to be debated. To disentangle the competing effects of the substrate and interlayer and intralayer processes, we present here results of density functional theory (DFT)-based analysis of the electronic structure of unsupported FeSe films consisting of 1 to 5 layers (1L-5L). Furthermore, by solving the Bardeen-Schrieffer-Cooper (BCS) equation with spin-wave exchange attraction derived from the Hubbard model, we find the superconducting criti…
Interface enhanced superconductivity at two dimensional limit has become one of most intriguing research directions in condensed matter physics. Here, we report the superconducting properties of ultra-thin FeSe films with the thickness of one unit cell (1-UC) grown on conductive and insulating SrTiO3 (STO) substrates. For the 1-UC FeSe on conductive STO substrate (Nb-STO), the magnetization versus temperature (M-T) measurement shows a diamagnetic signal at 85 K, suggesting the possibility of superconductivity appears at this high temperature. For the FeSe films on insulating STO substrate, sys…
Biaxially textured FeSe1-xTex films have been realized on Fe-buffered MgO substrates by pulsed laser deposition. Similar to the Fe/BaFe2As2 bilayers, the crystalline quality of FeSe1-xTex films exhibit a sharp out-of-plane and in-plane texture less than 0.9°. The Fe/FeSe1-xTex bilayers showed high superconducting transition temperatures of over 17 K. The angular-dependent critical current densities exhibit peaks positioned at H // ab similar to other pnictide thin films. The volume pinning force of FeSe1-xTex in this direction is very strong compared with that of Co-doped BaFe2As2, due to a go…
This is a "perspective" inspired by the forthcoming article, "What makes the $T_c$ of monolayer FeSe on SrTiO so high: a sign-problem free quantum Monte Carlo study," by Z-X. Li, F. Wang, H. Yao, and D-H. Lee, arXiv:1512.06179.
This paper reports that ~10-nm-thick FeSe thin films exhibit insulator-like behavior in terms of the temperature dependence of their electrical resistivity even though bulk FeSe has a metallic electronic structure that has been confirmed by photoemission spectroscopy and first-principles calculations. This apparent contradiction is explained by potential barriers formed in the conduction band. Very thin FeSe epitaxial films with various [Fe]/[Se] were fabricated by molecular beam epitaxy and classified into two groups with respect to lattice strain and electrical properties. Lattice parameter …
Ultrathin FeSe films grown on SrTiO$_{3}$ substrates are a recent milestone in atomic material engineering due to their important role in understanding unconventional superconductivity in Fe-based materials. Using femtosecond time- and angle-resolved photoelectron spectroscopy, we study phonon frequencies in ultrathin FeSe/SrTiO$_{3}$ films grown by molecular beam epitaxy. After optical excitation, we observe periodic modulations of the photoelectron spectrum as a function of pump-probe delay for 1 unit cell, 3 unit cell, and 60 unit cell thick FeSe films. The frequencies of the coherent inten…
The mechanism of high temperature superconductivity in the iron-based superconductors remains an outstanding issue in condensed matter physics. The electronic structure, in particular the Fermi surface topology, is considered to play an essential role in dictating the superconductivity. Recent revelation of distinct electronic structure and possible high temperature superconductivity with a transition temperature Tc above 65 K in the single-layer FeSe films grown on the SrTiO3 substrate provides key information on the roles of Fermi surface topology and interface in inducing or enhancing super…
The pressure effect on the resistivity and superconducting Tc of prestrained thin films of the iron chalcogenide superconductor FeSe0.5Te0.5 is studied. Films with different anion heights above the Fe layer showing different values of ambient pressure Tc's are compressed up to a pressure of 1.7 GPa. All films exhibit a significant increase of Tc with pressure. The results cannot solely be explained by a pressure-induced decrease of the anion height but other parameters have to be considered to explain the data for all films.
We report comprehensive angle-resolved photoemission investigations on the electronic structure of single crystal multiple-layer FeSe films grown on CaF2 substrate by pulsed laser deposition (PLD) method. Measurements on FeSe/CaF2 samples with different superconducting transition temperatures Tc of 4 K, 9 K and 14 K reveal electronic difference in their Fermi surface and band structure. Indication of the nematic phase transition is observed from temperature-dependent measurements of these samples; the nematic transition temperature is 140-160 K, much higher than 90 K for the bulk FeSe. Potassi…
The accurate theoretical description of the underlying electronic structures is essential for understanding the superconducting mechanism of iron-based superconductors. Compared to bulk FeSe, the superconducting single-layer FeSe/SrTiO3 films exhibit a distinct electronic structure consisting of only electron Fermi pockets, due to the formation of a new band gap at the Brillouin zone (BZ) corners and an indirect band gap between the BZ center and corners. Although intensive studies have been carried out, the origin of such a distinct electronic structure and its connection to bulk FeSe remain …
Superconductivity is significantly enhanced in monolayer FeSe grown on SrTiO3, but not for multilayer films, in which large strength of nematicity develops. However, the link between the high-transition temperature superconductivity in monolayer and the correlation related nematicity in multilayer FeSe films is not well understood. Here, we use low-temperature scanning tunneling microscopy to study few-layer FeSe thin films grown by molecular beam epitaxy. We observe an incommensurate long-range smectic phase, which solely appears in bilayer FeSe films. The smectic order still locally exists a…
The discovery of high-temperature superconductivity in FeSe/STO has trigged great research interest to reveal a range of exotic physical phenomena in this novel material. Here we present a temperature dependent magnetotransport measurement for ultrathin FeSe/STO films with different thickness and protection layers. Remarkably, a surprising linear magnetoresistance (LMR) is observed around the superconducting transition temperatures but absent otherwise. The experimental LMR can be reproduced by magnetotransport calculations based on a model of magnetic field dependent disorder induced by spin …
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 …
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. Intrigu…
In a material prone to a nematic instability, anisotropic strain in principle provides a preferred symmetry-breaking direction for the electronic nematic state to follow. This is consistent with experimental observations, where electronic nematicity and structural anisotropy typically appear hand-in-hand. In this work, we discover that electronic nematicity can be locally decoupled from the underlying structural anisotropy in strain-engineered iron-selenide (FeSe) thin films. We use heteroepitaxial molecular beam epitaxy to grow FeSe with a nanoscale network of modulations that give rise to sp…
By the first-principles electronic structure calculations, we have studied electronic structures of FeSe monolayer and bilayer thin films on SrTiO$_3$ (001) with SrO-termination or TiO$_2$ termination. We find that both FeSe monolayer and bilayer on either termination behave like a slightly doped semiconductor and a collinear antiferromagnetic order on Fe ions. There is no substantial charge transfer between the FeSe layers and the substrate. FeSe is adhered to the SrTiO$_3$ surface by a dipole-dipole interaction. The Fermi surface is mainly the contribution of Fe-3d orbitals. A valence band c…
We report the superconductivity evolution of one unit cell (1-UC) and 2-UC FeSe films on SrTiO3(001) substrates with potassium (K) adsorption. By in situ scanning tunneling spectroscopy measurement, we find that the superconductivity in 1-UC FeSe films is continuously suppressed with increasing K coverage, whereas non-superconducting 2-UC FeSe films become superconducting with a gap of ~17 meV or ~11 meV depending on whether the underlying 1-UC films are superconducting or not. This work explicitly reveals that the interface electron-phonon coupling is strongly related to the charge transfer a…
The transition from insulator to superconductor was achieved in the non-superconducting FeSe ultrathin film via simple Mg coating technique in present work. It was found that in non-superconducting FeSe ultrathin film without Mg coating, insulating \b{eta}-Fe1-xSe phase with iron-vacancy disorders is the main phase and more likely to be the parent phase of FeSe superconducting system. Proper Mg coating on the surface of FeSe films can lead to Mg entering FeSe crystal lattice to fill up these Fe vacancies rather than replace Fe. Simultaneously, additional electron doping is introduced and the e…
FeSe$_{1-x}$Te$_{x}$ thin films with PbO-type structure are successfully grown on MgO(100) and LaSrAlO$_{4}$(001) substrates from FeSe$_{1-x}$Te$_{x+d}$ polycrystalline targets by pulsed-laser deposition. The film deposited on the MgO substrate (film thickness $\sim$ 63 nm) shows superconductivity at 6.7 K (onset) and 5.5 K (zero resistivity). On the other hand, the film deposited on the LaSrAlO$_{4}$ substrate (film thickness $\sim$ 52 nm) exhibits only the onset of superconducting transition at 2.6 K, but does not show zero resistivity. This indicates the strong influence of epitaxial strain…
Interface-enhanced high-temperature superconductivity in one unit-cell (UC) FeSe film on SrTiO3(001) (STO) substrate has recently attracted much attention in condensed matter physics and material science. Here, by ex situ transport measurements, we report on the superconductivity in FeSe ultra-thin films with different thickness on STO substrate. We find that the onset superconducting transition temperature (Tc) decreases with increasing film thickness of FeSe, which is opposite to the behavior usually observed in traditional superconductor films. By systematic post-annealing of 5 UC FeSe film…
The origin of the high-temperature superconducting state observed in FeSe thin films, whose phase diagram displays no sign of magnetic order, remains a hotly debated topic. Here we investigate whether fluctuations arising due to the proximity to a nematic phase, which is observed in the phase diagram of this material, can promote superconductivity. We find that nematic fluctuations alone promote a highly degenerate pairing state, in which both $s$-wave and $d$-wave symmetries are equally favored, and $T_{c}$ is consequently suppressed. However, the presence of a sizable spin-orbit coupling or …
The significantly enhanced superconducting transition temperature ($T_c$) of an FeSe monolayer on SrTiO$_3$(001) substrate has attracted extensive attention in recent years. Here, based on first-principles electronic structure calculations, we propose another candidate substrate LaO(001) for the epitaxial growth of FeSe monolayer to realize superconductivity. Our calculations show that for the optimal adsorption structure of FeSe monolayer on LaO(001), the stripe antiferromagnetic state and the dimer antiferromagnetic state are almost energetically degenerate, indicating the existence of stron…
The superconducting FeSe films were successfully fabricated using the electrochemical synthesis. The composition ratio of Fe and Se can be controlled by the electric potential and pH value. We found that the FeSe films deposited at the electric potential -1.75 V and pH 2.3 show the superconducting transition at 3.5 K. The establishment of this electrochemical synthesis technique will provide many advantages for application.
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 have fabricated high-quality FeSe1-x superconducting films with a bulk Tc of 11-12 K on different substrates, Al2O3(0001), SrTiO3(100), MgO(100), and LaAlO3(100), by using a pulsed laser deposition technique. All the films were grown at a high substrate temperature of 610 oC, and were preferentially oriented along the (101) direction, the latter being to be a key to fabricating of FeSe1-x superconducting thin films with high Tc. According to the energy dispersive spectroscopy data, the Fe:Se composition ratio was 1:0.90+-0.02. The FeSe1-x film grown on a SrTiO3 substrate showed the best qua…
Bridging atomic and mesoscopic length scales with Replica Scanning Tunneling Microscopy: Visualizing the atomic lattice of UTe$_2$ and the atomic scale superconducting gap modulations of FeSe close to micron length scales
Universidad Autónoma de Madrid（马德里自治大学）；Universidad del Rosario（罗萨里奥大学）
We report on the emergence of two disconnected superconducting domes in alkali-metal potassium (K)-doped FeSe ultra-thin films grown on graphitized SiC(0001). The superconductivity exhibits hypersensitivity to K dosage in the lower-Tc dome, whereas in the heavily electron-doped higher-Tc dome it becomes spatially homogeneous and robust against disorder, supportive of a conventional Cooper-pairing mechanism. Furthermore, the heavily K-doped multilayer FeSe films all reveal a large superconducting gap of ~ 14 meV, irrespective of film thickness, verifying the higher-Tc superconductivity only in …
Superconductivity was recently found in the simple tetragonal FeSe structure. Recent studies suggest that FeSe is unconventional, with the symmetry of the superconducting pairing state still under debate. To tackle these problems, clean single crystals and thin films are required. Here we report the fabrication of superconducting beta-phase FeSe1-x thin films on different substrates using a pulsed laser deposition (PLD) technique. Quite interestingly, the crystal orientation, and thus, superconductivity in these thin films is sensitive to the growth temperature. At 320C, films grow preferably …
The presumably unconventional superconductor Beta-FeSe was deposited by radio frequency sputtering and molecular beam epitaxy (MBE) from two elementary sources. Superconducting thin films were grown in (001)-orientation on MgO(100) and YAlO3(010) substrates. The morphology of the samples was studied and directly related to the superconducting properties of the Beta-FeSe thin films. The MBE grown thin films show microcracks down to the substrate and a roughness of about 100~nm. In contrast, sputter deposited superconducting thin films show a smooth surface with almost no precipitates. In both c…
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…
Superconductivity in the cuprate superconductors and the Fe-based superconductors is realized by doping the parent compound with charge carriers, or by application of high pressure, to suppress the antiferromagnetic state. Such a rich phase diagram is important in understanding superconductivity mechanism and other physics in the Cu- and Fe-based high temperature superconductors. In this paper, we report a phase diagram in the single-layer FeSe films grown on SrTiO3 substrate by an annealing procedure to tune the charge carrier concentration over a wide range. A dramatic change of the band str…
Competing Constraints on Superconductivity in Thick FeSe films
Materials Genome Institute, Shanghai University（上海大学材料基因组研究院）；College of Ocean Science and Engineering, Shanghai Maritime University（上海海事大学海洋科学与工程学院）；Department of Physics and Shanghai Key Laboratory for High Temperature Superconductors, Shanghai University（上海大学物理系及高温超导上海市重点实验室）；Institute for Quantum Science and Technology, Shanghai University（上海大学量子科学与技术研究院）
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.
Epitaxial Fe(Se,Te) thin films were prepared by pulsed laser deposition on (La0.18Sr0.82)(Al0.59Ta0.41)O3 (LSAT), CaF2-buffered LSAT and bare CaF2 substrates, which exhibit an almost identical in-plane lattice parameter. The composition of all Fe(Se,Te) films were determined to be FeSe0.7Te0.3 by energy dispersive X-ray spectroscopy, irrespective of the substrate. Albeit the lattice parameters of all templates have comparable values, the in-plane lattice parameter of the FeSe0.7Te0.3 films varies significantly. We found that the superconducting transition temperature (Tc) of FeSe0.7Te0.3 thin …
In order to investigate the effects of in-plane strain on the superconductivity of FeSe, epitaxial thin films of FeSe were fabricated on CaF$_2$ substrates. The films are compressed along the a-axis and their superconducting transition temperatures $T_{\mathrm c}^{\mathrm {zero}}$ reach 11.4 K, which is approximately 1.5 times higher than that of bulk crystals. The $T_{\mathrm c}$ values are weakly dependent on the ratio of the lattice constants, $c$ / $a$, compared to that of Fe(Se,Te). Our results indicate that even a binary system FeSe has room for improvement, and will open a new route for…
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 add…
We investigated the microwave conductivity spectrum of FeSe$_{0.5}$Te$_{0.5}$ epitaxial films on CaF$_2$ in the vicinity of the superconducting transition. We observed the critical behavior of the superconducting fluctuations in these films with a dimensional crossover from two-dimensional to three-dimensional as the film thickness increased. From the temperature dependence of the scaling parameters we conclude that the universality class of the superconducting transition in FeSe$_{0.5}$Te$_{0.5}$ is that of the 3D-XY model. The lower limit of the onset temperature of the superconducting fluct…
