Dung-Hai Lee
This note reviews some of the recent progresses in the study of high temperature superconductivity in the interface between a single unit cell FeSe and SrTiO$_3$. It offers the author's personal view of why $T_c$ is high and how to further increase it.
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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…
Temperature evolution of the Fermi surface of the FeSe monolayer on SrTiO$_3$
本研究通过分析FeSe/SrTiO$_3$动态电荷响应的温度演化，发现FeSe单层费米面在宽温区内基本不变，揭示其电子结构特殊性并为理解氧化物表面铁硫族单层超导机制提供依据。
Anisotropy of upper critical fields and interface superconductivity in FeSe/SrTiO3 grown by PLD
本研究通过脉冲激光沉积制备不同厚度FeSe/SrTiO₃薄膜，发现其具有大的上临界场各向异性，且垂直相干长度小于FeSe c轴长度、与膜厚无关，证实超导性局限于界面，为界面超导研究提供了实验依据。
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…
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…
In a recent experiment the superconducting gap of a single unit cell thick FeSe film on SrTiO$_3$ substrate is observed by scanning tunneling spectroscopy and angle-resolved photoemission spectroscopy. The value of the superconducting gap is much larger than that of the bulk FeSe under ambient pressure. In this paper we study the effects of screening due to the ferroelectric phonons on Cooper pairing. We conclude it can significantly enhance the energy scale of Cooper pairing and even change the pairing symmetry. Our results also raise some concerns on whether phonons can be completely ignored…
Monolayer FeSe films grown on SrTiO3 (STO) substrate show superconducting gap-opening temperatures (Tc) which are almost an order of magnitude higher than those of the bulk FeSe and are highest among all known Fe-based superconductors. Angle-resolved photoemission spectroscopy (ARPES) observed "replica bands" suggesting the importance of the interaction between FeSe electrons and STO phonons. These facts rejuvenated the quest for Tc enhancement mechanisms in iron-based, especially iron-chalcogenide, superconductors. Here, we perform the first numerically-exact sign-problem-free quantum Monte C…
We study the effect of combining spin fluctuations and forward scattering electron-phonon ({\eph}) coupling on the superconductivity in the FeSe/SrTiO$_3$ system modeled by a phenomenological two-band Hubbard model with long-range {\eph} interactions. We treat the electron and phonon degrees of freedom on an equal footing using a \emph{fully} self-consistent FLEX plus Migdal-Eliashberg calculation, which includes a self-consistent determination of the spin fluctuation spectrum. Based on FeSe monolayers, we focus on the case where one of the bands lies below the Fermi level (i.e. incipient), an…
Observation of replica bands in the ARPES spectra of the single-layer FeSe on strontium titanate substrate revealed a phonon component among mechanisms behind high Tc superconductivity there. We study the interaction of the in-layer FeSe electrons with the electric potential of the longitudinal (LO) modes at surface of bulk SrTiO3. A two-dimensional system of charges at the FeSe/SrTiO3 interface includes both the itinerant and immobile electrons. The latter significantly change the interface characteristics, increasing screening at the substrate surface and reducing thereby the strength of the…
We use scanning tunneling microscopy (STM) and quasiparticle interference (QPI) imaging to investigate the low-energy orbital texture of single-layer FeSe/SrTiO$_3$. We develop a $T$-matrix model of multi-orbital QPI to disentangle scattering intensities from Fe $3d_{xz}$ and $3d_{yz}$ bands, enabling the use of STM as a nanoscale detection tool of nematicity. By sampling multiple spatial regions of a single-layer FeSe/SrTiO$_3$ film, we quantitatively exclude static $xz/yz$ orbital ordering with domain size larger than $δr^2$ = 20 nm $\times$ 20 nm, $xz/yz$ Fermi wave vector difference larger…
Epitaxial engineering of solid-state heterointerfaces is a leading avenue to realizing enhanced or novel electronic states of matter. As a recent example, bulk FeSe is an unconventional superconductor with a modest transition temperature ($T_c$) of 9 K. When a single atomic layer of FeSe is grown on SrTiO$_3$, however, its $T_c$ can skyrocket by an order of magnitude to 65 K or 109 K. Since this discovery in 2012, efforts to reproduce, understand, and extend these findings continue to draw both excitement and scrutiny. In this review, we first present a critical survey of experimental measurem…
We use scanning tunneling spectroscopy to investigate the filled and empty electronic states of superconducting single-unit-cell FeSe deposited on SrTiO$_3$(001). We map the momentum-space band structure by combining quasiparticle interference imaging with decay length spectroscopy. In addition to quantifying the filled-state bands, we discover a $Γ$-centered electron pocket 75 meV above the Fermi energy. Our density functional theory calculations show the orbital nature of empty states at $Γ$ and suggest that the Se height is a key tuning parameter of their energies, with broad implications f…
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…
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 simultaneous…
We use density functional theory to study the structure and the band structure of the monolayer FeSe deposited on the SrTiO$_3$ substrate with the additional layer of Se between them. Top of the SrTiO$_3$ is formed by the double TiO layer with and without oxygen vacancies. Several structures with different arrangements of the additional Se atoms above the double TiO layer is considered. Equilibrium structures were found and the band structures for them were obtained. Near the $Γ=(0,0,0)$ point of the Brillouin zone, the hole Fermi surface pockets persist and, additionally, an electron pocket a…
High temperature superconductivity in one unit cell (1 UC) FeSe on SrTiO3 heterostructure has become a research frontier in condensed matter physics and material science. The superconducting transition temperature (Tc) of ultrathin FeSe film is significantly enhanced compared to its bulk counterpart and possibly approaches the liquid nitrogen region according to in situ spectroscopic measurements. Particularly, the Fermi surface topology of 1 UC FeSe consists of no hole pockets at Brillouin zone center, which poses a great challenge to the well accepted s+- wave pairing nesting the sign differ…
Using low-temperature scanning tunneling microscopy (STM), we studied the vortex states of single-layer FeSe film on SrTiO3 (100) substrate, and the local behaviors of superconductivity at sample boundaries. We clearly observed multiple discrete Caroli-de Gennes-Matricon (CdGM) states in the vortex core, and quantitative analysis shows their energies well follow the formula: E = μΔ^2/E_F, where μ is a half integer and Δ is the mean superconducting gap over the Fermi surface. Meanwhile, a fully gapped spectrum without states near zero bias is observed at [110](Fe) oriented boundary of 1 ML and …
Suppression and revival of superconducting phase coherence in monolayer FeSe/SrTiO$_3$
本研究针对单层FeSe/STO界面超导相位相干性难以探测的问题，结合原位互感测量与ARPES表征，发现少层样品抗磁性受抑制的现象及临界层数，揭示了FeTe包覆、紫外照射对超导特性的调控规律，为理解界面超导各向异性提供了实验依据。
Inferior interfacial superconductivity in 1 UC FeSe/SrVO$_3$/SrTiO$_3$ with screened interfacial electron-phonon coupling
本研究构建了界面电子-声子耦合被屏蔽的单层FeSe/SrVO$_3$/SrTiO$_3$超导界面，发现其配对温度低于相关体系，厘清了界面EPC与维度对超导增强的贡献，提供了界面超导研究新平台。
The dream of room temperature superconductors has inspired intense research effort to find routes for enhancing the superconducting transition temperature (Tc). Therefore, single-layer FeSe on a SrTiO3 substrate, with its extraordinarily high Tc amongst all interfacial superconductors and iron based superconductors, is particularly interesting, but the mechanism underlying its high Tc has remained mysterious. Here we show through isotope effects that electrons in FeSe couple with the oxygen phonons in the substrate, and the superconductivity is enhanced linearly with the coupling strength atop…
Suppression of nematicity by tensile strain in multilayer FeSe/SrTiO$_3$ films
结合 ARPES、NMR 和 STM 研究 MBE 生长的多层 FeSe/SrTiO$_3$ 薄膜，发现界面拉伸应变抑制向列性，而远离界面处恢复体相强度。
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…
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 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…
Checkerboard order state in superconducting FeSe/SrTiO3(001) monolayer
该研究通过STM/STS在超导FeSe/SrTiO3(001)单层中发现棋盘电荷序，周期为四倍铁原子间距，仅存在于超导态，且强度在Tc附近增强，暗示其与高Tc超导性相关。
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…
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 …
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 …
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 $T_Δ$ $\approx$ 60 K, but where a zero resistance state is only achieved below $T_{0}$ $<$ 30 K. We sh…
Dual Enhancement of Superconductivity in FeSe/SrTiO3 via Orbital and Correlation Synergy
研究以单层FeSe/SrTiO3为模型，利用针尖诱导拉伸应变实现dz2带与dxy带的杂化，通过两级增强将超导能隙从17.8 meV扩至23.6 meV，确立了调控超导态的新途径。
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.
The theory of EPI with strong forward scattering peak (FSP)[1-3] is recently applied in [4-5] in studying high Tc(~100 K) in a FeSe grown on SrTiO3 [4] and TiO2 [6]. The EPI is due to a long-range dipolar electric field created by the high-energy oxygen vibrations (E0~90 meV) at the interface [4-5]. Besides obtaining new results we also correct some misleading results from the recent literature. We show that the mean-field critical temperature Tc0 is an interplay between the maximal pairing potential and the FSP-width qc. For Tc0~100 K the gap (G) is G~16 meV in agreement with ARPES experiment…
Correlation Enhanced Electron-Phonon Coupling in FeSe/SrTiO$_3$ at a Magic Angle
结合第一性原理动力学平均场理论计算与外延生长实验，发现FeSe/SrTiO$_3$在FeX$_4$四面体魔角处超导能隙峰值与A$_{1g}$模式电子-声子耦合最大化，揭示电子关联通过增强EPC加强Cooper配对。
The discovery of high-temperature (Tc) superconductivity in monolayer FeSe on SrTiO3 raised a fundamental question whether high Tc is commonly realized in monolayer iron-based superconductors. Tetragonal FeS is a key material to resolve this issue because bulk FeS is a superconductor with Tc comparable to that of isostructural FeSe. However, difficulty in synthesizing tetragonal monolayer FeS due to its metastable nature has hindered further investigations. Here we report elucidation of band structure of monolayer FeS on SrTiO3, enabled by a unique combination of in-situ topotactic reaction an…
The FeSe superconductor and its related systems have attracted much attention in the iron-based superconductors owing to their simple crystal structure and peculiar electronic and physical properties. The bulk FeSe superconductor has a superconducting transition temperature (Tc) of ~8 K; it can be dramatically enhanced to 37 K at high pressure. On the other hand, its cousin system, FeTe, possesses a unique antiferromagnetic ground state but is non-superconducting. Substitution of Se by Te in the FeSe superconductor results in an enhancement of Tc up to 14.5 K and superconductivity can persist …
Emergent electronic phenomena in iron-based superconductors have been at the forefront of condensed matter physics for more than a decade. Much has been learned about the origin and intertwined roles of ordered phases, including nematicity, magnetism, and superconductivity, in this fascinating class of materials. In recent years, focus has been centered on the peculiar and highly unusual properties of FeSe and its close cousins. This family of materials has attracted considerable attention due to the discovery of unexpected superconducting gap structures, a wide range of superconducting critic…
The origin of enhanced superconductivity over 50 K in the recently discovered FeSe monolayer films grown on SrTiO$_{3}$ (STO), as compared to 8 K in bulk FeSe, is intensely debated. As with the ferrochalcogenides A$_{x}$Fe$_{2-y}$Se$_{2}$ and potassium doped FeSe, which also have a relatively high superconducting critical temperature ($T_c$), the Fermi surface (FS) of the FeSe/STO monolayer films is free of hole-like FS, suggesting that a Lifshitz transition by which these hole FSs vanish may help increasing $T_c$. However, the fundamental reasons explaining this increase of $T_c$ remain uncle…
The discovery of enhanced superconductivity (SC) in FeSe films grown on SrTiO3 (FeSe/STO) has revitalized the field of Fe-based superconductors. In the ultrathin limit, the superconducting transition temperature Tc is increased by almost an order of magnitude, raising new questions on the pairing mechanism. As in other unconventional superconductors, antiferromagnetic spin fluctuations have been proposed as a candidate to mediate SC in this system. Thus, it is essential to study the evolution of the spin dynamics of FeSe in the ultrathin limit to elucidate their relationship with superconducti…
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…
It is well known that superconductivity in Fe-based materials is favoured under tetragonal symmetry, whereas competing orders such as spin-density-wave (SDW) and nematic orders emerge or are reinforced upon breaking the fourfold (C4) symmetry. Accordingly, suppression of orthorhombicity below the superconducting transition temperature (Tc) is found in underdoped compounds. Epitaxial film growth on selected substrates allows the design of crystal specific lattice distortions. Here we show that despite the breakdown of the C4 symmetry induced by a 5% difference in the lattice parameters, monolay…
Layer thickness and substrate effects on superconductivity in epitaxial FeSe films on BLG/SiC(0001)
利用STM/STS和XPS研究SiC(0001)上双层石墨烯外延FeSe薄膜，发现少层薄膜无超导性，而较厚薄膜在6 K出现超导，表明衬底是抑制二维极限下FeSe超导性的关键因素。
Recently, monolayer CoSb/SrTiO$_3$ has been proposed as a candidate harboring interfacial superconductivity in analogy with monolayer FeSe/SrTiO$_3$. Experimentally, while the CoSb-based compounds manifesting as nanowires and thin films have been realized on SrTiO$_3$ substrates, serving as a rich playground, their electronic structures are still unknown and yet to be resolved. Here, we have fabricated CoSb$_{1-x}$ nanoribbons with quasi-one-dimensional stripes on SrTiO$_3$(001) substrates using molecular beam epitaxy, and investigated the electronic structure by in situ angle-resolved photoem…
In the quest for high temperature superconductors, the interface between a metal and a dielectric was proposed to possibly achieve very high superconducting transition temperature ($T_c$) through interface-assisted pairing. Recently, in single layer FeSe (SLF) films grown on SrTiO$_3$ substrates, signs for $T_c$ up to 65~K have been reported. However, besides doping electrons and imposing strain, whether and how the substrate facilitates the superconductivity are still unclear. Here we report the growth of various SLF films on thick BaTiO$_3$ films atop KTaO$_3$ substrates, with signs for $T_c…
Superconductivity in the cuprate superconductors and the Fe-based superconductors is realized by doping the parent compound with charge carriers, or by application of high pressure, to suppress the antiferromagnetic state. Such a rich phase diagram is important in understanding superconductivity mechanism and other physics in the Cu- and Fe-based high temperature superconductors. In this paper, we report a phase diagram in the single-layer FeSe films grown on SrTiO3 substrate by an annealing procedure to tune the charge carrier concentration over a wide range. A dramatic change of the band str…
We present ARPES data taken from the structurally simplest representative of iron-based superconductors, FeSe, in a wide temperature range. Apart from the variations related to the nematic transition, we detect very pronounced shifts of the dispersions on the scale of hundreds of kelvins. Remarkably, upon warming the sample up, the band structure has a tendency to relax to the one predicted by conventional band structure calculations, right opposite to what is intuitively expected. Our findings shed light on the origin of the dominant interaction shaping the electronic states responsible for h…
We report on the discovery and transport study of the superconducting ground state present at the (111)LaAlO$_3$/SrTiO$_3$ interface. The superconducting transition is consistent with a Berezinskii-Kosterlitz-Thouless transition and its 2D nature is further corroborated by the anisotropy of the critical magnetic field, as calculated by Tinkham. The estimated superconducting layer thickness and coherence length are 10 nm and 60 nm, respectively. The results of this work provide a new platform to clarify the microscopic details of superconductivity at LaAlO$_3$/SrTiO$_3$ interfaces, in particula…
Superconductivity in the PbO-type Structure alpha-FeSe
最近在层状铁基四元氧化物La[O 1-xFx] FeAs中发现了具有相对较高转变温度Tc的超导电性，这是一个真正的惊喜。在很短的时间内出版的后续作品的数量可以看出所产生的兴奋。虽然含Fe元素的合金也存在超导电性，但LaOMPn（M= Fe，Ni; Pn=P，As）是第一个Fe元素对超导电性起关键作用的体系。LaOMPn具有Fe基平面的层状晶体结构。人们很自然地会问，是否存在其他表现出超导性的铁基平面化合物。本文报道了在PbO型α-FeSe化合物中观察到的零电阻转变温度为8 K的超导电性。虽然FeSe已被广泛研究，但一个关键的观察结果是，干净的超导相只存在于那些故意缺硒制备的样品中。真正令人惊讶的是，这种化合物与层状氧磷族化合物具有相同的，也许更简单的平面晶体亚晶格。此外，与LaOFeAs相比，FeSe更容易处理和制造。鉴于PbO型结构化合物的丰富性，这一结果为寻找非常规超导体开辟了一条新的途径。
Since the discovery of high-temperature superconductivity in the thin-film FeSe/SrTiO$_3$ system, iron selenide and its derivates have been intensively scrutinized. Using ab initio density functional theory calculations we review the electronic structures that could be realized in iron-selenide if the structural parameters could be tuned at liberty. We calculate the momentum-dependence of the susceptibility and investigate the symmetry of electron pairing within the random phase approximation. Both the susceptibility and the symmetry of electron pairing depend on the structural parameters in a…
High-Temperature Anomalous Metal States in Iron-Based Interface Superconductors
本文系统研究了SrTiO3衬底上FeSe薄膜的反常金属态，发现零磁场下其可维持至20 K，并证明其源于欧姆耗散调节的涡旋量子隧穿，为理解二维玻色子系统中反常金属态的起源与调控提供了新视角。
The orbital multiplicity in multiband superconductors yields orbital differentiation in normal-state properties, and can lead to orbital-selective spin-fluctuation Cooper pairing. This phenomenon has become increasingly pivotal in clarifying the pairing 'enigma' particularly for multiband high-temperature superconductors. In one-unit-cell (1-UC) FeSe/SrTiO3, the thinnest and highest-Tc member of iron-based superconductors, the standard electron-hole Fermi pocket nesting scenario is apparently not applicable since the Gamma-centered hole pockets are absent, so the actual pairing mechanism is th…
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