Evolution of spin excitations from bulk to monolayer FeSe
J. Pelliciari, S. Karakuzu, Q. Song, R. Arpaia, A. Nag, M. Rossi, J. Li, T. Yu, X. Chen, R. Peng, M. Garcia-Fernandez, A. C. Walters, Q. Wang, J. Zhao, G. Ghiri… 展开作者
J. Pelliciari, S. Karakuzu, Q. Song, R. Arpaia, A. Nag, M. Rossi, J. Li, T. Yu, X. Chen, R. Peng, M. Garcia-Fernandez, A. C. Walters, Q. Wang, J. Zhao, G. Ghiringhelli, D. Feng, T. A. Maier, K. -J. Zhou, S. Johnston, R. Comin
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 superconductivity. Here, we investigate and compare the spin excitations in bulk and monolayer FeSe grown on STO using high-resolution resonant inelastic x-ray scattering (RIXS) and quantum Monte Carlo (QMC) calculations. Despite the absence of long-range magnetic order, bulk FeSe displays dispersive magnetic excitations reminiscent of other Fe-pnictides. Conversely, the spin excitations in FeSe/STO are gapped, dispersionless, and significantly hardened relative to the bulk counterpart. By comparing our RIXS results with simulations of a bilayer Hubbard model, we connect the evolution of the spin excitations to the Fermiology of the two systems. The present study reveals a remarkable reconfiguration of spin excitations in FeSe/STO, which is essential to understand the role of spin fluctuations in the pairing mechanism.
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 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…
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…
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 pairing mechanism in different classes of correlated materials, including iron based superconductors, is still under debate. For FeSe monolayers, uniform nematic fluctuations have been shown in a lattice Monte Carlo study to play a potentially important role. Here, using dynamical mean field theory calculations for the same model system, we obtain a similar phase diagram and provide an alternative interpretation of the superconductivity in terms of local orbital fluctuations and phase rigidity. Our study clarifies the relation between the superconducting order parameter, superfluid stiffne…
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…
Fermi surface topology and pairing symmetry are two pivotal characteristics of a superconductor. Superconductivity in one monolayer (1ML) FeSe thin film has attracted great interest recently due to its intriguing interfacial properties and possibly high superconducting transition temperature (Tc) over 77 K. Here, we report high-resolution measurements of the Fermi surface and superconducting gaps in 1ML FeSe using angle-resolved photoemission spectroscopy (ARPES). Two ellipse-like electron pockets are clearly resolved overlapping with each other at the Brillouin zone corner. The superconductin…
We comment two incorrect statements given in Ref.1. (A) - In order to show that the electron-phonon interaction (EPI) is very small and irrelevant for superconductivity in 1UC FeSe/SrTiO3 system, the authors of Ref.1 use an EPI coupling constant which does not enter in any theory of superconductivity. So, their conclusion on the smallness of the EPI in 1UC FeSe/SrTiO3 is incorrect. Accordingly, their coupling constant has also nothing to do with the EPI coupling with the forward scattering peak (EPI-FSP), which is proposed recently in order to explain high Tc in 1UC FeSe/SrTiO3. (B) - In Ref.1…
A nodeless $d$-wave state is likely in superconducting monolayer FeSe on SrTiO$_3$. The lack of nodes is surprising but has been shown to be a natural consequence of the observed small interband spin-orbit coupling. Here we examine the evolution from a nodeless state to the nodal state as this spin-orbit coupling is increased from a topological perspective. We show that this evolution depends strongly on the orbital content of the superconducting degrees of freedom. In particular, there are two $d$-wave solutions, which we call orbitally trivial and orbitally nontrivial. In both cases, the nod…
Based on first principle calculations we have investigated the evolution of magnetism in free-standing monolayer FeSe with respect to lattice constant and magnetism in bulk FeSe. The computational results show that the magnetic order in free-standing monolayer FeSe will change from anti-ferromagnetic pair-checkboard order to stripe collinear order along with enlarging lattice constant. The magnetic order in bulk FeSe will change from stripe collinear order to anti-ferromagnetic pair-checkboard order only if structure reconstruction is allowed. We use J$_1$-J$_2$-K$_1$ model to fit the calculat…
Despite of the importance of magnetism in possible relation to other key properties in iron-based superconductors, its understanding is still far from complete especially for FeSe systems. On one hand, the origin of the absence of magnetic orders in bulk FeSe is yet to be clarified. On the other hand, it is still not clear how close monolayer FeSe on SrTiO$_3$, with the highest transition temperature among iron-based superconductors, is to a magnetic instability. Here we investigate magnetic properties of bulk and monolayer FeSe using dynamical mean-field theory combined with density-functiona…
In contrast to bulk FeSe, which exhibits nematic order and low temperature superconductivity, atomic layers of FeSe reverse the situation, having high temperature superconductivity appearing alongside a suppression of nematic order. To investigate this phenomenon, we study a minimal electronic model of FeSe, with interactions that enhance nematic fluctuations. This model is sign problem free, and is simulated using determinant quantum Monte Carlo (DQMC). We developed a DQMC algorithm with parallel tempering, which proves to be an efficient source of global updates and allows us to access the r…
We compare electronic structures of single FeSe layer films on SrTiO$_3$ substrate (FeSe/STO) and K$_x$Fe$_{2-y}$Se$_{2}$ superconductors obtained from extensive LDA and LDA+DMFT calculations with the results of ARPES experiments. It is demonstrated that correlation effects on Fe-3d states are sufficient in principle to explain the formation of the shallow electron -- like bands at the M(X)-point. However, in FeSe/STO these effects alone are apparently insufficient for the simultaneous elimination of the hole -- like Fermi surface around the $Γ$-point which is not observed in ARPES experiments…
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…
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…
We compute the compressibility of the conduction electrons in both bulk orthorhombic FeSe and monolayer FeSe on SrTiO$_3$ substrate, including dynamical electronic correlations within slave-spin mean-field + density-functional theory. Results show a zone of enhancement of the electronic compressibility crossing the interaction-doping phase diagram of these compounds in accord with previous simulations on iron pnictides and in general with the phenomenology of Hund's metals. Interestingly at ambient pressure FeSe is found slightly away from the zone with enhanced compressibility but moved right…
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.
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…
Electronic spectra of typical single FeSe layer superconductors obtained from ARPES data reveal several puzzles: what is the origin of shallow and the so called "replica" bands near M-point and why the hole-like Fermi surfaces near $Γ$-point are absent. Our extensive LDA+DMFT calculations show that correlation effects on Fe-3d states can almost quantitatively reproduce rather complicated band structure, which is observed in ARPES, in close vicinity of the Fermi level for FeSe/STO and K$_x$Fe$_{2-y}$Se$_{2}$. Rather unusual shallow electron-like bands around the M(X)-point in the Brillouin zone…
We have investigated the electronic structures of recently discovered superconductor FeSe by soft-x-ray and hard-x-ray photoemission spectroscopy with high bulk sensitivity. The large Fe 3d spectral weight is located in the vicinity of the Fermi level (EF), which is demonstrated to be a coherent quasi-particle peak. Compared with the results of the band structure calculation with local-density approximation, Fe 3d band narrowing and the energy shift of the band toward EF are found, suggesting an importance of the electron correlation effect in FeSe. The self energy correction provides the larg…
FeSe${}_{0.45}$Te${}_{0.55}$ (FeSeTe) has recently emerged as a promising candidate to host topological superconductivity, with a Dirac surface state and signatures of Majorana bound states in vortex cores. However, correlations strongly renormalize the bands compared to electronic structure calculations, and there is no evidence for the expected bulk band inversion. We present here a comprehensive angle resolved photoemission (ARPES) study of FeSeTe as function of photon energies ranging from 15 - 100 eV. We find that although the top of bulk valence band shows essentially no $k_z$ dispersion…
FeSe undergoes a transition from a tetragonal to a slightly orthorhombic phase at 90\,K, and becomes a superconductor below 8\,K. The orthorhombic phase is sometimes called a nematic phase because quantum oscillation, neutron, and other measurements detect a significant asymmetry in $x$ and $y$. How nematicity affects superconductivity has recently become a matter of intense speculation. Here we employ an advanced \emph{ab-initio} Green's function description of superconductivity and show that bulk tetragonal FeSe would, in principle, superconduct with almost the same T$_{c}$ as the nematic ph…
In contrast to bulk FeSe superconductor, heavily electron-doped FeSe-derived superconductors show relatively high Tc without hole Fermi surfaces and nodal superconducting gap structure, which pose great challenges on pairing theories in the iron-based superconductors. In the heavily electron-doped FeSe-based superconductors, the dominant factors and the exact working mechanism that is responsible for the high Tc need to be clarified. In particular, a clean control of carrier concentration remains to be a challenge for revealing how superconductivity and Fermi surface topology evolves with carr…
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…
FeSe is a unique member of the family of iron-based superconductors, not only because of the high values of $T_{c}$ in FeSe monolayer, but also because in bulk FeSe superconductivity emerges inside a nematic phase without competing with long-range magnetic order. Near $T_{c}$, superconducting order necessarily has $s+d$ symmetry, because nematic order couples linearly the $s$-wave and $d$-wave harmonics of the superconducting order parameter. Here we argue that the near-degeneracy between $s$-wave and $d$-wave pairing instabilities in FeSe, combined with the sign-change of the nematic order pa…
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 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 …
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…
Superconductivity originates from pairing of electrons. Pairing channel on Fermi surface and pairing glue are thus two pivotal issues for understanding a superconductor. Recently, high-temperature superconductivity over 40 K was found in electron-doped FeSe superconductors including K$_x$Fe$_{2-y}$Se$_2$, Li$_{0.8}$Fe$_{0.2}$OHFeSe, and 1 monolayer FeSe thin film. However, their pairing mechanism remains controversial. Here, we studied the systematic evolution of electronic structure in potassium-coated FeSe single crystal. The doping level is controlled precisely by in situ evaporating potass…
One of the most important properties of very recently reported FeSe based superconductors is the robustness of their superconductivity under applied magnetic field. The synthesis and control of superconductivity in FeSe based compounds is rather a difficult task. Synthesis and physical property characterization for optimized superconductivity of FeSe1/2Te1/2 at 13 K is reported here. The compound crystallized in a tetragonal structure with lattice parameters a = 3.8008(10) and c = 6.0187 (15) A. Magnetization measurements indicated bulk superconductivity with lower critical field (Hc1) of arou…
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…
We revisit bulk FeSe through the systematic first-principles electronic structure calculations. We find that there are a series of staggered $n$-mer antiferromagnetic (AFM) states with corresponding energies below that of the collinear AFM state which is the ground state for the parent compounds of most iron-based superconductors. Here the staggered $n$-mer ($n$ any integer $>1$) means that a set of $n$ adjacent spins parallel on a line along $b$-axis with spins in antiparallel between $n$-mers and along $a$-axis. Among them, the lowest energy states are quasi-degenerate staggered dimer and st…
The superconducting transition temperature, $T_{\rm{c}}$, of FeSe can be significantly enhanced several-fold by applying pressure, electron doping, intercalating spacing layer, and reducing dimensionality. Various ordered electronic phases, such as nematicity and spin density waves, have also been observed accompanying high-$T_{\rm{c}}$ superconductivity. Investigation on the evolution of the electronic structure with $T_{\rm{c}}$ is essential to understanding electronic behavior and high-$T_{\rm{c}}$ superconductivity in FeSe and its derived superconductors. In this report, we have found a se…
FeSe is a unique superconductor that can be manipulated to enhance its superconductivity using different routes while its monolayer form grown on different substrates reaches a record high temperature for a two-dimensional system. In order to understand the role played by the substrate and the reduced dimensionality on superconductivity, we examine the superconducting properties of exfoliated FeSe thin flakes by reducing the thickness from bulk down towards 9 nm. Magnetotransport measurements performed in magnetic fields up to 16T and temperatures down to 2K help to build up complete supercond…
We study the lattice dynamics of iron superconductor FeSe, and address the fundamental question of how important is proper description of fluctuating magnetic moments in metallic systems for phonon dispersion and phonon density of states. We show that Density Functional Theory (DFT)+ embedded Dynamical Mean-Field Theory (eDMFT) functional approach, which truly captures the fluctuating local moments, largely eliminates the deficiency of DFT for description of lattice dynamics in correlated metallic systems, and predicts phonon dispersion and phonon density of states in very good agreement with …
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…
Distinctive superconducting behaviors between bulk and monolayer FeSe make it challenging to obtain a unified picture of all FeSe-based superconductors. We investigate the ultrafast quasiparticle (QP) dynamics of an intercalated superconductor (Li1-xFex)OHFe1-ySe, which is a bulk crystal but shares a similar electronic structure with single-layer FeSe on SrTiO3. We obtain the electron-phonon coupling (EPC) constant λA1g (0.22 +/- 0.04), which well bridges that of bulk FeSe crystal and single-layer FeSe on SrTiO3. Moreover, we find that such a positive correlation between λA1g and superconducti…
A general feature of unconventional superconductors is the existence of a superconducting dome in the phase diagram as a function of carrier concentration. For the simplest iron-based superconductor FeSe (with transition temperature Tc ~ 8 K), its Tc can be greatly enhanced by doping electrons via many routes, even up to 65 K in monolayer FeSe/SiTiO3. However, a clear phase diagram with carrier concentration for FeSe-derived superconductors is still lacking. Here, we report the observation of a series of discrete superconducting phases in FeSe thin flakes by continuously tuning carrier concent…
Heavily electron-doped and single-layer FeSe superconduct at much higher temperatures than bulk FeSe. There have been a number of proposals attempting to explain the origin of the enhanced transition temperature, including the proximity to magnetic, nematic and antiferro-orbital critical points, as well as possible strong interfacial phonon coupling in the case of single-layer FeSe. In this paper, we examine the effect of the various mechanisms in an effective two-band model. Within our model, the fluctuations associated with these instabilities contribute to different parts of the effective m…
High-temperature superconductivity and a wide variety of exotic superconducting states discovered in FeSe-based materials have been at the frontier of research on condensed matter physics over the past decade. Unique properties originating from the multiband electronic structure, strongly orbital-dependent phenomena, extremely small Fermi energy, electronic nematicity, and topological aspects give rise to many distinct and fascinating superconducting states. Here, we provide an overview of our current understanding of the superconductivity of {\it bulk} FeSe-based materials, focusing on FeSe 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…
In FeSe-derived superconductors, the lack of a systematic and clean control on the carrier concentration prevents the comprehensive understanding on the phase diagram and the interplay between different phases. Here by K dosing and angle resolved photoemission study on thick FeSe films and FeSe$_{0.93}$S$_{0.07}$ bulk crystals, the phase diagram of FeSe as a function of electron doping is established, which is extraordinarily different from other Fe-based superconductors. The correlation strength remarkably increases with increasing doping, while an insulting phase emerges in the heavily overd…
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…
