Low Temperature Dynamic Polaron Liquid in a Manganite Exhibiting Colossal Magnetoresistance.

Polarons-fermionic charge carriers bearing a strong companion lattice deformation-exhibit a natural tendency for self-localization due to the recursive interaction between electrons and the lattice. While polarons are ubiquitous in insulators, how they evolve in transitions to metallic and superconducting states in quantum materials remains an open question. Here, we use resonant inelastic x-ray scattering to track the electron-lattice coupling in the colossal magneto-resistive bi-layer manganite La_{1.2}Sr_{1.8}Mn_{2}O_{7} across its metal-to-insulator transition. The response in the insulating high-temperature state features harmonic emissions of a dispersionless oxygen phonon at small energy transfer. Upon cooling into the metallic state, we observe a drastic redistribution of spectral weight from the region of these harmonic emissions to a broad high energy continuum. In concert with theoretical calculations, we show that this evolution implies a shift in electron-lattice coupling from static to dynamic lattice distortions that leads to a distinct polaronic ground state in the low temperature metallic phase-a dynamic polaron liquid.

Three-dimensional collective charge excitations in electron-doped copper oxide superconductors.

High-temperature copper oxide superconductors consist of stacked CuO2 planes, with electronic band structures and magnetic excitations that are primarily two-dimensional1,2, but with superconducting coherence that is three-dimensional. This dichotomy highlights the importance of out-of-plane charge dynamics, which has been found to be incoherent in the normal state3,4 within the limited range of momenta accessible by optics. Here we use resonant inelastic X-ray scattering to explore the charge dynamics across all three dimensions of the Brillouin zone. Polarization analysis of recently discovered collective excitations (modes) in electron-doped copper oxides5-7 reveals their charge origin, that is, without mixing with magnetic components5-7. The excitations disperse along both the in-plane and out-of-plane directions, revealing its three-dimensional nature. The periodicity of the out-of-plane dispersion corresponds to the distance between neighbouring CuO2 planes rather than to the crystallographic c-axis lattice constant, suggesting that the interplane Coulomb interaction is responsible for the coherent out-of-plane charge dynamics. The observed properties are hallmarks of the long-sought 'acoustic plasmon', which is a branch of distinct charge collective modes predicted for layered systems8-12 and argued to play a substantial part in mediating high-temperature superconductivity10-12.

Ab Initio Multiplet-Plus-Cumulant Approach for Correlation Effects in X-Ray Photoelectron Spectroscopy.

The treatment of electronic correlations in open-shell systems is among the most challenging problems of condensed matter theory. Current approximations are only partly successful. Ligand-field multiplet theory has been widely successful in describing intra-atomic correlation effects in x-ray spectra, but typically ignores itinerant states. The cumulant expansion for the one-electron Green's function has been successful in describing shake-up effects but ignores atomic multiplets. More complete methods, such as dynamic mean-field theory can be computationally demanding. Here, we show that separating the dynamic Coulomb interactions into local and longer-range parts with ab initio parameters yields a combined multiplet-plus-cumulant approach that accounts for both local atomic multiplets and satellite excitations. The approach is illustrated in transition metal oxides and explains the multiplet peaks, charge-transfer satellites, and distributed background features observed in XPS experiment.

Publisher Correction: Electronic structure of the parent compound of superconducting infinite-layer nickelates.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Electronic structure of the parent compound of superconducting infinite-layer nickelates.

The search continues for nickel oxide-based materials with electronic properties similar to cuprate high-temperature superconductors1-10. The recent discovery of superconductivity in the doped infinite-layer nickelate NdNiO2 (refs. 11,12) has strengthened these efforts. Here, we use X-ray spectroscopy and density functional theory to show that the electronic structure of LaNiO2 and NdNiO2, while similar to the cuprates, includes significant distinctions. Unlike cuprates, the rare-earth spacer layer in the infinite-layer nickelate supports a weakly interacting three-dimensional 5d metallic state, which hybridizes with a quasi-two-dimensional, strongly correlated state with [Formula: see text] symmetry in the NiO2 layers. Thus, the infinite-layer nickelate can be regarded as a sibling of the rare-earth intermetallics13-15, which are well known for heavy fermion behaviour, where the NiO2 correlated layers play an analogous role to the 4f states in rare-earth heavy fermion compounds. This Kondo- or Anderson-lattice-like 'oxide-intermetallic' replaces the Mott insulator as the reference state from which superconductivity emerges upon doping.

Hybridization of Bogoliubov Quasiparticles between Adjacent CuO_{2} Layers in the Triple-Layer Cuprate Bi_{2}Sr_{2}Ca_{2}Cu_{3}O_{10+δ} Studied by Angle-Resolved Photoemission Spectroscopy.

Hybridization of Bogoliubov quasiparticles (BQPs) between the CuO_{2} layers in the triple-layer cuprate high-temperature superconductor Bi_{2}Sr_{2}Cu_{2}Cu_{3}O_{10+δ} is studied by angle-resolved photoemission spectroscopy (ARPES). In the superconducting state, an anticrossing gap opens between the outer- and inner-BQP bands, which we attribute primarily to interlayer single-particle hopping with possible contributions from interlayer Cooper pairing. We find that the d-wave superconducting gap of both BQP bands smoothly develops with momentum without an abrupt jump in contrast to a previous ARPES study. Hybridization between the BQPs also gradually increases in going from the off nodal to the antinodal region, which is explained by the momentum dependence of the interlayer single-particle hopping. As possible mechanisms for the enhancement of the superconducting transition temperature, the hybridization between the BQPs as well as the combination of phonon modes of the triple CuO_{2} layers and spin fluctuations represented by a four-well model are discussed.

Interfacial mode coupling as the origin of the enhancement of T(c) in FeSe films on SrTiO3.

Films of iron selenide (FeSe) one unit cell thick grown on strontium titanate (SrTiO3 or STO) substrates have recently shown superconducting energy gaps opening at temperatures close to the boiling point of liquid nitrogen (77 kelvin), which is a record for the iron-based superconductors. The gap opening temperature usually sets the superconducting transition temperature Tc, as the gap signals the formation of Cooper pairs, the bound electron states responsible for superconductivity. To understand why Cooper pairs form at such high temperatures, we examine the role of the SrTiO3 substrate. Here we report high-resolution angle-resolved photoemission spectroscopy results that reveal an unexpected characteristic of the single-unit-cell FeSe/SrTiO3 system: shake-off bands suggesting the presence of bosonic modes, most probably oxygen optical phonons in SrTiO3 (refs 5, 6, 7), which couple to the FeSe electrons with only a small momentum transfer. Such interfacial coupling assists superconductivity in most channels, including those mediated by spin fluctuations. Our calculations suggest that this coupling is responsible for raising the superconducting gap opening temperature in single-unit-cell FeSe/SrTiO3.

Stroboscopic Tests for Thermalization of Electrons in Pump-Probe Experiments.

One of the goals of pump-probe spectroscopies is to determine how electrons relax after they have been driven out of equilibrium. It is challenging to determine how close electrons are to a thermal state solely by fitting their distribution to a Fermi-Dirac distribution. Instead, we propose that one compare the effective temperatures of both fermions and collective bosonic modes (derived from the fermions) to determine the distance from a thermal state. Measurements of effective fermionic and bosonic temperatures can be achieved directly via photoemission and nonresonant Raman scattering. Their difference quantifies the distance from thermal equilibrium.

Pressure Effects on the 4f Electronic Structure of Light Lanthanides.

Using the satellite structure of the Lγ_{1} line in nonresonant x-ray emission spectra, we probe the high-pressure evolution of the bare 4f signature of the early light lanthanides at ambient temperature. For Ce and Pr the satellite peak experiences a sudden reduction concurrent with their respective volume collapse (VC) transitions. These new experimental results are supported by calculations using state-of-the-art extended atomic structure codes for Ce and Pr, and also for Nd, which does not exhibit a VC. Our work suggests that changes to the 4f occupation are more consistently associated with evolution of the satellite than is the reduction of the 4f moment. Indeed, we show that in the case of Ce, mixing of a higher atomic angular momentum state, driven by the increased hybridization, acts to obscure the expected satellite reduction. These measurements emphasize the importance of a unified study of a full set of microscopic observables to obtain the most discerning test of the underlying, fundamental f-electron phenomena at high pressures.

Ideal charge-density-wave order in the high-field state of superconducting YBCO.

The existence of charge-density-wave (CDW) correlations in cuprate superconductors has now been established. However, the nature of the CDW ground state has remained uncertain because disorder and the presence of superconductivity typically limit the CDW correlation lengths to only a dozen unit cells or less. Here we explore the field-induced 3D CDW correlations in extremely pure detwinned crystals of YBa2Cu3O2 (YBCO) ortho-II and ortho-VIII at magnetic fields in excess of the resistive upper critical field ([Formula: see text]) where superconductivity is heavily suppressed. We observe that the 3D CDW is unidirectional and possesses a long in-plane correlation length as well as significant correlations between neighboring CuO2 planes. It is significant that we observe only a single sharply defined transition at a critical field proportional to [Formula: see text], given that the field range used in this investigation overlaps with other high-field experiments including quantum oscillation measurements. The correlation volume is at least two to three orders of magnitude larger than that of the zero-field CDW. This is by far the largest CDW correlation volume observed in any cuprate crystal and so is presumably representative of the high-field ground state of an "ideal" disorder-free cuprate.

Light-Enhanced Spin Fluctuations and d-Wave Superconductivity at a Phase Boundary.

Time-domain techniques have shown the potential of photomanipulating existing orders and inducing new states of matter in strongly correlated materials. Using time-resolved exact diagonalization, we perform numerical studies of pump dynamics in a Mott-Peierls system with competing charge and spin density waves. A light-enhanced d-wave superconductivity is observed when the system resides near a quantum phase boundary. By examining the evolution of spin, charge, and superconducting susceptibilities, we show that a subdominant state in equilibrium can be stabilized by photomanipulating the charge order to allow superconductivity to appear and dominate. This work provides an interpretation of light-induced superconductivity from the perspective of order competition and offers a promising approach for designing novel emergent states out of equilibrium.

Tailoring the nature and strength of electron-phonon interactions in the SrTiO3(001) 2D electron liquid.

Surfaces and interfaces offer new possibilities for tailoring the many-body interactions that dominate the electrical and thermal properties of transition metal oxides. Here, we use the prototypical two-dimensional electron liquid (2DEL) at the SrTiO3(001) surface to reveal a remarkably complex evolution of electron-phonon coupling with the tunable carrier density of this system. At low density, where superconductivity is found in the analogous 2DEL at the LaAlO3/SrTiO3 interface, our angle-resolved photoemission data show replica bands separated by 100 meV from the main bands. This is a hallmark of a coherent polaronic liquid and implies long-range coupling to a single longitudinal optical phonon branch. In the overdoped regime the preferential coupling to this branch decreases and the 2DEL undergoes a crossover to a more conventional metallic state with weaker short-range electron-phonon interaction. These results place constraints on the theoretical description of superconductivity and allow a unified understanding of the transport properties in SrTiO3-based 2DELs.

Using Nonequilibrium Dynamics to Probe Competing Orders in a Mott-Peierls System.

Competition between ordered phases, and their associated phase transitions, are significant in the study of strongly correlated systems. Here, we examine one aspect, the nonequilibrium dynamics of a photoexcited Mott-Peierls system, using an effective Peierls-Hubbard model and exact diagonalization. Near a transition where spin and charge become strongly intertwined, we observe antiphase dynamics and a coupling-strength-dependent suppression or enhancement in the static structure factors. The renormalized bosonic excitations coupled to a particular photoexcited electron can be extracted, which provides an approach for characterizing the underlying bosonic modes. The results from this analysis for different electronic momenta show an uneven softening due to a stronger coupling near k_{F}. This behavior reflects the strong link between the fermionic momenta, the coupling vertices, and ultimately, the bosonic susceptibilities when multiple phases compete for the ground state of the system.

Superconducting Gap Anisotropy in Monolayer FeSe Thin Film.

Superconductivity originates from pairing of electrons near the Fermi energy. The Fermi surface topology and pairing symmetry are thus two pivotal characteristics of a superconductor. Superconductivity in one monolayer (1 ML) FeSe thin film has attracted great interest recently due to its intriguing interfacial properties and possibly high superconducting transition temperature over 65 K. Here, we report high-resolution measurements of the Fermi surface and superconducting gaps in 1 ML FeSe using angle-resolved photoemission spectroscopy. Two ellipselike electron pockets are clearly resolved overlapping with each other at the Brillouin zone corner. The superconducting gap is nodeless but moderately anisotropic, which puts strong constraint on determining the pairing symmetry. The gap maxima locate on the d_{xy} bands along the major axis of the ellipse and four gap minima are observed at the intersections of electron pockets. The gap maximum location combined with the Fermi surface geometry deviate from a single d-wave, extended s-wave or s_{±} gap function, suggesting an important role of the multiorbital nature of Fermi surface and orbital-dependent pairing in 1 ML FeSe. The gap minima location may be explained by a sign change on the electron pockets, or a competition between intra- and interorbital pairing.

Distinct Electronic Structure for the Extreme Magnetoresistance in YSb.

An extreme magnetoresistance (XMR) has recently been observed in several nonmagnetic semimetals. Increasing experimental and theoretical evidence indicates that the XMR can be driven by either topological protection or electron-hole compensation. Here, by investigating the electronic structure of a XMR material, YSb, we present spectroscopic evidence for a special case which lacks topological protection and perfect electron-hole compensation. Further investigations reveal that a cooperative action of a substantial difference between electron and hole mobility and a moderate carrier compensation might contribute to the XMR in YSb.

Interface ferroelectric transition near the gap-opening temperature in a single-unit-cell FeSe film grown on Nb-Doped SrTiO3 substrate.

We report findings of strong anomalies in both mutual inductance and inelastic Raman spectroscopy measurements of single-unit-cell FeSe film grown on Nb-doped SrTiO3, which occur near the temperature where the superconductinglike energy gap opens. Analysis suggests that the anomaly is associated with a broadened ferroelectric transition in a thin layer near the FeSe/SrTiO3 interface. The coincidence of the ferroelectric transition and gap-opening temperatures adds credence to the central role played by the film-substrate interaction on the strong Cooper pairing in this system. We discuss scenarios that could explain such a coincidence.

Real-space visualization of remnant Mott gap and magnon excitations.

We demonstrate the ability to visualize real-space dynamics of charge gap and magnon excitations in the Mott phase of the single-band Hubbard model and the remnants of these excitations with hole or electron doping. At short times, the character of magnetic and charge excitations is maintained even for large doping away from the Mott and antiferromagnetic phases. Doping influences both the real-space patterns and long timescales of these excitations with a clear carrier asymmetry attributable to particle-hole symmetry breaking in the underlying model. Further, a rapidly oscillating charge-density-wave-like pattern weakens, but persists as a visible demonstration of a subleading instability at half-filling which remains upon doping. The results offer an approach to analyzing the behavior of systems where momentum space is either inaccessible or poorly defined.

Nonequilibrium "melting" of a charge density wave insulator via an ultrafast laser pulse.

We employ an exact solution of the simplest model for pump-probe time-resolved photoemission spectroscopy in charge-density-wave systems to show how, in nonequilibrium, the gap in the density of states disappears while the charge density remains modulated, and then the gap reforms after the pulse has passed. This nonequilibrium scenario qualitatively describes the common short-time experimental features in TaS(2) and TbTe(3), indicating a quasiuniversality for nonequilibrium "melting" with qualitative features that can be easily understood within a simple picture.

Distinguishing bulk and surface electron-phonon coupling in the topological insulator Bi(2)Se(3) using time-resolved photoemission spectroscopy.

We report time- and angle-resolved photoemission spectroscopy measurements on the topological insulator Bi(2)Se(3). We observe oscillatory modulations of the electronic structure of both the bulk and surface states at a frequency of 2.23 THz due to coherent excitation of an A(1g) phonon mode. A distinct, additional frequency of 2.05 THz is observed in the surface state only. The lower phonon frequency at the surface is attributed to the termination of the crystal and thus reduction of interlayer van der Waals forces, which serve as restorative forces for out-of-plane lattice distortions. Density functional theory calculations quantitatively reproduce the magnitude of the surface phonon softening. These results represent the first band-resolved evidence of the A(1g) phonon mode coupling to the surface state in a topological insulator.

Electron-mediated relaxation following ultrafast pumping of strongly correlated materials: model evidence of a correlation-tuned crossover between thermal and nonthermal states.

We examine electron-electron mediated relaxation following ultrafast electric field pump excitation of the fermionic degrees of freedom in the Falicov-Kimball model for correlated electrons. The results reveal a dichotomy in the temporal evolution of the system as one tunes through the Mott metal-to-insulator transition: in the metallic regime relaxation can be characterized by evolution toward a steady state well described by Fermi-Dirac statistics with an increased effective temperature; however, in the insulating regime this quasithermal paradigm breaks down with relaxation toward a nonthermal state with a complicated electronic distribution as a function of momentum. We characterize the behavior by studying changes in the energy, photoemission response, and electronic distribution as functions of time. This relaxation may be observable qualitatively on short enough time scales that the electrons behave like an isolated system not in contact with additional degrees of freedom which would act as a thermal bath, especially when using strong driving fields and studying materials whose physics may manifest the effects of correlations.