We investigate the excitation spectrum of strongly correlated sodium cobaltate within a realistic many-body description beyond dynamical mean-field theory (DMFT). At lower doping around $x$=0.3, rather close to Mott-critical half-filling, the single-particle spectral function of Na$_x$CoO$_2$ displays an upper Hubbard band which is captured within DMFT. Momentum-dependent self-energy effects beyond DMFT become dominant at higher doping. Around a doping level of $x\sim 0.67$, the incoherent excitations give way to finite-energy spin-polaron excitations in close agreement with optics experiments. These excitations are a direct consequence of the formation of bound states between quasiparticles and paramagnons in the proximity to in-plane ferromagnetic ordering.
We discuss photogenerated midgap states of a one-dimensional (1D) dimerized Mott insulator, potassium-tetracyanoquinodimethane (K-TCNQ). Two types of phonon modes are taken into account: intermolecular and intramolecular vibrations. We treat these phonon modes adiabatically and analyze a theoretical model by using the density-matrix renormalization group (DMRG). Our numerical results demonstrate that the intermolecular lattice distortion is necessary to reproduce the photoinduced midgap absorption in K-TCNQ. We find two types of midgap states. One is a usual polaronic state characterized by a …
The motion of doped electrons or holes in an antiferromagnetic lattice with strong on-site Coulomb interactions touches one of the most fundamental open problems in contemporary condensed matter physics. The doped charge may strongly couple to elementary spin excitations resulting in a dressed quasiparticle which is subject to confinement. This 'spin-polaron' possesses internal degrees of freedom with a characteristic 'ladder' excitation spectrum. Despite its fundamental importance for understanding high-temperature superconductivity, clear experimental spectroscopic signatures of these intern…
Heterointerfaces in complex oxide systems open new arenas in which to test models of strongly correlated material, explore the role of dimensionality in metal-insulator-transitions (MITs) and small polaron formation. Close to the quantum critical point Mott MITs depend on band filling controlled by random disordered substitutional doping. Delta-doped Mott insulators are potentially free of random disorder and introduce a new arena in which to explore the effect of electron correlations and dimensionality. Epitaxial films of the prototypical Mott insulator GdTiO3 are delta-doped by substituting…
We study the electronic spectral properties in two examples of strongly interacting systems: a Mott-Hubbard insulator with additional electron-boson interactions, and a polaronic semiconductor. An approximate unified framework is developed for the high energy part of the spectrum, in which the electrons move in a random field determined by the interplay between magnetic and bosonic fluctuations. When the boson under consideration is a lattice vibration, the resulting isotope effect on the spectral properties is similar in both cases, being strongly temperature and energy dependent, in qualitat…
Polarons are among the most elementary quasiparticles of interacting quantum matter, consisting of a charge carrier dressed by an excited background. In Mott insulators, they take the form of a dopant surrounded by a distorted spin-background and are expected to dictate effective mass, transport properties and interactions between carriers. Despite the fundamental importance of polarons for the electronic structure of strongly correlated systems, access to their internal structure was only recently realized in experiments, while theoretical results are still lacking due to the sign problem. He…
The density driven Mott transition is studied by means of Dynamical Mean-Field Theory in the Hubbard-Holstein model, where the Hubbard term leading to the Mott transition is supplemented by an electron-phonon (e-ph) term. We show that an intermediate e-ph coupling leads to a first-order transition at T=0, which is accompanied by phase separation between a metal and an insulator. The compressibility in the metallic phase is substantially enhanced. At quite larger values of the coupling a polaronic phase emerges coexisting with a non-polaronic metal.
We report on new LEED, STM and ARPES studies of alkali/Si(111) previously established as having a Mott insulating ground state at surface. The observation of a strong temperature dependent Franck-Condon broadening of the surface band together with the novel $\sqrt{3}\times\sqrt{3}\to2(\sqrt{3}\times\sqrt{3})$ charge and lattice ordering below 270 K evidence a surface charge density wave (SCDW) in the strong e-ph coupling limit ($g\approx8$). Both the adiabatic ratio $\hbarω_0/t\approx0.8$ and the effective pairing energy $V_{eff}=U-2g\hbarω_0\approx-800$ $meV$ are consistent with the possible …
Altermagnetic polarons: the fate of alter magnetic band splittings at strong coupling
Universität Stuttgart（斯图加特大学）；University of Warsaw（华沙大学）；Leibniz-Institut für Festkörper- und Werkstoffforschung（莱布尼茨固体与材料研究所）；Technische Universität Dresden（德累斯顿工业大学）
The competition between antiferromagnetism and hole motion in two-dimensional Mott insulators lies at the heart of a doping-dependent transition from an anomalous metal to a conventional Fermi liquid. Condensed matter experiments suggest charge carriers change their nature within this crossover, but a complete understanding remains elusive. We observe such a crossover in Fermi-Hubbard systems on a cold-atom quantum simulator and reveal the transformation of multi-point correlations between spins and holes upon increasing doping at temperatures around the superexchange energy. Conventional obse…
A charge excitation in a two-dimensional Mott insulator is strongly coupled with the surrounding spins, which is observed as magnetic-polaron formations of doped carriers and a magnon sideband in the Mott-gap transition spectrum. However, the dynamics related to the spin sector are difficult to measure. Here, we show that pump-probe reflection spectroscopy with 7-fs laser pulses can detect the optically induced spin dynamics in Nd$_2$CuO$_4$, a cuprate Mott insulator. The bleaching signal at the Mott-gap transition is enhanced at $\sim$18 fs, which corresponds to the spin-relaxation time in ma…
We explore the effects of disordered charged defects on the electronic excitations observed in the photoemission spectra of doped transition metal oxides in the Mott insulating regime by the example of the $R_{1-x}$Ca$_x$VO$_3$ perovskites, where $R=$La,$\dots$,Lu. A fundamental characteristic of these vanadium $d^2$ compounds with partly filled $t_{2g}$ valence orbitals is the persistence of spin and orbital order up to high doping, in contrast to the loss of magnetic order in high-$T_c$ cuprates at low defect concentration. We demonstrate that the disordered electronic structure of doped Mot…
We address the spectral properties of Mott insulators with orbital degrees of freedom, and investigate cases where the orbital symmetry leads to Ising-like superexchange in the orbital sector. The paradigm of a hole propagating by its coupling to quantum fluctuations, known from the spin t-J model, then no longer applies. We find instead that when one of the two orbital flavors is immobile, as in the Falicov-Kimball model, trapped orbital polarons coexist with free hole propagation emerging from the effective three-site hopping in the regime of large on-site Coulomb interaction U. The spectral…
We study the problem of one-dimensional (1D) Luttinger liquids in the insulating Mott-Hubbard phase in the presence of acoustic phonons in the semiclassical limit. We show that solitonic excitations can propagate freely in the system and the energy required to produce a soliton is reduced by a polaronic effect. We find a critical value of the electron-phonon coupling constant for which this energy vanishes.
The elementary optical excitations in two dimensional semiconductors hosting itinerant electrons are attractive and repulsive polarons -- excitons that are dynamically screened by electrons. Exciton-polarons have hitherto been studied in translationally invariant degenerate Fermi systems. Here, we show that electronic charge order breaks the excitonic translational invariance and leads to a direct optical signature in the exciton-polaron spectrum. Specifically, we demonstrate that new optical resonances appear due to spatially modulated interaction between excitons and electrons in an incompre…
Many-body interactions in topological quantum systems can give rise to new phases of matter, which simultaneously exhibit both rich spatial features and topological properties. In this work, we consider spinless fermions on a checkerboard lattice with nearest and next-to-nearest neighbor interactions. We calculate the phase diagram at half filling, which presents, in particular, an interaction-induced quantum anomalous Hall phase. We study the system at incommensurate fillings using an unrestricted Hartree-Fock ansatz and report a rich zoo of solutions such as self-trapped polarons and domain …
We study the spectral function of two-leg Hubbard ladders with the time-dependent density matrix renormalization group method (tDMRG). The high-resolution spectrum displays features of spin-charge separation and a scattering continuum of excitations with coherent bands of bound states `leaking' from it. As the inter-leg hopping is increased, the continuum in the bonding channel moves to higher energies and spinon and holon branches merge into a single coherent quasi-particle band. Simultaneously, the spectrum undergoes a crossover from a regime with two minima at incommensurate values of $k_x$…
We study the effect of strong DC and pulsed electric fields on a Mott insulating system with coupling to optical phonons. A DC field of the order of the gap induces a metallic state characterized by polaronic features in the gap region and a partially inverted population. In this quasi-steady state, the field-induced doublon-hole production is balanced by a phonon-enhanced doublon-hole recombination. The photo-excitation of carriers by a pulsed field leads to similar modifications of the electronic structure in the gap region, and an associated reduction of the doublon life-time. We demonstrat…
As a generic model describing quasi-one-dimensional Mott and Peierls insulators, we investigate the Holstein-Hubbard model for half-filled bands using numerical techniques. Combining Lanczos diagonalization with Chebyshev moment expansion we calculate exactly the photoemission and inverse photoemission spectra and use these to establish the phase diagram of the model. While polaronic features emerge only at strong electron-phonon couplings, pronounced phonon signatures, such as multi-quanta band states, can be found in the Mott insulating regime as well. In order to corroborate the Mott to Pei…
In a number of physical situations, from polarons to Dirac liquids and to non-Fermi liquids, one encounters the "beyond quasiparticles" regime, in which the inelastic scattering rate exceeds the thermal energy of quasiparticles. Transport in this regime cannot be described by the kinetic equation. We employ the Diagrammatic Monte Carlo method to study the mobility of a Fröhlich polaron in this regime and discover a number of non-perturbative effects: a strong violation of the Mott-Ioffe-Regel criterion at intermediate and strong couplings, a mobility minimum at $T \sim Ω$ in the strong-couplin…
We study real-time dynamics of a charge carrier introduced into undoped Mott insulator propagating under a constant electric field F on the t-J ladder and square lattice. We calculate quasistationary current. In both systems adiabatic regime is observed followed by the positive differential resistivity (PDR) at moderate fields where carrier mobility is determined. Quantitative differences between ladder and 2-dimensional (2D) system emerge when at large fields both systems enter negative differential resistivity (NDR) regime. In the ladder system Bloch-like oscillations prevail, while in 2D th…
We study the spectral function of a single hole doped into the (a,b) plane of the Mott insulator LaVO$_3$, with antiferromagnetic (AF) spin order of S=1 spins accompanied by alternating orbital (AO) order of active $\{d_{yz},d_{zx}\}$ orbitals. Starting from the respective t-J model, with spin-orbital superexchange and effective three-site hopping terms, we derive the polaron Hamiltonian and show that a hole couples simultaneously to the collective excitations of the AF/AO phase, magnons and orbitons. Next, we solve this polaron problem using the self-consistent Born approximation and find a s…
As a prototypical Mott insulator with ferromagnetic ordering, YTiO3 (YTO) is of great interest in the study of strong electron correlation effects and orbital ordering. Here we report the first molecular beam epitaxy (MBE) growth of YTO films, combined with theoretical and experimental characterization of the electronic structure and charge transport properties. The obstacles of YTO MBE growth are discussed and potential routes to overcome them are proposed. DC transport and Seebeck measurements on thin films and bulk single crystals identify p-type Arrhenius transport behavior, with an activa…
Studying the antiferromagnetic phase of the Hubbard model by dynamical mean field theory, we observe striking differences with static (Hartree-Fock) mean field: The Slater band is strongly renormalized and spectral weight is transferred to spin-polaron side bands. Already for intermediate values of the interaction $U$ the overall bandwidth is larger than in Hartree-Fock, and the gap is considerably smaller. Such differences survive any renormalization of $U$. Our photoemission experiments for Cr-doped V$_2$O$_3$ show spectra qualitatively well described by dynamical mean field theory.
In this work we investigate doping and temperature dependences of electronic structure of system with strong electronic correlations and strong electron-phonon interaction modeling cuprates in the frameworks of the three-band p-d-Holstein model by a polaronic version of the generalized tight binding (GTB) method. Within this approach the electronic structure is formed by polaronic quasiparticles constructed as excitations between initial and final polaronic multielectron states. Doping and temperature effects are taken into account by occupation numbers of local excited polaronic states and va…
Theory of Angle Resolved Photoemission Spectroscopy of Altermagnetic Mott Insulators
Technical University of Munich（慕尼黑工业大学）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）；Indian Institute of Science, Bangalore（印度科学学院班加罗尔分校）
Basic mechanisms controlling orbital order and orbital fluctuations in transition metal oxides are discussed. The lattice driven classical orbital picture, e.g. like in manganites LaMnO$_3$, is contrasted to the quantum behavior of orbitals in frustrated superexchange models as realised in pseudocubic titanites ATiO$_3$ and vanadates AVO$_3$. In YVO$_3$, the lattice and superexchange effects strongly compete -- this explains the extreme sensitivity of magnetic states to temperature and doping. Lifting the $t_{2g}$ orbital degeneracy by a relativistic spin-orbital coupling is considered on exam…
We study transient dynamics of hole carriers injected at a certain time into a Mott insulator with antiferromagnetic long range order. This is termed ``dynamical hole doping" as contrast with chemical hole doping. Theoretical framework for the transient carrier dynamics are presented based on the two dimensional $t-J$ model. Time dependences of the optical conductivity spectra as well as the one-particle excitation spectra are calculated based on the Keldysh Green's function formalism at zero temperature combined with the self-consistent Born approximation. At early stage after dynamical hole …
A phenomenological model with itinerant bands and local states trapped by the lattice on the Cu-sites, is discussed to describe global features of cuprates. Relative energy positions of localized and itinerant states being tuned (thermodynamically or by doping), the system must undergo 1st order Mott metal-insulator transition. Decreasing the local level (from the metallic end of a stoichiometric compound), charge separation instability occurs first before the Mott transition. Crossing and hybridization between local (flat) and itinerant bands introduce a structure in density of states which m…
An analytical solution of the Mott transition is obtained for the Hubbard model on the Bethe lattice in the large coordination number ($z$) limit. The excitonic binding of doublons (doubly occupied sites) and holons (empty sites) is shown to be the origin of a continuous Mott transition between a metal and an emergent quantum spin liquid insulator. The doublon-holon binding theory enables a different large-$z$ limit and a different phase structure than the dynamical meanfield theory by allowing intersite spinon correlations to lift the $2^N$-fold degeneracy of the local moments in the insulati…
LaTiO$_{3+δ/2}$, NdTiO$_{3+δ/2}$, and Nd$_{1-x}$Sr$_{x}$TiO$_{3+δ/2}$ thin films have been epitaxially grown on (100)SrTiO$_{3}$ and (100)LaAlO$_{3}$ single crystal substrates by using the pulsed laser deposition technique. The oxygen pressure during deposition has been carefully controlled to ensure that the films are lightly doped in the metal side near the metal-Mott-insulator boundary. A steep drop of the effective carrier number at low temperatures has been observed in some of the films, which may correspond to a gradually opening of the Spin Density Wave (SDW) gap due to the antiferromag…
Using spectral ellipsometry, we have measured the dielectric function of a Na$_{0.82(2)}$CoO$_2$ crystal that exhibits bulk antiferromagnetism with T$_{N}$=19.8 K. We identify two prominent transitions as a function of temperature. The first one at 280 K involves marked changes of the electronic and the lattice response that are indicative of charge ordering in the CoO$_{2}$ layers. The second transition coincides with T$_{N}$=19.8 K and reveals a sizeable spin-charge coupling. The data are discussed in terms of charge ordering and formation of magneto-polarons due to a charge-induced spin-sta…
We establish the spectral line shape of orbital excitations created by resonant inelastic X-ray scattering for the model Mott insulator CoO. Improved experimental energy resolution reveals that the line shapes are strikingly different from expectations in a first principles-based atomic multiplet model. Extended theoretical simulations are performed to identify the underlying physical origins, which include a pronounced thermal tail reminiscent of anti-Stokes scattering on the energy gain side of excitations, and an essential contribution from interatomic many-body dynamics on the energy loss …
We study the effects of lattice type on polaron dynamics using a continuous-time quantum Monte-Carlo approach. Holstein and screened Froehlich polarons are simulated on a number of different Bravais lattices. The effective mass, isotope coefficients, ground state energy and energy spectra, phonon numbers, and density of states are calculated. In addition, the results are compared with weak and strong coupling perturbation theory. For the Holstein polaron, it is found that the crossover between weak and strong coupling results becomes sharper as the coordination number is increased. In higher d…
Recently, strong reduction of the quasiparticle peaks and pronounced incoherent structures have been observed in the photoemission spectra of layered cobaltates. Surprisingly, these many-body effects are found to increase near the band insulator regime. We explain these unexpected observations in terms of a novel spin-polaron model for CoO_2 planes which is based on a fact of the spin-state quasidegeneracy of Co^{3+} ions in oxides. Scattering of the photoholes on spin-state fluctuations suppresses their coherent motion. The observed ``peak-dip-hump'' type lineshapes are well reproduced by the…
Determining the nature of band gaps in transition-metal compounds remains challenging. We present a first-principles study on electronic and optical properties of CoO using hybrid functional pseudopotentials. We show that optical absorption spectrum can provide a clear fingerprint to distinguish between Mott-Hubbard, intermediate and charge-transfer insulators. This discrimination is reflected by the qualitative difference in peak satellites due to unique interplay between $d$-$d$ and $p$-$d$ excitations, thus allowing identification from experimental data alone, unlike the existing methods th…
We perform a comprehensive theoretical study of the pressure-induced evolution of the electronic structure, magnetic state, and phase stability of the late transition metal monoxides MnO, FeO, CoO, and NiO using a fully charge self-consistent DFT+dynamical mean-field theory method. Our results reveal that the pressure-induced Mott insulator-to-metal phase transition in MnO-NiO is accompanied by a simultaneous collapse of local magnetic moments and lattice volume, implying a complex interplay between chemical bonding and electronic correlations. We compute the pressure-induced evolution of rela…
In the framework of cluster perturbation theory for the 2D Hubbard and Hubbard-Holstein models at low hole doping we have studied the effect of local and short-range correlations in strongly correlated systems on the anomalous features in the electronic spectrum by investigating the fine structure of quasiparticle bands. Different anomalous features of spectrum are obtained as the result of intrinsic properties of strongly correlated electron and polaron bands in the presence of short-range correlations. Particularly, features similar to the electron-like Fermi-pockets of cuprates at hole dopi…
We have studied the electronic structure and charge ordering (Verwey) transition of magnetite (Fe3O4) by soft x-ray photoemission. Due to the enhanced probing depth and the use of different surface preparations we are able to distinguish surface and volume effects in the spectra. The pseudogap behavior of the intrinsic spectra and its temperature dependence give evidence for the existence of strongly bound small polarons consistent with both dc and optical conductivity. Together with other recent structural and theoretical results our findings support a picture in which the Verwey transition c…
Copper oxides become superconductors rapidly upon doping with electron holes, suggesting a fundamental pairing instability. The Cooper mechanism explains normal superconductivity as an instability of a fermi-liquid state, but high-temperature superconductors derive from a Mott-insulator normal state, not a fermi liquid. We show that precocity to pair condensation with doping is a natural property of competing antiferromagnetism and d-wave superconductivity on a singly-occupied lattice, thus generalizing the Cooper instability to doped Mott insulators, with significant implications for the high…
We derive an effective Hamiltonian for spin polarons forming in weakly doped antiferromagnets and demonstrate that the system becomes superconducting at finite doping. We argue that the driving mechanism which gives rise to superconductivity is lowering of the kinetic energy by formation of mobile antiferromagnetic spin bipolarons. That source of attraction between holes is by definition effective if the antiferromagnetic correlation length is longer than the radius of forming polarons. Notwithstanding that the attraction is strongest in the undoped system with long range order, the supercondu…
Charge transport in the hole-doped quasi-1D model system Y$_{2-x}$Ca$_x$BaNiO$_5$ (x $ leq$ 0.15) is investigated in the 50-300 K temperature range. The resistivity temperature dependence is characterized by a constant activation energy $E_{a}/k_{B} sim$ 1830 K at room temperature while $E_{a}$ decreases upon cooling. We suggest that $E_{a}$ measures the binding energy of the doped holes which form magneto-acoustic polarons when polarizing the neighboring Ni spins. A semi-classical model is proposed which allows to relate the electrical measurements and the bulk magnetic susceptibility. This m…
The translationally invariant diagrammatic quantum perturbation theory (TPT) is applied to the polaron problem on the 1D lattice, modeled through the Holstein Hamiltonian with the phonon frequency omega0, the electron hopping t and the electron-phonon coupling constant g. The self-energy diagrams of the fourth-order in g are calculated exactly for an intermittently added electron, in addition to the previously known second-order term. The corresponding quadratic and quartic corrections to the polaron ground state energy become comparable at t/omega0>1 for g/omega0~(t/omega0)^{1/4} when the ele…
Neutron scattering is used to investigate the single-ion spin and orbital excitations below the Mott-Hubbard gap in CoO. Three excitations are reported at 0.870 $\pm$ 0.009 eV, 1.84 $\pm$ 0.03, and 2.30 $\pm$ 0.15 eV. These were parameterized within a weak crystal field scheme with an intra-orbital exchange of $J(dd)$=1.3 $\pm$ 0.2 eV and a crystal field splitting 10Dq=0.94 $\pm$ 0.10 eV. A reduced spin-orbit coupling of λ=-0.016 $\pm$ 0.003 eV is derived from dilute samples of Mg$_{0.97}$Co$_{0.03}$O, measured to remove complications due to spin exchange and structural distortion parameters w…
How a Mott insulator develops into a weakly coupled metal upon doping is a central question to understanding various emergent correlated phenomena. To analyze this evolution and its connection to the high-$T_c$ cuprates, we study the single-particle spectrum for the doped Hubbard model using cluster perturbation theory on superclusters. Starting from extremely low doping, we identify a heavily renormalized quasiparticle dispersion that immediately develops across the Fermi level, and a weakening polaronic side band at higher binding energy. The quasiparticle spectral weight roughly grows at tw…
