Charge Excitation Spectrum Research Articles

Low-energy plasmon excitations in infinite-layer nickelates

The discovery of superconductivity in infinite-layer nickelates is presently an important topic in condensed-matter physics, and potential similarities to and differences from cuprates are under intense debate. We determine general features of the charge excitation spectrum in nickelates from two opposite viewpoints: (i) Nickelates are regarded as strongly correlated electron systems like cuprate superconductors and thus can be described by the $t\text{\ensuremath{-}}J$ model, and (ii) electron correlation effects are not as strong as in cuprates, and thus, random-phase approximation (RPA) calculations may capture the essential physics. We find that in both cases, plasmon excitations are realized around the momentum transfer $\mathbf{q}=(0,0,{q}_{z})$, although they tend to be damped more strongly in the RPA. In particular, this damping is enhanced by the relatively large interlayer hopping expected in nickelates. Besides reproducing the optical plasmon at $\mathbf{q}=(0,0,0)$ observed in ${\mathrm{Nd}}_{0.8}{\mathrm{Sr}}_{0.2}{\mathrm{NiO}}_{2}$, we obtain low-energy plasmons with gaps of $\ensuremath{\sim}360$ and $\ensuremath{\sim}560$ meV at $\mathbf{q}=(0,0,{q}_{z})$ for finite ${q}_{z}$ in cases (i) and (ii), respectively. The present work offers a possible theoretical hint to answer whether nickelates are cupratelike or not and contributes to the general understanding of the charge dynamics in nickelates.

Quasiparticle excitations in a one-dimensional interacting topological insulator: Application for dopant-based quantum simulation

We study the effects of electron-electron interactions on the charge excitation spectrum of the spinful Su-Schrieffer-Heeger (SSH) model, a prototype of a 1D bulk obstructed topological insulator. In view of recent progress in the fabrication of dopant-based quantum simulators we focus on experimentally detectable signatures of interacting topology in finite lattices. To this end we use Lanczos-based exact diagonalization to calculate the single-particle spectral function in real space which generalizes the local density of states to interacting systems. Its spatial and spectral resolution allows for the direct investigation and identification of edge states. By studying the non-interacting limit, we demonstrate that the topological in-gap states on the boundary are robust against both finite-size effects as well as random bond and onsite disorder which suggests the feasibility of simulating the SSH model in engineered dopant arrays in silicon. While edge excitations become zero-energy spin-like for any finite interaction strength, our analysis of the spectral function shows that the single-particle charge excitations are gapped out on the boundary. Despite the loss of topological protection we find that these edge excitations are quasiparticle-like as long as they remain within the bulk gap. Above a critical interaction strength of $U_c\approx 5 t$ these quasiparticles on the boundary loose their coherence which is explained by the merging of edge and bulk states. This is in contrast to the many-body edge excitations which survive the limit of strong coupling, as established in the literature. Our findings show that for moderate repulsive interactions the non-trivial phase of the interacting SSH model can be detected through remnant signatures of topological single-particle states using single-particle local measurement techniques such as scanning tunneling spectroscopy.

Electron self-energy from quantum charge fluctuations in the layered t−J model with long-range Coulomb interaction

Employing a large-N scheme of the layered t-J model with the long-range Coulomb interaction, which captures fine details of the charge excitation spectra recently observed in cuprate superconductors, we explore the role of the charge fluctuations on the electron self-energy. We fix temperature at zero and focus on quantum charge fluctuations. We find a pronounced asymmetry of the imaginary part of the self-energy Im$\Sigma({\bf k}, \omega)$ with respect to $\omega = 0$, which is driven by strong electron correlation effects. The quasiparticle weight is reduced dramatically, which occurs almost isotropically along the Fermi surface. Concomitantly an incoherent band and a sharp side band are newly generated and acquire sizable spectral weight. All these features are driven by usual on-site charge fluctuations, which are realized in a rather high-energy region and yield plasmon excitations. On the other hand, the low-energy region with the scale of the superexchange interaction J is dominated by bond-charge fluctuations. Surprisingly, compared with the effect of the on-site charge fluctuations, their effect on the electron self-energy is much weaker even if the system approaches close to bond-charge instabilities. Furthermore, quantum charge dynamics does not produce a clear kink nor a pseudogap in the electron dispersion.

Post-growth annealing effects on charge and spin excitations in Nd2−xCexCuO4

We report a Cu K- and L$_3$-edge resonant inelastic x-ray scattering study of charge and spin excitations of bulk Nd$_{2-x}$Ce$_x$CuO$_4$, with focus on post-growth annealing effects. For the parent compound Nd$_2$CuO$_4$ ($x = 0$), a clear charge-transfer gap is observed in the as-grown state, whereas the charge excitation spectra indicate that electrons are doped in the annealed state. This is consistent with the observation that annealed thin-film and polycrystalline samples of RE$_2$CuO$_4$ (RE = rare earth) can become metallic and superconducting at sufficiently high electron concentrations without Ce doping. For $x = 0.16$, a Ce concentration for which it is known that oxygen reduction destroys long-range antiferromagnetic order and induces superconductivity, we find that the high-energy spin excitations of non-superconducting as-grown and superconducting annealed crystals are nearly identical. This finding is in stark contrast to the significant changes in the low-energy spin excitations previously observed via neutron scattering.

Exotic symmetries, duality, and fractons in 2+1-dimensional quantum field theory

We discuss nonstandard continuum quantum field theories in 2+1 dimensions. They exhibit exotic global symmetries, a subtle spectrum of charged excitations, and dualities similar to dualities of systems in 1+1 dimensions. These continuum models represent the low-energy limits of certain known lattice systems. One key aspect of these continuum field theories is the important role played by discontinuous field configurations. In two companion papers, we will present 3+1-dimensional versions of these systems. In particular, we will discuss continuum quantum field theories of some models of fractons.

Non-Hermitian topological Mott insulators in one-dimensional fermionic superlattices

We study interaction-induced Mott insulators, and their topological properties in a 1D non-Hermitian strongly-correlated spinful fermionic superlattice system with either nonreciprocal hopping or complex-valued interaction. For the nonreciprocal hopping case, the low-energy neutral excitation spectrum is sensitive to boundary conditions, which is a manifestation of the non-Hermitian skin effect. However, unlike the single-particle case, particle density of strongly correlated system does not suffer from the non-Hermitian skin effect due to the Pauli exclusion principle and repulsive interactions. Moreover, the anomalous boundary effect occurs due to the interplay of nonreciprocal hopping, superlattice potential, and strong correlations, where some in-gap modes, for both the neutral and charge excitation spectra, show no edge excitations defined via only the right eigenvectors. We show that these edge excitations of the in-gap states can be correctly characterized by only biorthogonal eigenvectors. Furthermore, the topological Mott phase, with gapless particle excitations around boundaries, exists even for the purely imaginary-valued interaction, where the continuous quantum Zeno effect leads to the effective on-site repulsion between two-component fermions.

Efficient Excitations and Spectra within a Perturbative Renormalization Approach.

We present a self-consistent approach for computing the correlated quasiparticle spectrum of charged excitations in iterative computational time. This is based on the auxiliary second-order Green's function approach [Backhouse, O. J. Chem. Theory Comput., 2000], in which a self-consistent effective Hamiltonian is constructed by systematically renormalizing the dynamical effects of the self-energy at second-order perturbation theory. From extensive benchmarking across the W4-11 molecular test set, we show that the iterative renormalization and truncation of the effective dynamical resolution arising from the 2h1p and 1h2p spaces can substantially improve the quality of the resulting ionization potential and electron affinity predictions compared to benchmark values. The resulting method is shown to be superior in accuracy to similarly scaling quantum chemical methods for charged excitations in EOM-CC2 and ADC(2), across this test set, while the self-consistency also removes the dependence on the underlying mean-field reference. The approach also allows for single-shot computation of the entire quasiparticle spectrum, which is applied to the benzoquinone molecule and demonstrates the reduction in the single-particle gap due to the correlated physics, and gives direct access to the localization of the Dyson orbitals.

Time-resolved resonant inelastic x-ray scattering in a pumped Mott insulator

Collective excitations contain rich information about photoinduced transient states in correlated systems. In a Mott insulator, charge degrees of freedom are frozen, but can be activated by photodoping. The energy-momentum distribution of the charge excitation spectrum reflects the propagation of charge degrees of freedom, and provides information about the interplay among various intertwined instabilities on the time scale set by the pump. To reveal charge excitations out of equilibrium, we simulate time-resolved x-ray absorption and resonant inelastic x-ray scattering using a Hubbard model. After pumping, the former resolves photodoping, while the latter characterizes the formation, dispersion, weight, and nonlinear effects of collective excitations. Intermediate-state information from time-resolved resonant inelastic x-ray scattering (trRIXS) can be used to decipher the origin of these excitations, including bimagnons, Mott-gap excitations, doublon and single-electron in-gap states, and anti-Stokes relaxation during an ultrafast pump. This paper provides a theoretical foundation for existing and future trRIXS experiments.

Origin of high-energy charge excitations observed by resonant inelastic X-ray scattering in cuprate superconductors

The recent development of x-ray scattering techniques revealed the charge-excitation spectrum in high-Tc cuprate superconductors. While the presence of a dispersive signal in the high-energy charge-excitation spectrum is well accepted in the electron-doped cuprates, its interpretation and universality are controversial. Since charge fluctuations are observed ubiquitously in cuprate superconductors, the understanding of its origin is a pivotal issue. Here, we employ the layered t − J model with the long-range Coulomb interaction and show that an acoustic-like plasmon mode with a gap at in-plane momentum (0, 0) captures the major features of the high-energy charge excitations. The high-energy charge excitations, therefore, should be a universal feature in cuprate superconductors and are expected also in the hole-doped cuprates. Acoustic-like plasmons in cuprates have not been recognized yet in experiments. We propose several experimental tests to distinguish different interpretations of the high-energy charge excitations.

Dual structure in the charge excitation spectrum of electron-doped cuprates

Motivated by the recent resonant x-ray scattering (RXS) and resonant inelastic x-ray scattering (RIXS) experiments in electron-doped cuprates, we study the charge excitation spectrum in a layered t-J model with the long-range Coulomb interaction. We show that the spectrum is not dominated by a specific type of charge excitations, but by different kinds of charge fluctuations, and is characterized by a dual structure in the energy space. Low-energy charge excitations correspond to various types of bond-charge fluctuations driven by the exchange term (J-term) whereas high-energy charge excitations are due to usual on-site charge fluctuations and correspond to plasmon excitations above the particle-hole continuum. The interlayer coupling, which is frequently neglected in many theoretical studies, is particularly important to the high-energy charge excitations.

Particle-Hole Symmetry of Charge Excitation Spectra in the Paramagnetic Phase of the Hubbard Model

The Kotliar and Ruckenstein slave-boson representation of the Hubbard model allows to obtain an approximation of the charge dynamical response function resulting from the Gaussian fluctuations around the paramagnetic saddle-point in analytical form. Numerical evaluation in the thermodynamical limit yields charge excitation spectra consisting of a continuum, a gapless collective mode with anisotropic zero-sound velocity, and a correlation induced high-frequency mode at $\omega\approx U$. In this work we show that this analytical expression obeys the particle-hole symmetry of the model on any bipartite lattice with one atom in the unit cell. Other formal aspects of the approach are also addressed.

Collective modes in the paramagnetic phase of the Hubbard model

The charge dynamical response function of the Hubbard model is investigated on the square lattice in the thermodynamic limit. The obtained charge-excitation spectra consist of a continuum, a gapless collective mode with anisotropic zero-sound velocity, and a correlation-induced high-frequency mode at $\ensuremath{\omega}\ensuremath{\approx}U$. The correlation function is calculated from Gaussian fluctuations around the paramagnetic saddle point within the Kotliar and Ruckenstein slave-boson representation. Its dependence on the on-site Coulomb repulsion $U$ and density is studied in detail. An approximate analytical expression of the high-frequency mode, which holds for any lattice with one atom in the unit cell, is derived. Comparison with numerical simulations, perturbation theory, and the polarization potential theory is carried out. We also show that magnetic instabilities tend to vanish for $T\ensuremath{\gtrsim}t/6$, and finite-temperature phase diagrams are established.

Combining the Many-Body GW Formalism with Classical Polarizable Models: Insights on the Electronic Structure of Molecular Solids.

We present an original hybrid QM/MM scheme merging the many-body Green's function GW formalism with classical discrete polarizable models and its application to the paradigmatic case of a pentacene crystal. Our calculated transport gap is found to be in excellent agreement with reference periodic bulk GW calculations, together with properly parametrized classical microelectrostatic calculations, and with photoionization measurements at crystal surfaces. More importantly, we prove that the gap is insensitive to the partitioning of pentacene molecules in QM and MM subsystems, as a result of the mutual compensation of quantum and classical polarizabilities, clarifying the relation between polarization energy and delocalization. The proposed hybrid method offers a computationally attractive strategy to compute the full spectrum of charged excitations in complex molecular environments, accounting for both QM and MM contributions to the polarization energy, a crucial requirement in the limit of large QM subsystems.

Transport in Chern-Simons-matter theories

The frequency-dependent longitudinal and Hall conductivities --- $\sigma_{xx}$ and $\sigma_{xy}$ --- are dimensionless functions of $\omega/T$ in 2+1 dimensional CFTs at nonzero temperature. These functions characterize the spectrum of charged excitations of the theory and are basic experimental observables. We compute these conductivities for large $N$ Chern-Simons theory with fermion matter. The computation is exact in the 't Hooft coupling $\lambda$ at $N = \infty$. We describe various physical features of the conductivity, including an explicit relation between the weight of the delta function at $\omega = 0$ in $\sigma_{xx}$ and the existence of infinitely many higher spin conserved currents in the theory. We also compute the conductivities perturbatively in Chern-Simons theory with scalar matter and show that the resulting functions of $\omega/T$ agree with the strong coupling fermionic result. This provides a new test of the conjectured 3d bosonization duality. In matching the Hall conductivities we resolve an outstanding puzzle by carefully treating an extra anomaly that arises in the regularization scheme used.

Density matrix renormalization group study in energy space for a single-impurity Anderson model and an impurity quantum phase transition

The density matrix renormalization group method is applied to obtain the ground state phase diagram of the single impurity Anderson model on the honeycomb lattice at half filling. The calculation of local static quantities shows that the phase diagram contains two distinct phases, the local moment (LM) phase and the asymmetric strong coupling (ASC) phase. These results are supported by the local spin and charge excitation spectra, which exhibit qualitatively different behavior in these two phases and also reveal the existence of the valence fluctuating point at the phase boundary. For comparison, we also study the low-energy effective pseudogap Anderson model. Although the high-energy excitations are obviously different, we find that the ground state phase diagram and the asymptotically low-energy excitations are in good quantitative agreement with those for the single impurity Anderson model on the honeycomb lattice, thus providing the first quantitative justification for the previous studies based on low-energy approximate approaches. Furthermore, we find that the lowest entanglement level is doubly degenerate for the LM phase, whereas it is singlet for the ASC phase and is accidentally three fold degenerate at the valence fluctuating point. Our results therefore clearly demonstrate that the low-lying entanglement spectrum can be used to determine with high accuracy the phase boundary of the impurity quantum phase transition.

Gapped excitations of unconventional fractional quantum Hall effect states in the second Landau level

We report the observation of low-lying collective charge and spin excitations in the second Landau level at $\ensuremath{\nu}=2+1/3$ and also for the very fragile states at $\ensuremath{\nu}=2+2/5$ and $2+3/8$ in inelastic light scattering experiments. These modes exhibit a clear dependence on filling factor and temperature substantiating the unique access to the characteristic neutral excitation spectra of the incompressible fractional quantum Hall effect (FQHE) states. A detailed mode analysis reveals low-energy modes at around 70 $\ensuremath{\mu}\mathrm{eV}$ and a sharp mode slightly below the Zeeman energy interpreted as gap and spin-wave excitation, respectively. The lowest-energy collective charge excitation spectrum at $\ensuremath{\nu}=2+1/3$ exhibits significant qualitative similarities with its cousin state in the lowest Landau level at $\ensuremath{\nu}=1/3$ suggesting similar magnetoroton minima in the neutral excitations. The mode energies differ by a scaling of 0.15 indicating different interaction physics in the $N=0$ and $N=1$ Landau levels. The striking polarization dependence in elastic and inelastic light scattering is discussed in the framework of anisotropic electron phases that allow for the stabilization of nematic FQHE states. The observed excitation spectra provide new insights by accessing quantum phases in the bulk of electron systems and facilitate comparison with different theoretical descriptions of those enigmatic FQHE states.

Doping evolution of spin and charge excitations in the Hubbard model

To shed light on how electronic correlations vary across the phase diagram of the cuprate superconductors, we examine the doping evolution of spin and charge excitations in the single-band Hubbard model using determinant quantum Monte Carlo (DQMC). In the single-particle response, we observe that the effects of correlations weaken rapidly with doping, such that one may expect the random phase approximation (RPA) to provide an adequate description of the two-particle response. In contrast, when compared to RPA, we find that significant residual correlations in the two-particle excitations persist up to $40\%$ hole and $15\%$ electron doping (the range of dopings achieved in the cuprates). These fundamental differences between the doping evolution of single- and multi-particle renormalizations show that conclusions drawn from single-particle processes cannot necessarily be applied to multi-particle excitations. Eventually, the system smoothly transitions via a momentum-dependent crossover into a weakly correlated metallic state where the spin and charge excitation spectra exhibit similar behavior and where RPA provides an adequate description.

D-wave bond-order charge excitations in electron-doped cuprates

We study charge excitation spectra in the two-dimensional model on a square lattice to explore a charge-order tendency recently found in electron-doped cuprates around the carrier density 0.15. The static susceptibility of d-wave charge density, which corresponds to the nematic susceptibility at the momentum transfer , shows two characteristic peaks at momenta of the form and . These two peaks originate from the so-called 2kF scattering processes enhanced by the d-wave character of the bond-charge density. The peak at is much broader, but develops to be very sharp in the vicinity of its instability, whereas the peak at becomes sharper with decreasing temperature, but does not diverge. The equal-time correlation function, which is measured by resonant x-ray scattering, exhibits a momentum dependence similar to the static susceptibility. We also present energy-resolved charge excitation spectra. The spectra show a V-shaped structure around and bend back toward close-to-zero energy due to the charge-order tendency at and . The resulting spectra form gap-like features with a maximal gap at and . We discuss implications for the recent experiments in electron-doped cuprates.

Kondo interactions from band reconstruction in YbInCu(4).

We combine resonant inelastic x-ray scattering and model calculations in the Kondo lattice compound YbInCu_{4}, a system characterized by a dramatic increase in Kondo temperature and associated valence fluctuations below a first-order valence transition at T≃42 K. The bulk-sensitive, element-specific, and valence-projected charge excitation spectra reveal an unusual quasigap in the Yb-derived state density which drives an instability of the electronic structure and renormalizes the low-energy effective Hamiltonian at the transition. Our results provide long-sought experimental evidence for a link between temperature-driven changes in the low-energy Kondo scale and the higher-energy electronic structure of this system.

Toward Optimizing the Performance of Self-Regenerating Pt-Based Perovskite Catalysts

Self-regenerating automotive catalysts owe their remarkable performance to the repeated motion of the precious metal atoms in and out of the perovskite lattice under fluctuating oxidizing and reducing conditions, preventing coalescence of the metal nanoparticles. Here we use resonant inelastic X-ray scattering to characterize the occupied and unoccupied Pt 5d states in two self-regenerating Pt-perovskite catalysts, CaTi0.95Pt0.05O3 and CaZr0.95Pt0.05O3. Upon reduction, the element and symmetry-specific charge excitation spectra reveal a sizable hybridization between the Pt 5d and the Ti 3d or Zr 4d states at the interface between the nanoparticles and the perovskite, which involves the occupied states and is thus invisible in X-ray absorption spectra. A correlation is found between the strength of this d-band hybridization and the proportion of Pt nanoparticles that remain buried below the surface during reduction, indicating that the motion of the Pt atoms toward the surface is hindered by this hybridization specifically, rather than by the Pt–O bonding. These results provide direct evidence that the strength of the metal–metal d-band hybridization plays a pivotal role in determining the efficiency of self-regeneration in perovskite catalysts.