Publications

We investigate the effect of charge self-consistency (CSC) in density functional theory plus dynamical mean-field theory (DFT+DMFT) calculations compared to simpler "one-shot" calculations for materials where interaction effects lead to a strong redistribution of electronic charges between different orbitals or between different sites. We focus on two systems close to a metal-insulator transition, for which the importance of CSC is currently not well understood. Specifically, we analyze the strain-related orbital polarization in the correlated metal CaVO

Bardasis-Schrieffer modes in superconductors are fluctuations in subdominant pairing channels, e.g., d-wave fluctuations in an s-wave superconductor. This Rapid Communication shows that these modes also generically occur in excitonic insulators. In s-wave excitonic insulators, a p-wave Bardasis-Schrieffer mode exists below the gap energy, is optically active and hybridizes strongly with photons to form Bardasis-Schrieffer polaritons, which are observable in both far-field and near-field optical experiments.

A detailed understanding of strong matter-photon interactions requires first-principle methods that can solve the fundamental Pauli-Fierz Hamiltonian of non-relativistic quantum electrodynamics efficiently. A possible way to extend well-established electronic-structure methods to this situation is to embed the Pauli-Fierz Hamiltonian in a higher-dimensional light-matter hybrid auxiliary configuration space. In this work we show the importance of the resulting hybrid Fermi-Bose statistics of the polaritons, which are the new fundamental particles of the

We use excited-state quantum chemistry techniques to investigate the intraband absorption of doped semiconductor nanoparticles as a function of doping density, nanoparticle radius, and material properties. Modeling the excess electrons as interacting electrons confined to a sphere, we find that the excitation evolves from single-particle to plasmonic with increasing number of electrons at fixed density, and the threshold number of electrons to produce a plasmon increases with density due to quantum confinement and electron–hole attraction. In addition, the excitation passes through an intermediate regime where it is best characterized as an intraband exciton. We compare equation-of-motion coupled-cluster theory with those of more affordable single-excitation theories and identify the inclusion of electron–hole interactions as essential to describing the evolution of the excitation. Despite the simplicity of our model, the results are in reasonable agreement with the experimental spectra of doped ZnO nanoparticles at a doping density of 1.4 × 10

We study the motion of an interface separating two regions with different electronic orders following a short duration pump that drives the system out of equilibrium. Using a generalized Ginzburg-Landau approach and assuming that the main effect of the nonequilibrium drive is to transiently heat the system we address the question of the direction of interface motion; in other words, which ordered region expands and which contracts after the pump. Our analysis includes the effects of differences in free energy landscape and in order parameter dynamics and identifies circumstances in which the drive may act to increase the volume associated with the subdominant order, for example when the subdominant order has a second order free energy landscape while the dominant order has a first order one.

We develop coupled-cluster theory for systems of electrons strongly coupled to photons, providing a promising theoretical tool in polaritonic chemistry with a perspective of application to all types of fermion-boson coupled systems. We show benchmark results for model molecular Hamiltonians coupled to cavity photons. By comparing to full configuration interaction results for various ground-state properties and optical spectra, we demonstrate that our method captures all key features present in the exact reference, including Rabi splittings and multi-photon processes. Further, a path on how to incorporate our bosonic extension of coupled-cluster theory into existing quantum chemistry programs is given.

We consider a two-band spinless model describing an excitonic insulator (EI) on the two-dimensional square lattice with anisotropic hopping parameters and electron-phonon (el-ph) coupling, inspired by the EI candidate Ta

Recent advances in tuning electronic, magnetic, and topological properties of two-dimensional (2D) magnets have opened a new frontier in the study of quantum physics and promised exciting possibilities for future quantum technologies. In this study, we find that the dual-gate technology can well tune the electronic and topological properties of antiferromagnetic (AFM) even septuple-layer (SL) MnBi

We study equilibrium and nonequilibrium properties of the single-impurity Anderson model with a power-law pseudogap in the density of states. In equilibrium, the model is known to display a quantum phase transition from a generalized Kondo to a local moment phase. In the present work, we focus on the extension of these phases beyond equilibrium, i.e. under the influence of a bias voltage. Within the auxiliary master equation approach combined with a scheme based on matrix product states (MPS) we are able to directly address the current-carrying steady state. Starting with the equilibrium situation, we first corroborate our results by comparing with a direct numerical evaluation of ground state spectral properties of the system by MPS. Here, a scheme to locate the phase boundary by extrapolating the power-law exponent of the self energy produces a very good agreement with previous results obtained by the numerical renormalization group. Our nonequilibrium study as a function of the applied bias voltage is then carried out for two points on either side of the phase boundary. In the Kondo regime the resonance in the spectral function is splitted as a function of the increasing bias voltage. The local moment regime, instead, displays a dip in the spectrum near the position of the chemical potentials. Similar features are observed in the corresponding self energies. The Kondo split peaks approximately obey a power-law behavior as a function of frequency, whose exponents depend only slightly on voltage. Finally, the differential conductance in the Kondo regime shows a peculiar maximum at finite voltages, whose height, however, is below the accuracy level.

We analyze the dynamical nearest-neighbor and next-nearest-neighbor spin correlations in the 4-site and 8-site dynamical cluster approximation to the two-dimensional Hubbard model. Focusing on the robustness of these correlations at long imaginary times, we reveal enhanced ferromagnetic correlations on the lattice diagonal, consistent with the emergence of composite spin-1 moments at a temperature scale that essentially coincides with the pseudo-gap temperature T