Publications

We demonstrate that a dynamical modification of the Hubbard U in the model charge-transfer insulator NiO can be observed with state-of-the-art time-resolved absorption spectroscopy. Using a self-consistent time-dependent density functional theory plus U computational framework, we show that the dynamical modulation of screening and Hubbard U significantly changes the transient optical spectroscopy. Whereas we find the well-known dynamical Franz-Keldysh effect when the U is frozen, we observe a dynamical band-gap renormalization for dynamical U. The renormalization of the optical gap is found to be smaller than the renormalization of U. This work opens up the possibility of driving a light-induced transition from a charge-transfer into a Mott insulator phase.

The standard description of cavity-modified molecular reactions typically involves a single (resonant) mode, while in reality the quantum cavity supports a range of photon modes. Here we demonstrate that as more photon modes are accounted for, physico-chemical phenomena can dramatically change, as illustrated by the cavity-induced suppression of the important and ubiquitous process of proton-coupled electron-transfer. Using a multi-trajectory Ehrenfest treatment for the photon-modes, we find that self-polarization effects become essential, and we introduce the concept of self-polarization-modified Born-Oppenheimer surfaces as a new construct to analyze dynamics. As the number of cavity photon modes increases, the increasing deviation of these surfaces from the cavity-free Born-Oppenheimer surfaces, together with the interplay between photon emission and absorption inside the widening bands of these surfaces, leads to enhanced suppression. The present findings are general and will have implications for the description and control of cavity-driven physical processes of molecules, nanostructures and solids embedded in cavities.

We present a methodology to calculate radiative carrier capture coefficients at deep defects in semiconductors and insulators from first principles. Electronic structure and lattice relaxations are accurately described with hybrid density functional theory. Calculations of capture coefficients provide an additional validation of the accuracy of these functionals in dealing with localized defect states. We also discuss the validity of the Condon approximation, showing that even in the event of large lattice relaxations the approximation is accurate. We test the method on GaAs:V

Current-driven insulator-metal transitions are in many cases driven by Joule heating proportional to the square of the applied current. Recent nano-imaging experiments in Ca

In this work we present a set of virial relations for many electron systems coupled to field modes, described by the Pauli--Fierz Hamiltonian in dipole approximation and using length gauge. Currently, there is growing interest in solutions of this Hamiltonian due to its relevance for describing molecular systems strongly coupled to photonic modes in cavities, and in the possible modification of chemical properties of such systems compared to the ones in free space. The relevance of such virial relations is demonstrated by showing a connection to mass renormalization and by providing an exact way to obtain total energies from potentials in the framework of Quantum Electrodynamical Density Functional Theory.

We extend the semi-classical trajectory description for the high-order harmonic generation (HHG) from solids by integrating the effect of electron-scattering. Comparing the extended semi-classical trajectory model with a one-dimensional quantum mechanical simulation, we find that the multi-plateau feature of the HHG spectrum is formed by Umklapp scattering under the electron-hole acceleration dynamics by laser fields. Furthermore, by tracing the scattered trajectories in real-space, the model fairly describes the emitted photon energy and the emission timing of the HHG even in the higher plateau regions. We further consider the loss of trajectories by scattering processes with a mean-free-path approximation and evaluate the HHG cutoff energy as a function of laser wavelength. As a result, we find that the trajectory loss by scattering causes the wavelength independence of the HHG from solids.

`Strange metals' with resistivity depending linearly on temperature T down to low-T have been a long-standing puzzle in condensed matter physics. Here, we consider a model of itinerant spin-1/2 fermions interacting via on-site Hubbard interaction and random infinite-ranged spin-spin interaction. We show that the quantum critical point associated with the melting of the spin-glass phase by charge fluctuations displays non-Fermi liquid behaviour, with local spin dynamics identical to that of the Sachdev-Ye-Kitaev family of models. This extends the quantum spin liquid dynamics previously established in the large-M limit of SU(M) symmetric models, to models with physical SU(2) spin-1/2 electrons. Remarkably, the quantum critical regime also features a Planckian linear-T resistivity associated with a T-linear scattering rate and a frequency dependence of the electronic self-energy consistent with the Marginal Fermi Liquid phenomenology.

The Hubbard model and its extensions are important microscopic models for understanding high- $T_c$ superconductivity in cuprates. In the model with next-nearest-neighbor hopping $t'$ (the $t'$- Hubbard model), pairing is strongly influenced by $t'$ . In particular, a recent study on a width-4 cylinder observed quasi-long-rage superconducting order, associated with a negative $t'$ , which was taken to imply superconductivity in the two-dimensional (2D) limit. In this work we study more carefully pairing in the width-4 $t'$-Hubbard model. We show that in this specific system, the pairing symmetry with $t'<0$ is not the ordinary $d$-wave one would expect in the 2D limit. Instead we observe a so-called plaquette d-wave pairing. The plaquette d-wave exists only on a width-4 cylinder, and so is not representative of the 2D limit. We find that a negative $t'$ suppresses the conventional d-wave, leading to plaquette pairing. In contrast, a different $t''$ coupling acting diagonally on the plaquettes suppresses plaquette pairing, leading to conventional $d$-wave pairing.

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.