Publications

We revisit the cellular dynamical mean-field theory (CDMFT) for the single band Hubbard model on the square lattice at half filling, reaching real-space cluster sizes of up to 9 x 9 sites. Using benchmarks against direct lattice diagrammatic Monte Carlo at high temperature, we show that the self-energy obtained from a cluster center focused extrapolation converges faster with the cluster size than the periodization schemes previously introduced in the literature. The same benchmark also shows that the cluster spin susceptibility can be extrapolated to the exact result at large cluster size, even though its spatial extension is larger than the cluster size.

We investigate out-of-equilibrium dynamics in an excitonic insulator (EI) with a finite momentum pairing perturbed by a laser-pulse excitation and a sudden coupling to fermionic baths. The transient dynamics of the excitonic order parameter is resolved using the full nonequilibrium Green's function approach and the generalized Kadanoff-Baym ansatz (GKBA) within the second-Born approximation. The comparison between the two approaches after a laser pulse excitation shows a good agreement in the weak and the intermediate photo-doping regime. In contrast, the laser-pulse dynamics resolved by the GKBA does not show a complete melting of the excitonic order after a strong excitation. Instead we observe persistent oscillations of the excitonic order parameter with a predominant frequency given by the renormalized equilibrium bandgap. This anomalous behavior can be overcome within the GKBA formalism by coupling to an external bath, which leads to a transition of the EI system towards the normal state. We analyze the long-time evolution of the system and distinguish decay timescales related to dephasing and thermalization.

Advances in nanophotonics, quantum optics, and low-dimensional materials have enabled precise control of light-matter interactions down to the nanoscale. Combining concepts from each of these fields, there is now an opportunity to create and manipulate photonic matter via strong coupling of molecules to the electromagnetic field. Towards this goal, here we introduce a first principles framework to calculate polaritonic excited-state potential-energy surfaces for strongly coupled light-matter systems. In particular, we demonstrate the applicability of our methodology by calculating the polaritonic excited-state manifold of a Formaldehyde molecule strongly coupled to an optical cavity. This proof-of-concept calculation shows how strong coupling can be exploited to alter photochemical reaction pathways by influencing avoided crossings. Therefore, by introducing an ab initio method to calculate excited-state potential-energy surfaces, our work opens a new avenue for the field of polaritonic chemistry.

Turning a pristine Mott insulator into a correlated metal by chemical doping is a common procedure in strongly correlated materials physics, e.g. underlying the phenomenology of high-T

Recent optical conductivity measurements reveal the presence of Hubbard excitons in certain Mott insulators. In light of these results, it is important to revisit the dynamics of these materials to account for excitonic correlations. We investigate time-resolved excitation and relaxation dynamics as a function of temperature in perovskite-type LaVO

Time and angular resolved photoelectron spectroscopy is a powerful technique to measure electron dynamics in solids. Recent advances in this technique have facilitated band and energy resolved observations of the effect that excited phonons, have on the electronic structure. Here, we show with the help of

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