We demonstrate the feasibility of the time-linear scaling formulation of the $GW$ method [ Phys. Rev. Lett. 124, 076601 (2020)] for ab initio simulations of optically driven two-dimensional materials. The time-dependent $GW$ equations are derived and solved numerically in the basis of Bloch states. We address carrier multiplication and relaxation in photoexcited graphene and find deviations from the typical exponential behavior predicted by the Markovian Boltzmann approach. For a resonantly pumped semiconductor we discover a self-sustained screening cascade leading to the Mott transition of coherent excitons. Our results draw attention to the importance of non-Markovian and dynamical screening effects in out-of-equilibrium phenomena.

The interaction of electrons with quantized phonons and photons underlies the ultrafast dynamics of systems ranging from molecules to solids, and it gives rise to a plethora of physical phenomena experimentally accessible using time-resolved techniques. Green’s function methods offer an invaluable interpretation tool since scattering mechanisms of growing complexity can be selectively incorporated in the theory. Currently, however, real-time Green’s function simulations are either prohibitively expensive due to the cubic scaling with the propagation time or do neglect the feedback of electrons on the bosons, thus violating energy conservation. We put forward a computationally efficient Green’s function scheme which overcomes both limitations. The numerical effort scales linearly with the propagation time while the simultaneous dressing of electrons and bosons guarantees the fulfillment of all fundamental conservation laws. We present a real-time study of the phonon-driven relaxation dynamics in an optically excited narrow band-gap insulator, highlighting the nonthermal behavior of the phononic degrees of freedom. Our formulation paves the way to first-principles simulations of electron-boson systems with unprecedented long propagation times.

A theoretical analysis of the second harmonic generation of light from spherical particles is presented that unifies existing theories which are valid in the special cases of small particle size (Rayleigh limit), small refraction index, radiation by nonlocal dipole and quadrupole moments. We study the angular distribution of second harmonic using a nonlinear generalization of the linear Mie theory.

We present a diagrammatic approach to construct self-energy approximations within many-body perturbation theory with positive spectral properties. The method cures the problem of negative spectral functions which arises from a straightforward inclusion of vertex diagrams beyond the $GW$ approximation. Our approach consists of a two-step procedure: We first express the approximate many-body self-energy as a product of half-diagrams and then identify the minimal number of half-diagrams to add in order to form a perfect square. The resulting self-energy is an unconventional sum of self-energy diagrams in which the internal lines of half a diagram are time-ordered Green's functions, whereas those of the other half are anti-time-ordered Green's functions, and the lines joining the two halves are either lesser or greater Green's functions. The theory is developed using noninteracting Green's functions and subsequently extended to self-consistent Green's functions. Issues related to the conserving properties of diagrammatic approximations with positive spectral functions are also addressed. As a major application of the formalism we derive the minimal set of additional diagrams to make positive the spectral function of the $GW$ approximation with lowest-order vertex corrections and screened interactions. The method is then applied to vertex corrections in the three-dimensional homogeneous electron gas by using a combination of analytical frequency integrations and numerical Monte Carlo momentum integrations to evaluate the diagrams.

Charge excitations across an electronic band gap play an important role in opto-electronics and light harvesting. In contrast to conventional semiconductors, studies of above-band-gap photoexcitations in strongly correlated materials are still in their infancy. Here we reveal the ultrafast dynamics controlled by Hund’s physics in strongly correlated photoexcited NiO. By combining time-resolved two-photon photoemission experiments with state-of-the-art numerical calculations, an ultrafast (≲10 fs) relaxation due to Hund excitations and related photo-induced in-gap states are identified. Remarkably, the weight of these in-gap states displays long-lived coherent THz oscillations up to 2 ps at low temperature. The frequency of these oscillations corresponds to the strength of the antiferromagnetic superexchange interaction in NiO and their lifetime vanishes slightly above the Néel temperature. Numerical simulations of a two-bandt-Jmodel reveal that the THz oscillations originate from the interplay between local many-body excitations and antiferromagnetic spin correlations.

Simulations of interacting electrons and bosons out of equilibrium, starting from first principles and aiming at realistic multiscale scenarios, is a grand theoretical challenge. Here, using the formalism of nonequilibrium Green's functions and relying in a crucial way on the recently discovered time-linear formulation of the Kadanoff-Baym equations, we present a versatile toolbox for the simulation of correlated electron-boson dynamics. A large class of methods are available, from the Ehrenfest to the dressed $GD$ for the treatment of electron-boson interactions in combination with perturbative, i.e., Hartree-Fock and second-Born, or nonperturbative, i.e., $GW$ and $T$ matrices either without or with exchange effects, for the treatment of the Coulomb interaction. In all cases the numerical scaling is linear in time and the equations of motion satisfy all fundamental conservation laws.