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A novel mixed quantum-classical approach to simulating nonadiabatic dynamics of molecules at metal surfaces is presented. The method combines the numerically exact hierarchical equations of motion approach for the quantum electronic degrees…
Large scale electronic structure calculations require modern high performance computing (HPC) resources and, as important, mature HPC applications that can make efficient use of those. Real-space grid-based applications of Density…
The theoretical analysis of the Adiabatic Quantum Computation protocol presents several challenges resulting from the difficulty of simulating, with classical resources, the unitary dynamics of a large quantum device. We present here a…
We calculate the nonadiabatic relativistic correction to rovibrational energy levels of H$_2$, D$_2$, and HD molecules using the nonadiabatic perturbation theory. This approach allows one to obtain nonadiabatic corrections to all the…
A mixed quantum-classical approach to simulate the coupled dynamics of electrons and nuclei in nanoscale molecular systems is presented. The method relies on a second order expansion of the Lagrangian in time-dependent density functional…
This report presents a new approach for treating the coupling of electrons and nuclei in quantum mechanical calculations for molecules and condensed matter. It includes the standard "Born-Oppenheimer approximation" as a special case but…
The molecular junction geometry is modelled in terms of nuclear degrees of freedom that are embedded in a stochastic quantum environment of non-equilibrium electrons. Time-evolution of the molecular geometry is governed via a mean force, a…
We present a thermodynamically consistent method by which equations of state based on nonrelativistic potential models can be modified so that they respect causality at high densities, both at zero and finite temperature (entropy). We…
In this paper we propose an ab initio method to solve quantum many-body problems of molecular dynamics where both the electronic and the nuclear degrees are represented by ensembles of trajectories and guiding waves in physical space. Both…
The purpose of this text is to give a self-contained description of the basic theory of the projector augmented-wave (PAW) method, as well as most of the details required to make the method work in practice. These two topics are covered in…
We present valence electron Compton profiles calculated within the density-functional theory using the all-electron full-potential projector augmented-wave method (PAW). Our results for covalent (Si), metallic (Li, Al) and hydrogen-bonded…
Ultrafast electron diffraction/microscopy technique enables us to investigate the nonequilibrium dynamics of crystal structures in the femtosecond-nanosecond time domain. However, the electron diffraction intensities are in general…
Time-dependent orbital-free density functional theory (TD-OFDFT) is an efficient ab-initio method for calculating the electronic dynamics of large systems. In comparison to standard TD-DFT, it computes only a single electronic state…
Solving the time-dependent Schr\"odinger equation (TDSE) is pivotal for modeling non-adiabatic electron dynamics, a key process in ultrafast spectroscopy and laser-matter interactions. However, exact solutions to the TDSE remain…
The non-radiative electron-relaxation dynamics in C$_{60}$ molecule is studied after selective initial photoexcitations. The methodology includes nonadibabtic molecular simulation combined with time-dependent density functional theory (DFT)…
High-harmonic generation (HHG) is a nonlinear process in which a material sample is irradiated by intense laser pulses, causing the emission of high harmonics of the incident light. HHG has historically been explained by theories employing…
We develop numerical methods to calculate electron dynamics in crystalline solids in real-time time-dependent density functional theory employing exchange-correlation potentials which reproduce band gap energies of dielectrics; a meta…
We discuss and analyze the virtual element method on general polygonal meshes for the time-dependent Poisson-Nernst-Planck equations, which are a nonlinear coupled system widely used in semiconductors and ion channels. The spatial…
Non-adiabatic molecular phenomena, arising from the breakdown of the Born-Oppenheimer approximation, govern the fate of virtually all photo-physical and photochemical processes and limit the quantum efficiency of molecules and other…
Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an…