Mixed quantum-classical dynamics with time-dependent external fields: A time-dependent density-functional-theory approach
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The development and implementation of increasingly accurate methods for electronic structure calculations mean that, for many atomistic simulation problems, treating light nuclei as classical particles is now one of the most serious approximations. Even th ...
Simulating the exact quantum dynamics of realistic interacting systems is presently a task beyond reach but for the smallest of them, as the numerical cost for solving the time-dependent Schrodinger equation scales exponentially with the number of degrees ...
We investigate, theoretically, the joint relaxation of orbital and structure in postexcitation dynamics of Rydberg states of cluster BaArN (N = 250). Mixed quantum-classical dynamics is used to account for the nonadiabatic transitions among more than 160 e ...
Kohn-Sham density functional theory offers a powerful and robust formalism for investigating the electronic structure of many-body systems while providing a practical balance of accuracy and computational cost unmatched by other methods. Despite this succe ...
We carry out a first-principles atomistic study of the electronic mechanisms of ligand binding and discrimination in the myoglobin protein. Electronic correlation effects are taken into account using one of the most advanced methods currently available, na ...
Characterizing and predicting the nuclear dynamics of electronically excited molecules is of paramount importance to the understanding of photochemical and photophysical processes in molecules and to the development of new technologies in domains like sola ...
We derive a somewhat crude, yet very efficient semiclassical approximation for computing nonadiabatic spectra. The resulting method, which is a generalization of the multiple-surface dephasing representation, includes quantum effects through interference o ...
Including quantum mechanical effects on the dynamics of nuclei in the condensed phase is challenging, because the complexity of exact methods grows exponentially with the number of quantum degrees of freedom. Efforts to circumvent these limitations can be ...
We present a detailed study of the excited state properties of 5-benzyluracil (5BU) in the gas phase and in implicit solvent using different electronic structure approaches ranging from time-dependent density functional theory in the linear response regime ...
CONSPECTUS: Recent developments in nonadiabatic dynamics enabled ab inito simulations of complex ultrafast processes in the condensed phase. These advances have opened new avenues in the study of many photophysical and photochemical reactions triggered by ...