Critical appraisal of excited state nonadiabatic dynamics simulations of 9H-adenine.

Critical appraisal of excited state nonadiabatic dynamics simulations of 9H-adeninea)

The MP/SOFT methodology for simulations of quantum dynamics: Model study of the photoisomerization of the retinyl chromophore in visual rhodopsin

Rigorous simulations of excited-state nonadiabatic quantum dynamics in polyatomic chromophores are particularly challenging since they equire solving the multichannel time-dependent Schrödinger equation describing nuclear wavepackets evolving on electronically coupled potenial energy surfaces. This paper presents an overview of the matching-pursuit/split-operator-Fourier-transform (MP/SOFT) met...

Nonadiabatic dynamics within time-dependent density functional tight binding method.

A nonadiabatic molecular dynamics is implemented in the framework of the time-dependent density functional tight binding method (TDDFTB) combined with Tully's stochastic surface hopping algorithm. The applicability of our method to complex molecular systems is illustrated on the example of the ultrafast excited state dynamics of microsolvated adenine. Our results demonstrate that in the presenc...

Nuclear quantum effects on the nonadiabatic decay mechanism of an excited hydrated electron.

We present a kinetic analysis of the nonadiabatic decay mechanism of an excited state hydrated electron to the ground state. The theoretical treatment is based on a quantized, gap dependent golden rule rate constant formula which describes the nonadiabatic transition rate between two quantum states. The rate formula is expressed in terms of quantum time correlation functions of the energy gap a...

Large nonadiabatic quantum molecular dynamics simulations on parallel computers

We have implemented a quantummolecular dynamics simulation incorporating nonadiabatic electronic transitions onmassively parallel computers to study photoexcitation dynamics of electrons and ions. The nonadiabatic quantum molecular dynamics (NAQMD) simulation is based on Casida’s linear response time-dependent density functional theory to describe electronic excited states and Tully’s fewestswi...