Calculation of the zero-point energy from imaginary-time quantum trajectory dynamics in Cartesian coordinates

A method of molecular dynamics with quantum corrections, practical for studies of large molecular systems, is reviewed. The approach is based on the Bohmian formulation of the time-dependent Schrödinger equation in which a wavefunction is represented by an ensemble of interdependent trajectories. The quantum effects come from the quantum potential acting on trajectories on par with the usual classical potential. The quantum potential is determined from the evolving nuclear wavefunction, i.e. from the quantum trajectory (QT) ensemble itself. For practical and conceptual reasons the quantum potential and corresponding quantum nuclear effect are computed only for the selected light nuclei. For studies of reactive chemical processes, the classical potential is computed on-the-fly using the density functional tight binding method of electronic structure. A massively parallel implementation, based on the message passing interface allows for efficient simulations of ensembles of thousands of trajectories describing systems of up to 200 atoms. As a biochemical application, the approximate QT approach is used to model the tunnelling-dominated proton transfer in soybean-lipoxygenase-1. A materials science application is represented by a study of the nuclear quantum effect on adsorption of hydrogen and deuterium on a C 37 H 15 molecule, which is a model 'flake' of graphene.Keywords: quantum effect; hybrid dynamics of quantum/classical nuclei; on-the-fly electronic structure; densityfunctional tight-binding method

show abstract

“…For example in the ZPE calculations of Ref. [55] an ensemble of ,5000 QTs was adequate for model clusters consisting of 2-11 particles.…”

Section: Molecular Simulation 89mentioning

confidence: 99%

Approximate quantum trajectory dynamics for reactive processes in condensed phase

Garashchuk

Jakowski

Rassolov

2014

Molecular Simulation

Self Cite

View full text Add to dashboard Cite

show abstract

Calculation of the zero-point energy from imaginary-time quantum trajectory dynamics in Cartesian coordinates

Cited by 1 publication

References 52 publications

Approximate quantum trajectory dynamics for reactive processes in condensed phase

Approximate quantum trajectory dynamics for reactive processes in condensed phase

Contact Info

Product

Resources

About