Molecular dynamics with time dependent quantum Monte Carlo

Christov, Ivan P.

doi:doi:10.1063/1.3031214

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On collisional energy transfer in recombination and dissociation reactions: A Wiener–Hopf problem and the effect of a near elastic peak

The effect of the large impact parameter near-elastic peak of collisional energy transfer for unimolecular dissociation/bimolecular recombination reactions is studied. To this end, the conventional single exponential model, a biexponential model that fits the literature classical trajectory data better, a model with a singularity at zero energy transfer, and the most realistic model, a model with a near-singularity, are fitted to the trajectory data in the literature. The typical effect of the ...

A density matrix-based quasienergy formulation of the Kohn–Sham density functional response theory using perturbation- and time-dependent basis sets

A general method is presented for the calculation of molecular properties to arbitrary order at the Kohn–Sham density functional level of theory. The quasienergy and Lagrangian formalisms are combined to derive response functions and their residues by straightforward differentiation of the quasienergy derivative Lagrangian using the elements of the density matrix in the atomic orbital representation as variational parameters. Response functions and response equations are expressed in the atomic...

In this paper we propose an ab initio method to solve quantum many-body problems of molecular dynamics where both electronic and nuclear degrees are represented by ensembles of trajectories and guiding waves in physical space. Both electrons and nuclei can be treated quantum mechanically where the guiding waves obey a set of coupled Schrödinger equations (quantum-quantum description) or, alternatively, coupled Schrödinger–Newtonian equations are solved for the quantum-classical approximation. The method takes into account local and nonlocal quantum correlation effects in a self-consistent manner. The general formalism is applied to one- and two-dimensional hydrogen molecules subjected to a strong ultrashort optical pulse. Comparison is made with the results from the “exact” Ehrenfest molecular dynamics for the molecular ionization and for the evolution of the internuclear distance as the molecule dissociates.

Article Outline

INTRODUCTION
DERIVING TDQMC MD
LIMITING CASES
ENERGY ESTIMATIONS
NUMERICAL RESULTS
CONCLUSIONS

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KEYWORDS and PACS

Keywords

ab initio calculations, high-speed optical techniques, hydrogen neutral molecules, many-body problems, molecular dynamics method, molecule-photon collisions, photodissociation, photoionisation, Schrodinger equation

PACS

33.80.Eh

Autoionization, photoionization, and photodetachment
33.80.Gj

Diffuse spectra; predissociation, photodissociation
31.15.xv

Molecular dynamics and other numerical methods
31.15.at

Molecule transport characteristics; molecular dynamics; electronic structure of polymers
31.15.am

Relativistic configuration interaction (CI) and many-body perturbation calculations

ARTICLE DATA

Digital Object Identifier

http://dx.doi.org/10.1063/1.3031214

PUBLICATION DATA

ISSN

0021-9606 (print)

1089-7690 (online)

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American Institute of Physics

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