https://doi.org/10.1140/epjd/e2003-00086-8
Non-adiabatic quantum molecular dynamics: General formalism and case study H2+ in strong laser fields
Institut für Theoretische Physik,
Technische Universität Dresden, 01062 Dresden, Germany
Corresponding authors: a kunert@physik.tu-dresden.de - b schmidt@physik.tu-dresden.de
Received:
5
August
2002
Revised:
29
January
2003
Published online:
29
April
2003
A general formalism of the so-called non-adiabatic quantum
molecular dynamics is presented, which applies to atomic many-body
systems in external laser fields. The theory treats the nuclear
dynamics and electronic transitions simultaneously and self-consistently
in a mixed classical-quantum approach. The equations of motion are
derived from a general action principle by combining time-dependent density
functional theory in basis-set-expansion with classical
molecular dynamics. Structure and properties of the resulting
equations of motion as well as the energy and momentum balance
equations in this formalism are discussed in detail. For the model
system H
, the classical-quantum equations of
motion are solved. The results agree very well with that of full quantum
mechanical calculations. Moreover, from the present calculation a
transparent physical interpretation of the mechanisms of energy
absorption and dissociation dynamics can be obtained. Future
applications and approximations of the formalism presented here are
briefly outlined.
PACS: 36.40.-c – Atomic and molecular clusters / 31.15.Ew – Density-functional theory / 34.50.Gb – Electronic excitation and ionization of molecules; intermediate molecular states (including lifetimes, state mixing, etc.)
© EDP Sciences, Società Italiana di Fisica, Springer-Verlag, 2003
