Time-dependent variational approach to molecules in strong laser fields

Thomas Kreibich, Robert Van Leeuwen, E. K.U. Gross*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

25 Scopus citations


We study the dynamics of the electronic and nuclear degrees of freedom for molecules in strong laser fields using an ansatz for the wavefunction that explicitly incorporates the electron-nuclear correlation. Equations of motion for this wavefunction are derived on the basis of the stationary action principle. The method is tested on a one-dimensional model of the H 2 + molecule that can be solved essentially exactly by numerical integration of the time-dependent Schrödinger equation. By comparison with this exact solution we find that the correlated approach improves significantly on a mean-field treatment, especially for laser fields strong enough to cause substantial dissociation. These results are very promising since our method still has a simple orbital structure and can hence be applied to realistic many-electron molecules.

Original languageAmerican English
Pages (from-to)183-202
Number of pages20
JournalChemical Physics
Issue number1-2
StatePublished - 13 Sep 2004
Externally publishedYes

Bibliographical note

Funding Information:
This work was supported in part by the Deutsche Forschungsgemeinschaft, by the EX!TiNG Research and Training Network of the European Union and by the NANOQUANTA Network of Excellence. E.K.U.G. wishes to thank Ali Alavi, Garnet Chan and Michiel Sprik for inspiring discussions and the warm hospitality at the Cambridge University Computational Chemistry Centre where part of this work was done. A Schlumberger fellowship and a fellowship as visiting fellow at Trinity College, Cambridge are gratefully acknowledged.


  • Action principle
  • Dissociation
  • Intense lasers
  • Ionization
  • Molecules


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