Time-dependent variational approach to molecules in strong laser fields

Thomas Kreibich; Robert Van Leeuwen; E. K.U. Gross

doi:10.1016/j.chemphys.2004.04.016

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 journal › Article › peer-review

25 Scopus citations

Abstract

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 language	English
Pages (from-to)	183-202
Number of pages	20
Journal	Chemical Physics
Volume	304
Issue number	1-2
DOIs	https://doi.org/10.1016/j.chemphys.2004.04.016
State	Published - 13 Sep 2004
Externally published	Yes

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.

Keywords

Action principle
Dissociation
Intense lasers
Ionization
Molecules

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10.1016/j.chemphys.2004.04.016

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title = "Time-dependent variational approach to molecules in strong laser fields",

abstract = "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 Schr{\"o}dinger 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.",

keywords = "Action principle, Dissociation, Intense lasers, Ionization, Molecules",

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AU - Van Leeuwen, Robert

AU - Gross, E. K.U.

N1 - 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.

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N2 - 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.

AB - 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.

KW - Action principle

KW - Dissociation

KW - Intense lasers

KW - Ionization

KW - Molecules

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JF - Chemical Physics

IS - 1-2

ER -

Time-dependent variational approach to molecules in strong laser fields

Abstract

Bibliographical note

Keywords

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