Laser-controlled dissociation of C2H2(2+): Ehrenfest dynamics using time-dependent density functional theory

Wenkel Liang; Christine M Isborn; Xiaosong Li

doi:10.1021/jp811431u

Laser-controlled dissociation of C2H2(2+): Ehrenfest dynamics using time-dependent density functional theory

J Phys Chem A. 2009 Apr 16;113(15):3463-9. doi: 10.1021/jp811431u.

Authors

Wenkel Liang¹, Christine M Isborn, Xiaosong Li

Affiliation

¹ University of Washington, Department of Chemistry, Box 351700, Seattle, Washington 98195-1700, USA.

PMID: 19354313
DOI: 10.1021/jp811431u

Abstract

Intense laser field dissociations of the acetylene dication C(2)H(2)(2+) are studied by an ab initio Ehrenfest dynamics method with time-dependent density functional theory. Various field frequencies (9.5 to approximately 13.6 eV) and field directions are applied to a Boltzmann ensemble of C(2)H(2)(2+) molecules. With the laser field perpendicular to the molecular axis, four fragmentation channels are observed at high frequency with no dominant pathway. With the field parallel to the molecular axis, fragmentations occur at all frequencies and the amount of C-H bond breakage increases with laser frequency. Selective dissociation patterns are observed with low-frequency fields parallel to the molecular axis. A systematic analysis of excited-state potential energy surfaces is used to rationalize the simulation results.