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We study UV laser induced photodesorption of diatomic molecules from solid surfaces by means of the time-dependent Hartree grid-configuration interaction (TDHG-CI) method [J. Chem. Phys. 93, 4740 (1990)]. Converged partial and total absorption cross sections are computed in several cases to demonstrate the flexibility and accuracy of the method. Comparison to TDHG results without CI corrections is also made. The failure of simple TDHG dynamics to reproduce state resolved rotational cross sections in various strong coupling limits is noted as a justification for the development of TDHG-CI algorithms. © 1993 American Institute of Physics.This work was partially supported by EEC Grant No. SC1.l45.C. RDC acknowledges financial support from the National Science Foundation, Grant No. CHE-9101432, and the Camille and Henry Dreyfus Foundation.Peer Reviewe

Application of the time-dependent Hartree grid–configuration interaction method to the desorption of diatomic molecules from solid surfaces