Restricted open-shell Kohn-Sham theory: simulation of the pyrrole photodissociation.
The authors study the photodissociation reactions of pyrrole and N-methylpyrrole using first-principles molecular dynamics. The first excited state is described with restricted open-shell Kohn-Sham theory. They find a small barrier in the excited state potential energy surface. The possibility of energy redistribution near the Franck-Condon region leads to two different reaction channels in on-the-fly simulations on a single diabatic potential energy surface. The results are discussed in comparison with previous ab initio calculations and with experiments.
Frank
Irmgard
I
Department Chemie und Biochemie, Universitat München, Butenandtstrasse 11, 81377 München, Germany. frank@cup.uni-muenchen.de
Damianos
Konstantina
K