Restricted open-shell Kohn-Sham theory for pi-pi* transitions. III. Dynamics of aggregates.
We present molecular-dynamics simulations for 1,3-butadiene, 2,3-dimethyl-1,3-butadiene, and cyclopentadiene at finite temperature using periodic boundary conditions. These systems form weakly bound aggregates in the ground state and exhibit bond formation in the excited state. Monomeric excitation of an ensemble of butadiene molecules leads to a transfer of the excitation between two molecules in the excited state with an intermediate delocalization of the wave function over both moieties.
Nonnenberg
Christel
C
Department Chemie und Biochemie, Ludwig-Maximilians-Universität München, Butenandtstrasse 11, 81377 Munich, Germany.
Bräuchle
Christoph
C
Frank
Irmgard
I