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Vibrational motions in optically excited polyacetylene and polydiacetylene oligomers are calculated using potential surfaces obtained from the collective electronic oscillators (CEO) technique. The role of the effective conjugation coordinate (ECC) in the relaxation processes following an impulsive vertical excitation from the ground state is demonstrated. Real-space analysis of the electronic transition density matrices shows the charge and bond-order redistribution taking place upon photoexcitation

Excited-State Molecular Dynamics Simulations of Conjugated Oligomers Using the Electronic Density Matrix