Abstract
A simple model is developed to describe lattice distortions following photon absorption by a molecular crystal. For excitation localised on the vibrational time scale, the classical motion of a one-dimensional lattice with realistic nearest neighbour interactions is examined. The lattice structure is initially unstable and relaxes via two competing mechanisms: one leads directly to a new symmetric equilibrium, the other produces an intermediate metastable asymmetric lattice structure. This second structure is a possible precursor to excimer formation and photochemical reaction. We present algebraic and numerical analyses to demonstrate that the phonon distribution before excitation determines the dominant relaxation mechanism. In this model, acoustic phonon modes near the zone boundary promote the excimer-like distortion.
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