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Nonadiabatic dynamics of A-state photodissociation of ammonia: a four-dimensional wave packet study.

The nonadiabatic photodissociation dynamics of the A-state ammonia (NH(3)) was investigated using a four-dimensional wave packet model. The branching ratio between the excited NH(2)(A(2)A(1)) and ground NH(2)(X(2)B(1)) products was obtained as a function of energy for photodissociation mediated by several low-lying vibrational states in the ground electronic state of NH(3). The calculated results could not fully account for the experimental observations of strong mode specificity in nonadiabatic dynamics but agree qualitatively with a recent trajectory-based coupled-surface study using the same potential energy surfaces. Several possible sources of inaccuracy are discussed.