Two-pulse coherent control of electronic branching in Li2 photodissociation

Control over the product branching ratio in the photodissociation of Li-2 into Li(2s)+Li(2p) and Li(2s)+Li(3p) channels is explored computationally using the pump-pump coherent control scenario. Extensive control over the Li(3p)/Li(2p) branching ratio is demonstrated as the delay time between the two pulses is varied. The pulse width dependence is examined and better control is found to result from a narrow pump pulse which excites a superposition of only two levels, followed by a broad dissociation pulse. (C) 1998 American Institute of Physics. [S0021-9606(98)01707-3].