Coherent radiative control of unimolecular reactions: Selective bond breaking with picosecond pulses

We show that the principle of coherent control of chemical reactions can be implemented, in a two pulse sequence, to control the relative yield of reaction products in unimolecular dissociation. Experimental control parameters in this implementation are seen to be the intensity of the pulses and the delay time between them, with required delay times in the experimentally accessible picosecond range. As an example, application is made to control the production of D + H₂ vs HD + H in the dissociation of a model collinear molecule with DH₂ masses. In addition, plots of the evolving superposition state are presented in order to emphasize relevant characteristics of excitation with slow pulses.