Simulation of coherent control of hydroxyl formed due to HCl adsorption on MgO(0Â 0Â 1)

A laser-excitation scheme is proposed to excite the stretching vibration of the hydroxyl ion formed at the surface of MgO(0 0 1) due to HCl adsorption as example for a photoinduced reaction in a molecule in contact with a crystal. A dissipation operator was constructed using a dissipation lifetime obtained from classical molecular dynamics simulations. The optimal control technique is used to design laser fields that maximise the yield of hydroxyl molecules in a vibrationally highly excited state. The main frequencies and chirp parameters of the predicted fields are extracted. Predicted pulses involve considerable contributions from double excitations. Taking dissipation into account, a lowering of the excitation yield is predicted but only by 50%, so that the proposed process remains effective. A radiative mechanism is proposed to desorb hydrogen from the vibrationally excited state of OH−.