Optimally controlling the internal dynamics of a randomly oriented ensemble of molecules

The internal dynamics of a randomly oriented ensemble of molecules in the gas and condensed phases, was discussed. The degree to which all member of the ensemble might be controlled with respect to their internal motion by a single laser pulse, was addressed. The unperturbed Hamiltonian H₀ would depend on the internal molecular degrees of freedom. Numerical optimal control simulations showed that good quality full ensemble control could be achieved with reasonable constraints placed on the control fields.