Locally optimized control pulses with nonlinear interactions

: The local control theory has been extended to deal with nonlinear interactions, such as polarizability interaction, as well as a combination of dipole and polarizability interactions. We explain herein how to implement the developed pulse-design algorithm in a standard computer code that numerically integrates the Liouville equation and/or the Schrodinger equation without incurring additional high computational cost. Through a case study of the rotational dynamics control of crystalline orbital molecules, the effectiveness of the locally optimized control pulses is demonstrated by adopting four types of control objectives, namely, two types of state-selective excitation, alignment, and orientation control.