We present an implementation of optimal control theory for the first-principles nonadiabatic Ehrenfest molecular dynamics model, which describes a condensed matter system by considering classical point-particle nuclei, and quantum electrons, handled in our case with time-dependent density-functional theory. The scheme is demonstrated by optimizing the Coulomb explosion of small sodium clusters: the algorithm is set to find the optimal femtosecond laser pulses that disintegrate the clusters, for a given total duration, fluence, and cutoff frequency. We describe the numerical details and difficulties of the method.

• Received 27 June 2016
• Revised 11 November 2016

DOI:https://doi.org/10.1103/PhysRevA.94.063421