Resumen: 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. Idioma: Inglés DOI: 10.1103/PhysRevA.94.063421 Año: 2016 Publicado en: Physical review. A, Atomic, molecular, and optical physics 94, 6 (2016), 063421 [10 PP.] ISSN: 1050-2947 Factor impacto SCIMAGO: 1.482 - Atomic and Molecular Physics, and Optics (Q1)