Optimal control with non-adiabatic Molecular Dynamics: application to the Coulomb explosion of Sodium clusters

TL;DR

This paper develops an optimal control method integrated with non-adiabatic Ehrenfest Molecular Dynamics and TDDFT to optimize laser-induced Coulomb explosions in sodium clusters, enabling precise control of ultrafast molecular disintegration.

Contribution

It introduces a novel implementation of optimal control theory within a first-principles non-adiabatic MD framework using TDDFT, applied to sodium cluster Coulomb explosions.

Findings

Successfully optimized femtosecond laser pulses for cluster disintegration

Demonstrated the feasibility of controlling Coulomb explosions with tailored pulses

Addressed numerical challenges in combining optimal control with non-adiabatic dynamics

Abstract

We present an implementation of optimal control theory for the first-principles non-adiabatic 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 pulse duration, fluence, and cut-off frequency. We describe the numerical details and difficulties of the methodology.