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

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.

arXiv commentAdded computations for longer pulse times in the Na2 and Na4 clusters

References in corpus (8)

• Control of quantum phenomena: Past, present, and future
• Laser-driven nonlinear cluster dynamics
• Structure and properties of small sodium clusters
• Controlling the Dynamics of Many-Electron Systems from First Principles: A Marriage of Optimal Control and Time-Dependent Density-Functional Theory
• Electrons as probes of dynamics in molecules and clusters : a contribution from Time Dependent Density Functional Theory
• Optimization Schemes for Selective Molecular Cleavage with Tailored Ultrashort Laser Pulses
• Optical response of small closed-shell sodium clusters
• Optimal control theory for quantum-classical systems: Ehrenfest Molecular Dynamics based on time-dependent density-functional theory