Topology of Classical Molecular Optimal Control Landscapes in Phase Space

Abstract

Optimal control of molecular dynamics is commonly expressed from a quantum mechanical perspective. However, in most contexts the preponderance of molecular dynamics studies utilize classical mechanical models. This paper treats laser-driven optimal control of molecular dynamics in a classical framework. We consider the objective of steering a molecular system from an initial point in phase space to a target point, subject to the dynamic constraint of Hamilton's equations. The classical control landscape corresponding to this objective is a functional of the control field, and the topology of the landscape is analyzed through its gradient and Hessian with respect to the control. Under specific assumptions on the regularity of the control fields, the classical control landscape is found to be free of traps that could hinder reaching the objective. The Hessian associated with an optimal control field is shown to have finite rank, indicating the presence of an inherent degree of robustness to control noise. Extensive numerical simulations are performed to illustrate the theoretical principles on a) a model diatomic molecule, b) two coupled Morse oscillators, and c) a chaotic system with a coupled quartic oscillator, confirming the absence of traps in the classical control landscape. We compare the classical formulation with the mathematically analogous state-to-state transition probability control landscape of N-level quantum systems. The absence of traps in both circumstances provides a broader basis to understand the growing number of successful control experiments with complex molecules, which can have dynamics that transcend the classical and quantum regimes.