Optimal control theory for quantum-classical systems: Ehrenfest Molecular Dynamics based on time-dependent density-functional theory

Abstract

We derive the fundamental equations of an optimal control theory for systems containing both quantum electrons and classical ions. The system is modeled with Ehrenfest dynamics, a non-adiabatic variant of molecular dynamics. The general formulation, that needs the fully correlated many-electron wave function, can be simplified by making use of time-dependent density-functional theory. In this case, the optimal control equations require some modifications that we will provide. The abstract general formulation is complemented with the simple example of the H${}_2^{+}$ molecule in the presence of a laser field.

References in corpus (2)

• Optimal Control of Quantum Rings by Terahertz Laser Pulses
• Optical Control of Entangled States in Quantum Wells

Cited by in corpus (7)

• Atoms and Molecules in Cavities: From Weak to Strong Coupling in QED Chemistry
• Real-space grids and the Octopus code as tools for the development of new simulation approaches for electronic systems
• Self-interaction effects on charge-transfer collisions
• Tailored pump-probe transient spectroscopy with time-dependent density-functional theory: controlling absorption spectra
• Optimal control theory for quantum electrodynamics: an initial state problem
• Hamiltonian formulation and symplectic split-operator schemes for time-dependent density-functional-theory equations of electron dynamics in molecules
• Optimal control with non-adiabatic Molecular Dynamics: application to the Coulomb explosion of Sodium clusters