Quantum optimal control theory for a molecule interacting with a plasmonic nanoparticle

Abstract

In this work, we extend the quantum optimal control theory of molecules subject to laser pulses to the case of molecules close to plasmonic metal nanoparticles. Explicitly including the nanoparticle dielectric response in the system Hamiltonian, the electronic dynamics for the molecule in the presence of the laser pulse is coupled with the polarization dynamics of the nanoparticle itself. A characteristic feature of a plasmonic environment is that it both amplifies the laser pulse field and introduces nonlocal time effects (a behavior of inherent interest for the quantum optimal control theory), impacting on the shape of the optimized light pulse. The optimal control theory is formulated using a genetic algorithm; numerical examples of a target molecule and nanoparticles of different shapes are presented and discussed.