Optimal Control of Open Quantum Systems Applied to the Photochemistry of Surfaces

Abstract

A quantum system in a condensed phase undergoes strong dissipative processes. The last decades have seen the rise of experimental and theoretical approaches for gaining control over dissipative phenomena. From a theoretical viewpoint it is important to model such processes in a rigorous way. An efficient and accurate method to find control fields is optimal control theory (OCT). In this Letter, a control scheme relying on OCT with time-dependent targets is employed to minimize dissipation, modeled within the surrogate Hamiltonian approach, on adsorbate-surface systems.

Controlling open quantum systems: tools, achievements, and limitations

“…It will be concluded by briefly mentioning examples from other fields of current interest: Quantum optimal control for open systems has been employed in the context of quantum thermodynamics, in order to determine the optimal efficiency of a noisy heat engine [195]; biological chromophore complexes, in order to maximize exciton transfer [196,197]; molecules immersed in dissipative media, in order to maximally align them with respect to a laboratory axis [198][199][200]; molecular junctions, in order to control the current, shot noise and Fano factors [201]; as well as chemical reaction dynamics [202][203][204], including charge transfer in molecules [205], and surface photochemistry [206][207][208]. The numerous applications attest to the maturity as well as versatility of the quantum control toolbox [1].…”

Quantum dynamics of a vibronically coupled linear chain using a surrogate Hamiltonian approach

“…This sensitive behavior also indicates another possibility of controlling system dynamics by modulating the system-bath interaction, which is in line with the previous studies, 56,87 in addition to controlling it by an external field. 88 …”

Applications of the Cross-Entropy Method to Importance Sampling and Optimal Control of Diffusions

“…An example is the alignment of a molecule in solution in a laser field (modelled by u), where the cost measures the deviation of the molecule from a given reference configuration and the energy exterted by the laser [21]. Other applications of stochastic control problems of the form (2.16)-(2.17) involve molecular dynamics [20], photochemistry [1], material science [22], or mechanical engineering [26], to mention just a few.…”