Heidelberg 2015 – wissenschaftliches Programm

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MO: Fachverband Molekülphysik

MO 2: Quantum Control

MO 2.4: Vortrag

Montag, 23. März 2015, 12:30–12:45, PH/HS1

Quantum optimal control of a carbonyl reaction in an explicit solvent cage using tailored laser pulses — •Daniel Keefer, Sebastian Thallmair, and Regina de Vivie-Riedle — Department Chemie, LMU München

Influencing the outcome of a chemical reaction is an everyday struggle for chemists. A powerful tool to directly interact with a molecular process is to address its quantum nature, which is achieved by using specifically tailored laser pulses. Theoretically, the tailoring is accomplished using optimal control theory (OCT).

Investigating a chemical process which takes place in solution, a proper theoretical treatment becomes more challenging. Electrostatic and dynamic solvent effects influence the quantum dynamical behaviour during the ultrafast reaction. We present a way to account for these effects in OCT optimizations. Therefore, a QD/MD approach combining quantum dynamics (QD) and classical molecular dynamics (MD) is used. The motion of the explicitly included solvent molecules around the reactant is described by MD. Different solvent cage arrangements are extracted from the MD trajectories. These arrangements alter the potential energy surface for the chemical reaction in different ways. The various solvent cage configurations are included in the Hamiltonian to approximate the thermodynamical distribution of the solvent molecules in the solution. Optimizations are conducted to obtain laser pulses for optimal control of an ensemble of solvent arrangements. Significant effects on the shape of the laser pulses controlling the reaction are observed.