Berlin 2014 – scientific programme
Parts | Days | Selection | Search | Updates | Downloads | Help
MO: Fachverband Molekülphysik
MO 9: Theory 2: Molecular Dynamics & Quantum Chemistry
MO 9.2: Talk
Tuesday, March 18, 2014, 14:15–14:30, BEBEL SR144
Nonlinear Absorption Dynamics Using Field-Induced Surface Hopping: Zinc Porphyrin in Water — •Merle I. S. Röhr1, Jens Petersen2, and Roland Mitric2 — 1Fachbereich Physik, Freie Universität Berlin, Arnimallee 14, 14195 Berlin — 2Institut für Physikalische und Theoretische Chemie, Julius-Maximilians-Universität Würzburg, Am Hubland, 97074 Würzburg
The field-induced surface hopping (FISH) method [1] for the simulation and control of light-induced nonadiabatic dynamics in complex systems will be introduced and applied to the investigation of nonlinear absorption processes [2]. For this purpose, a systematic comparison of the FISH approach with exact quantum dynamics simulations on a multistate model system is provided, and it is demonstrated that FISH allows for accurate simulations of nonlinear excitation processes including multiphoton electronic transitions. The applicability of our method to complex molecular systems is illustrated by simulating the linear and nonlinear laser-driven dynamics in zinc (Zn) porphyrin in the gas phase and in water. To this end, the FISH approach is connected with the quantum mechanical-molecular mechanical approach (QM/MM) [2] which is generally applicable to large classes of complex systems. Our findings that multiphotonic processes increase the population of higher excited states of Zn porphyrin in the nonlinear regime provides a means for manipulating excited-state properties, such as transient absorption dynamics and electronic relaxation.
1. R. Mitric et al., Phys. Rev. A 79, 053416 (2009).
2. M. I. S. Röhr et al., ChemPhysChem 14, 1377 (2013).