Hannover 2013 – scientific programme

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MO: Fachverband Molekülphysik

MO 14: Poster 1: Cluster, Femtosecond Spectroscopy

MO 14.7: Poster

Tuesday, March 19, 2013, 16:00–18:30, Empore Lichthof

Tensorial approach to anisotropy effects in third-order response spectroscopy with arbitrarily polarized laser pulses — •Sebastian Schott, Andreas Steinbacher, Patrick Nuernberger, and Tobias Brixner — Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg, Germany

We present a theoretical study in which an arbitrary tensor of rank four is used to describe the properties of a molecular sample. Since most studies focus on the investigation of isotropic samples, we apply as only assumption rotational averaging over randomly oriented molecules to the response function tensor. By also choosing the most general polarization state and an arbitrary propagation direction for each laser pulse the simulation of various experimental scenarios is possible.

We specifically calculate the magic angle condition for transient absorption spectroscopy and expand the well-known condition for linearly polarized pump and probe pulses to arbitrarily polarized pulses. Implications for experiments with polarization shaped laser pulses as e.g. used in quantum control are addressed. We further explore which role contributions due to anisotropy may play in coherent two-dimensional spectroscopy and how to circumvent them by variation of the polarization of the laser pulses.