Hannover 2016 – wissenschaftliches Programm
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MO: Fachverband Molekülphysik
MO 6: Posters 1: Novelties in Molecular Physics: Femtosecond Spectroscopy
MO 6.1: Poster
Montag, 29. Februar 2016, 16:30–19:00, Empore Lichthof
Vibrational and vibronic coherences in the two dimensional spectroscopy of coupled electron-nuclear motion — •Julian Albert1, Mirjam Falge1, Sandra Gomez2, Ignacio Sola2, Heiko Hildenbrand1, and Volker Engel1 — 1Universität Würzburg, Institut für Physikalische und Theoretische Chemie, Emil-Fischer-Str. 42, Campus Nord, 97074 Würzburg, Germany — 2Departamento de Quimica Fisica, Universidad Complutense, 28040 Madrid, Spain
We theoretically investigate the photon-echo spectroscopy of coupled electron-nuclear quantum dynamics [1]. Two situations are treated. In the first case, the Born-Oppenheimer (adiabatic) approximation holds. It is then possible to interprete the two-dimensional (2D) spectra in terms of vibrational motion taking place in different electronic states. In particular, pure vibrational coherences which are related to oscillations in the time-dependent third-order polarization can be identified. This concept fails in the second case, where strong non-adiabatic coupling leads to the breakdown of the Born-Oppenheimer-approximation. Then the 2D-spectra reveal a complicated vibronic structure and vibrational coherences cannot be disentangled from the electronic motion.
[1] J. Albert, M. Falge, S. Gomez, I. R. Sola, H. Hildenbrand, V. Engel,J. Chem. Phys. 143, 041102 (2015)