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MO: Fachverband Molekülphysik
MO 3: SYED: Electronic 2D Spectroscopy from Small to Large Systems I
MO 3.1: Invited Talk
Monday, March 18, 2013, 11:00–11:30, E 415
Signatures of vibronic and vibrational coherences in electronic 2D-spectra of monomers and aggregates — Franz Milota1, Tomas Mancal2, Harald F. Kauffmann3,4, and •Jürgen Hauer1 — 1Photonics Institute, Vienna University of Technology, Gusshausstrasse 27, 1040 Vienna, Austria — 2Institute of Physics, Faculty of Mathematics and Physics, Charles University, KeKarlovu 5, Prague 121 16, Czech Republic — 3Faculty of Physics, University of Vienna, Strudlhofgasse 4, 1090 Vienna, Austria — 4Faculty of Physics, Vienna University of Technology, WiednerHauptstrasse 8-10, 1040 Vienna, Austria
From a quantum mechanical perspective, most molecular systems can be reduced to certain simple discrete level structures. Many properties of such multilevel systems do not depend on their exact nature, e.g. vibrational or electronic. While reflecting distinctly different physics, one common feature is the possibility to excite a coherent superposition of energy eigenstates, referred to as a wavepacket. As shown in numerous recent studies on natural light harvesting complexes, two-dimensional electronic spectroscopy (2D-ES) has a unique disposition for the study of such coherences due to its ability to resolve cross peaks. We identify and describe vibrational and vibronic modulations in electronic 2D-spectra in experimental studies on monomers and molecular J-aggregates. We discuss coherences in coupled molecular aggregates involving both electronic and nuclear degrees of freedom. We conclude that a general distinguishing criterion based on the experimental data alone cannot be devised.