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Combining High-Resolution and Ultrafast Measurements

Date Mo, 29.04.2013 - Mo, 29.04.2013
Time 16:45
Speaker Thomas Schultz, Max-Born Institut, Berlin
Location ETH Zurich, Hönggerberg Campus, HPF G-6
Program Combining High-Resolution and Ultrafast Measurements

Host: Ursula Keller, Ultrafast Laser Physics, IQE

Abstract:
Femtosecond time-resolved spectroscopy can observe photochemical processes in real time and map out the pathway from a reaction educt to a product. We combine gas-phase spectroscopy and high-level theory to resolve the mechanism of excited state processes in isolated molecules, predominantly building blocks of DNA [1]. In biological systems, biomolecules are embedded in a structured environment and interactions with the local environment affect molecular properties. Molecular clusters can reproduce crucial structural elements to facilitate the bottom-up characterization of biological photochemistry.

The information content of femtosecond experiments is limited by the Heisenberg uncertainty principle and is rarely sufficient for the spectroscopic assignment of complex molecular structure. Experiments on impure samples or samples containing unknown molecular structures (e.g., the clusters mentioned above) are therefore difficult. With a novel technique of correlated rotational alignment spectroscopy (CRASY, [2]), we correlate high-resolution rotational structure with femtosecond pump-probe data. This technique allows the isomer-selective investigation of electronic structure and dynamics, the simultaneous characterization of all species in an impure sample, and the assignment of fragmentation channels in molecules and clusters. Just as multidimensional methods in the field of NMR greatly expanded the utility of nuclear-spin spectroscopy, CRASY may pave the way for optical spectroscopy of complex samples.

[1] J. Phys. Chem. A, 113, 8195 (2009), http://pubs.acs.org/doi/abs/10.1021/jp903460b
[2] Science 1011, 333 (2011), http://www.sciencemag.org/cgi/rapidpdf/science.1204352?ijkey=kzUlrMvtgFUXQ&keytype=ref&siteid=sci
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