Objectif
The Born-Oppenheimer approximation is one of the corner stones of classic photochemistry and photophysics. As important as its implications are for understanding the principles of light matter interactions, as critical is its break down in rationalizing how energy absorbed in the form of light is dissipated. In fact, the most efficient electronic relaxation processes such as internal conversion and intersystem crossing, fundamentally depend on nuclear degrees of freedom directly coupling the interacting electronic states, often through conical intersections. Although such processes are well studied theoretically, they have been difficult to address experimentally. Here, I propose to use ultra high time-resolution and sensitivity transient absorption spectroscopy to directly visualize the evolution of vibrational coherence in all available nuclear degrees of freedom during ultrafast internal conversion and intersystem crossing. Based on recent experimental results, I propose to investigate, for the first time, which nuclear degrees of freedom are involved in such decay processes and which act as spectator coordinates. I will study both well-established systems, such as carotenoids, but also novel and poorly understood ones, such as next generation solar energy devices based on singlet fission in thin films. In this way, I will be able to identify the crucial structure-function relationship underlying efficient photochemistry and photophysics.
Champ scientifique
Thème(s)
Appel à propositions
FP7-PEOPLE-2013-IEF
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Régime de financement
MC-IEF - Intra-European Fellowships (IEF)Coordinateur
OX1 2JD Oxford
Royaume-Uni