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Content archived on 2024-06-18

Vibrational coherence as a quantum probe for ultrafast molecular dynamics

Objective

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.

Fields of science (EuroSciVoc)

Topic(s)

Call for proposal

FP7-PEOPLE-2013-IEF
See other projects for this call

Funding Scheme

MC-IEF - Intra-European Fellowships (IEF)

Coordinator

THE CHANCELLOR, MASTERS AND SCHOLARS OF THE UNIVERSITY OF OXFORD
EU contribution
€ 221 606,40
Address
WELLINGTON SQUARE UNIVERSITY OFFICES
OX1 2JD Oxford
United Kingdom
Region
South East (England) Berkshire, Buckinghamshire and Oxfordshire Oxfordshire
Activity type
Higher or Secondary Education Establishments
Links
Total cost
No data