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Wave packet movements near the conical intersection between two excited potential surfaces may create observable
S Sorgues1, J M Mestdagh, J P Visticot
1Laboratoire Francis Perrin, CEA/DRECAM/Service des Photons, Atomes et Molécules, C.E.N. Saclay, F-91191 Gif-sur-Yvette Cedex, France.
Physical Review Letters
|October 4, 2003
Summary
Femtosecond pump-probe experiments reveal that tetrakis(dimethylamino)ethylene
Area of Science:
- Physical Chemistry
- Molecular Dynamics
- Spectroscopy
Background:
- Tetrakis(dimethylamino)ethylene (TMAE) is a molecule with a unique electronic structure.
- Understanding its excited-state dynamics is crucial for applications in photochemistry.
Purpose of the Study:
- To investigate the ultrafast molecular dynamics of TMAE following pi-pi(*) excitation.
- To elucidate the reaction pathway and identify key vibrational modes involved.
Main Methods:
- Femtosecond pump-probe spectroscopy was employed.
- Time-resolved measurements were analyzed to track molecular evolution.
Main Results:
- Excitation of the CC double bond leads to movement on a single adiabatic potential surface.
- Deformation along multiple coordinates and passage near a conical intersection were observed.
- Surprisingly, the umbrella mode of amino groups was excited, inducing oscillations.
Conclusions:
- The study reveals a novel excited-state pathway in TMAE.
- The excitation of the umbrella mode presents a new avenue for controlling molecular dynamics.