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Int. J. Mol. Sci. 2010, 11(4), 1888-1929; doi:10.3390/ijms11041888

Excited-State Dynamics of Overlapped Optically-Allowed 1Bu+ and Optically-Forbidden 1Bu- or 3Ag- Vibronic Levels of Carotenoids: Possible Roles in the Light-Harvesting Function

1
Faculty of Science and Technology, Kwansei Gakuin University, Sanda, Hyogo 669-1337, Japan
2
Kobe City University of Foreign Studies, Gakuen Higashimachi, Nishi-ku, Kobe 651-2187, Japan
*
Author to whom correspondence should be addressed.
Received: 20 February 2010 / Revised: 16 March 2010 / Accepted: 21 March 2010 / Published: 26 April 2010
(This article belongs to the Section Biochemistry, Molecular Biology and Biophysics)

Abstract

The unique excited-state properties of the overlapped (diabatic) optically-allowed 1Bu+ and the optically-forbidden 1Bu- or 3Ag- vibronic levels close to conical intersection (‘the diabatic pair’) are summarized: Pump-probe spectroscopy after selective excitation with ~100 fs pulses of all-trans carotenoids (Cars) in nonpolar solvent identified a symmetry selection rule in the diabatic electronic mixing and diabatic internal conversion, i.e., ‘1Bu+-to-1Bu- is allowed but 1Bu+-to-3Ag- is forbidden’. On the other hand, pump-probe spectroscopy after coherent excitation with ~30 fs of all-trans Cars in THF generated stimulated emission with quantum beat, consisting of the long-lived coherent diabatic cross term and a pair of short-lived incoherent terms.
Keywords: carotenoids; 1Bu+; 3Ag-; 1Bu- and 2Ag- states; diabatic (overlapped) vibronic levels carotenoids; 1Bu+; 3Ag-; 1Bu- and 2Ag- states; diabatic (overlapped) vibronic levels
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This is an open access article distributed under the Creative Commons Attribution License (CC BY 3.0).

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MDPI and ACS Style

Koyama, Y.; Kakitani, Y.; Miki, T.; Christiana, R.; Nagae, H. Excited-State Dynamics of Overlapped Optically-Allowed 1Bu+ and Optically-Forbidden 1Bu- or 3Ag- Vibronic Levels of Carotenoids: Possible Roles in the Light-Harvesting Function. Int. J. Mol. Sci. 2010, 11, 1888-1929.

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