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

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,* , 1, 1, 1 and 2
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 Bioinorganic Chemistry)

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
This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

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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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