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

doi:10.3390/ijms11041888

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

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

Yasushi Koyama^1,* , Yoshinori Kakitani¹, Takeshi Miki¹, Rebecca Christiana¹ and Hiroyoshi Nagae²

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; in revised form: 16 March 2010 / Accepted: 21 March 2010 / Published: 26 April 2010

(This article belongs to the Section Biochemistry, Molecular Biology and Biophysics)

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Abstract: The unique excited-state properties of the overlapped (diabatic) optically-allowed 1B_u⁺ and the optically-forbidden 1B_u^- or 3A_g^- 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., ‘1B_u⁺-to-1B_u^- is allowed but 1B_u⁺-to-3A_g^- 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; 1B_u⁺; 3A_g^-; 1B_u^- and 2A_g^- states; diabatic (overlapped) vibronic levels

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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 1B_u⁺ and Optically-Forbidden 1B_u^- or 3A_g^- Vibronic Levels of Carotenoids: Possible Roles in the Light-Harvesting Function. Int. J. Mol. Sci. 2010, 11, 1888-1929.

AMA Style

Koyama Y, Kakitani Y, Miki T, Christiana R, Nagae H. Excited-State Dynamics of Overlapped Optically-Allowed 1B_u⁺ and Optically-Forbidden 1B_u^- or 3A_g^- Vibronic Levels of Carotenoids: Possible Roles in the Light-Harvesting Function. International Journal of Molecular Sciences. 2010; 11(4):1888-1929.

Chicago/Turabian Style

Koyama, Yasushi; Kakitani, Yoshinori; Miki, Takeshi; Christiana, Rebecca; Nagae, Hiroyoshi. 2010. "Excited-State Dynamics of Overlapped Optically-Allowed 1B_u⁺ and Optically-Forbidden 1B_u^- or 3A_g^- Vibronic Levels of Carotenoids: Possible Roles in the Light-Harvesting Function." Int. J. Mol. Sci. 11, no. 4: 1888-1929.

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