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Excited-State Processes in the Carotenoid Zeaxanthin after Excess Energy Excitation

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Department of Chemical Physics, Chemical Center, Lund University, Box 124, 22100 Lund, Sweden, and Department of Chemistry, The University of Western Ontario, London, Ontario, N6A 5B7, Canada
Cite this: J. Phys. Chem. A 2005, 109, 31, 6852–6859
Publication Date (Web):July 19, 2005
https://doi.org/10.1021/jp052227s
Copyright © 2005 American Chemical Society

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    Abstract

    Aiming for better understanding of the large complexity of excited-state processes in carotenoids, we have studied the excitation wavelength dependence of the relaxation dynamics in the carotenoid zeaxanthin. Excitation into the lowest vibrational band of the S2 state at 485 nm, into the 0−3 vibrational band of the S2 state at 400 nm, and into the 2Bu+ state at 266 nm resulted in different relaxation patterns. While excitation at 485 nm produces the known four-state scheme (S2 → hot S1 → S1 → S0), excess energy excitation led to additional dynamics occurring with a time constant of 2.8 ps (400 nm excitation) and 4.9 ps (266 nm excitation), respectively. This process is ascribed to a conformational relaxation of conformers generated by the excess energy excitation. The zeaxanthin S* state was observed regardless of the excitation wavelength, but its population increased after 400 and 266 nm excitation, suggesting that conformers generated by the excess energy excitation are important for directing the population toward the S* state. The S2−S1 internal conversion time was shortened from 135 to 70 fs when going from 485 to 400 nm excitation, as a result of competition between the S2−S1 internal conversion from the vibrationally hot S2 state and S2 vibrational relaxation. The S1 lifetime of zeaxanthin was within experimental error the same for all excitation wavelengths, yielding ∼9 ps. No long-lived species have been observed after excitation by femtosecond pulses regardless of the excitation wavelength, but excitation by nanosecond pulses at 266 nm generated both zeaxanthin triplet state and cation radical.

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     Lund University.

     The University of Western Ontario.

    *

     Corresponding author. Current address:  Institute of Physical Biology, University of South Bohemia, Zámek 136, CZ-337 33 Nové Hrady, Czech Republic. Telephone:  +420-386-361-259. Fax:  +420-386-361-219. E-mail:  [email protected].

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    Raw data showing transient absorption spectra at selected delay times for different excitation wavelengths. This material is available free of charge via the Internet at http://pubs.acs.org.

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