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    Spectroscopic and Dynamic Properties of the Peridinin Lowest Singlet Excited States†
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    Department of Chemical Physics, Lund University, Box 124, S-22100 Lund, Sweden, and Department of Biological Sciences, Macquarie University, NSW, Australia 2109
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    The Journal of Physical Chemistry A

    Cite this: J. Phys. Chem. A 2001, 105, 45, 10296–10306
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    https://doi.org/10.1021/jp010022n
    Published June 5, 2001
    Copyright © 2001 American Chemical Society
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    Abstract

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    Spectroscopic properties as well as excited state dynamics of the carotenoid peridinin in several solvents of different polarities were investigated by time-resolved fluorescence and transient absorption techniques. A strong dependence of the peridinin lowest excited states dynamics on solvent polarity was observed after excitation into the strongly allowed S2 state. Peridinin relaxes to the ground state within 10 ps in the strongly polar solvent methanol, while in the nonpolar solvent n-hexane a 160 ps lifetime was observed, thus confirming the previous observations revealed by transient absorption spectroscopy in the visible region (Bautista, J. A.; et al. J. Phys. Chem. B1999, 103, 8751). In addition, the solvent dependence in the near-IR region is demonstrated by a strong negative feature in the transient absorption spectrum of peridinin in methanol, which is not present in n-hexane. This band, characterized by a 1 ps rise time, is ascribed to stimulated emission from an intramolecular charge-transfer (ICT) state. Time-resolved fluorescence data support assignment of this band to the emissive singlet state, whose dynamic characteristics depend strongly on the dielectric strength of the medium. On the basis of all our time-resolved measurements combined with simulations of the observed kinetics, we propose the following model:  the initially populated S2 state decays to the S1 state within less than 100 fs for both solvents. Then, the population is transferred from the S1 state to the S0 and ICT states. The S1 → ICT transfer is controlled by a solvent polarity dependent barrier. In n-hexane the barrier is high enough to prevent the S1 → ICT transfer and only S1 → S0 relaxation characterized by a time constant of 160 ps is observed. An increase of solvent polarity leads to a significant decrease of the barrier, enabling a direct quenching of the S1 state by means of the S1 → ICT transfer, which is characterized by a time constant of 148 ps for tetrahydrofuran, 81 ps for 2-propanol, and 11 ps for the most polar solvent methanol. The ICT state is then rapidly depopulated to the ground state. This relaxation also exhibits solvent dependence, having a time constant of 1 ps in methanol, 2.5 ps in 2-propanol, and 3.5 ps in tetrahydrofuran.

    Copyright © 2001 American Chemical Society

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    †

     This work was presented at the PP2000 in Costa do Estoril, Portugal, honoring Professor Ralph Becker's contributions.

    ‡

     Lund University.

    §

     Macquarie University.

    *

     Corresponding author. E-mail:  [email protected]. Fax:  +46−46−2224119.

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    Cite this: J. Phys. Chem. A 2001, 105, 45, 10296–10306
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