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The dependence of the ultrafast relaxation kinetics of the and states in -carotene homologs and lycopene on conjugation length studied by femtosecond time-resolved absorption and Kerr-gate fluorescence spectroscopies
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10.1063/1.3147008
/content/aip/journal/jcp/130/21/10.1063/1.3147008
http://aip.metastore.ingenta.com/content/aip/journal/jcp/130/21/10.1063/1.3147008

Figures

Image of FIG. 1.
FIG. 1.

Stationary absorption (broken lines) and time-resolved fluorescence spectra at a delay time of 0.1 ps (solid lines) of the -carotene homologues and lycopene. Insets show the chemical structures of the carotenoids. The solid arrows indicate the excitation energies used in each sample. The broken arrows indicate the photon energies used for kinetics traces.

Image of FIG. 2.
FIG. 2.

Spectra of the photoinduced absorbance change in the carotenoids at a delay time of 0.1 ps (solid lines), 1.0 ps (broken lines), and 6.0 ps (dashed and dotted lines). Arrows show the energy used for analysis of the temporal responses.

Image of FIG. 3.
FIG. 3.

Time courses of the transient absorption signals of the carotenoids. The probe photon energies are indicated by arrows in Fig. 2. The solid lines are the best fit curves using the exponential function described in the text.

Image of FIG. 4.
FIG. 4.

(a) The relaxation rates plotted as a function of the energy gap. The broken line is the best fit to the energy gap law using Eq. (1). (b) The relaxation rates plotted as a function of the energy gap. The dashed-dotted line was calculated using Eqs. (2) and (3). 

Image of FIG. 5.
FIG. 5.

A schematic representation of the two potential surfaces where (a) and (b). , , , and in this figure, are the relative energy gap, the displacement of the potential energy minima, the activation energy and the reorganization energy between the electronic states of and , respectively.

Image of FIG. 6.
FIG. 6.

Schematics of the possible relaxation pathways including the relative positions of the , , , and potential energy curves along the normal coordinates of the stretching mode in order of the number of conjugated double bonds .

Image of FIG. 7.
FIG. 7.

The population dynamics of (open circles) and (closed circles) measured by time-resolved fluorescence and absorption, respectively.

Image of FIG. 8.
FIG. 8.

Modeling of the kinetics of the carotenoids excited singlet states. The solid lines, broken lines, and dashed-dotted lines represent , , and , respectively. (a) Temporal profiles calculated using Eq. (4) with time constants of , , and and (b) temporal profiles calculated using Eq. (5) with time constants of , , and .

Tables

Generic image for table
Table I.

The time constants of the decay determined by time-resolved fluorescence spectroscopy and those of the rise and decay determined by time-resolved absorption spectroscopy.

Generic image for table
Table II.

The calculated energy gap between and and the activation energy of the relaxation to .

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/content/aip/journal/jcp/130/21/10.1063/1.3147008
2009-06-03
2014-04-18
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: The dependence of the ultrafast relaxation kinetics of the S2 and S1 states in β-carotene homologs and lycopene on conjugation length studied by femtosecond time-resolved absorption and Kerr-gate fluorescence spectroscopies
http://aip.metastore.ingenta.com/content/aip/journal/jcp/130/21/10.1063/1.3147008
10.1063/1.3147008
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