期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 4, 期 16, 页码 2605-2609出版社
AMER CHEMICAL SOC
DOI: 10.1021/jz401443q
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- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, United States Department of Energy [DOE DE-FG02-09ER16117]
- National Institutes of Health [GM068552]
The ultrafast mechanisms underlying the initial photoisomerization (P-r -> Lumi-R) in the forward reaction of the cyanobacterial photoreceptor Cph1 were explored with multipulse pump-dump-probe transient spectroscopy. A recently postulated multipopulation model was used to fit the transient pump-dump-probe and dump-induced depletion signals. We observed dump-induced depletion of the Lumi-R photoproduct, demonstrating that photoisomerization occurs via evolution on both the excited- and ground-state electronic surfaces. Excited-state equilibrium was not observed, as shown via the absence of a dump-induced excited-state Le Chatelier redistribution of excited-state populations. The importance of incorporating the inhomogeneous dynamics of Cph1 in interpreting measured transient data is discussed.
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