Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 10, Issue 20, Pages 6197-6201Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.9b02446
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Funding
- National Institute of Health [GM118332]
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Bacteriophytochromes are photoreceptors that regulate various physiological processes induced by photo-isomerization in a linear tetrapyrrole chromophore upon red/farred light absorption. Here, we investigate the photoinduced Pfr-state isomerization mechanism of a bathy bacteriophytochrome from Pseudomonas aeruginosa combining femtosecond-resolved fluorescence and absorption methods. We observed initial coherent oscillation motions in the first 1 ps with low-frequency modes below 60 cm(-1), then a bifurcation of the wavepacket with the distinct excited-state lifetimes in a few picoseconds, and finally chromophore-protein coupled ground-state conformational evolution on nanosecond time scales. Together with systematic mutational studies, we revealed the critical roles of hydrogen bonds in tuning the photoisomerization dynamics. These results provide a clear molecular picture of the Pfr-state photoisomerization, a mechanism likely applicable to the other phytochromes.
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