Ultrafast energy relaxation in bacteriorhodopsin studied by time-integrated fluorescence
文献信息
S. Schenkl, E. Portuondo, G. Zgrablić, M. Chergui, S. Haacke, N. Friedman, M. Sheves
Time-integrated fluorescence experiments on native bacteriorhodopsin and on its non-isomerizing form bR5.12 are reported. The experimental set-up was designed such as to observe emission exclusively from the excited state intermediate I-460. We obtain the first systematic investigation of the fluorescence spectra as a function of the excitation wavelength tuned throughout the entire absorption band of bR. An important finding is that the position of the fluorescence maximum does not show a systematic shift when the excitation wavelength is shortened. For excitation with high excess energy, we observe a broadening of the blue wing of the bR fluorescence, indicating incomplete vibrational energy relaxation on the time scale of the lifetime of I-460. Due to a much longer excited state lifetime, vibrational energy relaxation is more effective in bR5.12 and the fluorescence spectra are much less dependent on excitation wavelength. The results are placed in the general framework of thermalization between the retinal chromophore and the protein environment, and are compared with information obtained by femtosecond experiments.
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来源期刊
Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.










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