The intact core antenna-reaction center (LH1-RC) core complex of thermophilic photosynthetic bacterium Thermochromatium (Tch.) tepidum is peculiar in its long-wavelength LH1-Q(y) absorption (915 nm). We have attempted comparative studies on the excitation dynamics of bacteriochlorophyll (BChl) and carotenoid (Car) between the intact core complex and the EDTA-treated one with the Q(y) absorption at 889 nm. For both spectral forms, the overall Car-to-BChl excitation energy transfer efficiency is determined to be approximately 20%, which is considerably lower than the reported values, e.g., approximately 35%, for other photosynthetic purple bacteria containing the same kind of Car (spirilloxanthin). The RC trapping time constants are found to be 50 approximately 60 ps (170 approximately 200 ps) for RC in open (closed) state irrespective to the spectral forms and the wavelengths of Q(y) excitation. Despite the low-energy LH1-Q(y) absorption, the RC trapping time are comparable to those reported for other photosynthetic bacteria with normal LH1-Q(y) absorption at 880 nm. Selective excitation to Car results in distinct differences in the Q(y)-bleaching dynamics between the two different spectral forms. This, together with the Car band-shift signals in response to Q(y) excitation, reveals the presence of two major groups of BChls in the LH1 of Tch. tepidum with a spectral heterogeneity of approximately 240 cm(-1), as well as an alteration in BChl-Car geometry in the 889-nm preparation with respect to the native one.
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http://dx.doi.org/10.1529/biophysj.108.133835 | DOI Listing |
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College of Chemistry, Jilin Province Research Center for Engineering and Technology of Spectral Analytical Instruments, Jilin University, Changchun 130012, China.
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Emory University School of Medicine, Atlanta, GA, USA.
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Department of Chemistry, Boston University, 590 Commonwealth Avenue, Boston, Massachusetts 02215, USA.
The computational spectroscopy of water has proven to be a powerful tool for probing the structure and dynamics of chemical systems and for providing atomistic insight into experimental vibrational spectroscopic results. However, such calculations have been limited for biochemical systems due to the lack of empirical vibrational frequency maps for the TIP3P water model, which is used in many popular biomolecular force fields. Here, we develop an empirical map for the TIP3P model and evaluate its efficacy for reproducing the experimental vibrational spectroscopy of water.
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School of Energy and Environment, City University of Hong Kong, Kowloon 999077, Hong Kong.
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Department of Chemistry, Institut - Courtois, Quebec Center for Advanced Materials (QCAM), and Regroupement Québécois sur les Matériaux de Pointe (RQMP), Université de Montréal, Montréal, Quebec H3C 3J7, Canada.
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