RAPID-FLOW RESONANCE RAMAN-SPECTROSCOPY OF BACTERIAL PHOTOSYNTHETIC REACTION CENTERS

被引:102
作者
SHREVE, AP
CHEREPY, NJ
FRANZEN, S
BOXER, SG
MATHIES, RA
机构
[1] UNIV CALIF BERKELEY,DEPT CHEM,BERKELEY,CA 94720
[2] STANFORD UNIV,DEPT CHEM,STANFORD,CA 94305
关键词
ELECTRON TRANSFER; HOLE-BURNING SPECTROSCOPY; EXCITED-STATE DYNAMICS; RESONANCE RAMAN INTENSITIES;
D O I
10.1073/pnas.88.24.11207
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Rapid-flow resonance Raman vibrational spectra of bacterial photosynthetic reaction centers from the R-26 mutant of Rhodobacter sphaeroides have been obtained by using excitation wavelengths (810-910 nm) resonant with the lowest energy, photochemically active electronic absorption. The technique of shifted excitation Raman difference spectroscopy is used to identify genuine Raman scattering bands in the presence of a large fluorescence background. The comparison of spectra obtained from untreated reaction centers and from reaction centers treated with the oxidant K3Fe(CN)6 demonstrates that resonance enhancement is obtained from the special pair. Relatively strong Raman scattering is observed for special pair vibrations with frequencies of 36, 94, 127, 202, 730, and 898 cm-1; other modes are observed at 71, 337, and 685 cm-1. Qualitative Raman excitation profiles are reported for some of the strong modes, and resonance enhancement is observed to occur throughout the near-IR absorption band of the special pair. These Raman data determine which vibrations are coupled to the optical absorption in the special pair and, thus, probe the nuclear motion that occurs after electronic excitation. Implications for the interpretation of previous hole-burning experiments and for the excited-state dynamics and photochemistry of reaction centers are discussed.
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页码:11207 / 11211
页数:5
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