Institut für Chemie, Humboldt-Universität zu Berlin, 12489 Berlin, Germany.
J Phys Chem A. 2010 Feb 11;114(5):2179-88. doi: 10.1021/jp904132f.
Donor-acceptor substituted styrenes and phenylbutadienes with substituents varying in donor and acceptor strength and as reconstituted chromophore-protein complexes were investigated as model compounds for the protonated Schiff base chromophore in bacteriorhodopsin (bR) both experimentally and theoretically. Charge distribution, donor-acceptor strength, and the shift of the absorption energy are correlated. The effect of the external electrostatic field was tested with a compound carrying an additional nonconjugated charge. The concept of overpolarization by the external charge, that is, the reversal of the relative importance of the two main resonance structures in S(0) and S(1), has been emphasized and related to a simple qualitative 2 x 2 interaction model. The variable donor approach is a new way for a better understanding of the Opsin shift in Bacteriorhodopsin.
供体-受体取代的苯乙烯和苯基丁二烯,取代基在供体和受体强度上有所不同,并作为重构的生色团-蛋白质复合物,被研究为菌紫质(bR)中质子化的席夫碱生色团的模型化合物,无论是在实验上还是理论上。电荷分布、供体-受体强度和吸收能量的位移都相关。用携带额外非共轭电荷的化合物测试了外部静电场的影响。通过外部电荷的过极化概念,即 S(0)和 S(1)中两个主要共振结构的相对重要性的反转,已经被强调,并与一个简单的定性 2 x 2 相互作用模型相关。可变供体方法是更好地理解菌紫质中 Opsin 位移的一种新方法。