Jang D J, el-Sayed M A
Department of Chemistry and Biochemistry, University of California, Los Angeles 90024.
Proc Natl Acad Sci U S A. 1989 Aug;86(15):5815-9. doi: 10.1073/pnas.86.15.5815.
The rates of the quenching and recovery of tryptophan fluorescence are determined in the microsecond-millisecond time scale during the photocycle of bacteriorhodopsin under different perturbations. The kinetics suggest the presence of two quenching processes, a rapid one (on the time scale of photocycle intermediate L550 formation or faster) and a slow one (slightly slower than the slow component of intermediate M412 formation). The slow quenching process is found to respond to different perturbations in the same manner as the slow component of M412 formation. It has the same activation energy, it is inhibited if metal cations are removed, it is negligible at pH values greater than the pKa of tyrosine, and its rate is slowed down when 75% of the lipids are removed. These results, together with the observed value of the quenching activation energy, suggest that the rates of the tryptophan fluorescence quenching, like those of tyrosinate and M412 formations during the cycle, are all determined by the rates of the protein conformation changes. The pH studies of the slow quenching process show that the maximum quenching probability occurs at neutral pH. A rapid decrease in quenching occurs at lower pH (approximately 3 and approximately 5.5) and higher pH (approximately 9). Two quenching mechanisms involving energy transfer to either retinal or to tyrosinate are considered. Protein conformation changes resulting from a change in the ionization state of amino acids of different pKa values could change the tryptophan-retinal (or tryptophan-tyrosinate) coupling and thus the quenching efficiency.
在不同扰动条件下,测定细菌视紫红质光循环过程中微秒至毫秒时间尺度内色氨酸荧光猝灭和恢复的速率。动力学研究表明存在两个猝灭过程,一个快速过程(在光循环中间体L550形成的时间尺度上或更快)和一个缓慢过程(略慢于中间体M412形成的慢成分)。发现缓慢猝灭过程对不同扰动的响应方式与M412形成的慢成分相同。它具有相同的活化能,如果去除金属阳离子则受到抑制,在pH值大于酪氨酸pKa时可忽略不计,并且当去除75%的脂质时其速率会减慢。这些结果与观察到的猝灭活化能值一起表明,色氨酸荧光猝灭的速率,与循环过程中酪氨酸盐和M412形成的速率一样,均由蛋白质构象变化的速率决定。对缓慢猝灭过程的pH研究表明,最大猝灭概率出现在中性pH值。在较低pH值(约为3和约为5.5)和较高pH值(约为9)时,猝灭迅速降低。考虑了两种涉及能量转移至视黄醛或酪氨酸盐的猝灭机制。不同pKa值的氨基酸电离状态变化导致的蛋白质构象变化可能会改变色氨酸 - 视黄醛(或色氨酸 - 酪氨酸盐)的耦合,从而改变猝灭效率。