Re-evaluation of rhodopsin's relaxation kinetics determined from femtosecond stimulated Raman lineshapes.
Re-evaluation of rhodopsin's relaxation kinetics determined from femtosecond stimulated Raman lineshapes.
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DOI：
10.1021/jp2028164
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发表时间：
2011-07-28
影响因子：
3.3
通讯作者：
McCamant, David W.
中科院分区：
文献类型：
--
作者：
McCamant, David W.
在飞秒受激拉曼光谱(FSRs)实验中，当被探测的振动在其自由感应衰减过程中发生显著的频率漂移时，我们提出了一种理论处理方法。该理论被应用于模拟先前在视紫红质中观察到的FSR线形(Kukura等，Science，2005,310,1006)先前确定的形成视紫红质反光产物的驰豫时间是使用关于观察到的频移的时间依赖的错误方程来计算的。在这里，通过计算在自由振动感应衰变过程中发生的校正频率扫描来重新分析数据。结果表明，计算的频移和原始工作的一般结论是正确的，但C10、C11和C12氢离面振动的相干振动频率漂移的时间常数是140f，而不是以前报道的325f的时间常数。这个时间常数为顺式到反式异构化过程的动力学模型提供了一个重要的约束条件。
We present a theoretical treatment of the vibrational lineshape generated in a femtosecond stimulated Raman spectroscopy (FSRS) experiment under conditions in which the probed vibration undergoes a significant frequency shift during its free induction decay. This theory is applied to simulate the FSRS lineshapes previously observed in rhodopsin.(Kukura et al., Science, 2005, 310, 1006) The previously determined relaxation times for formation of the trans-photoproduct of rhodopsin were calculated using an incorrect equation for the time-dependence of the observed frequency shifts. Here the data is reanalyzed by calculation of the corrected frequency sweep occurring during the vibrational free induction decay. It is shown that the calculated frequency shifts and general conclusions of the original work are sound, but that the coherent vibrational frequency shifts of the C10, C11, and C12 hydrogen out-of-plane vibrations occur with a 140-fs time constant rather than the previously reported 325-fs time constant. This time-constant provides an important constraint for models of the dynamics of the cis to trans isomerization process.
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影响因子：
56.9
作者：
Kukura, P;McCamant, DW;Mathies, RA
通讯作者：
Mathies, RA
影响因子：
64.8
作者：
Polli, Dario;Altoe, Piero;Cerullo, Giulio
通讯作者：
Cerullo, Giulio
影响因子：
15
作者：
Tomasello, Gaia;Olaso-Gonzalez, Gloria;Garavelli, Marco
通讯作者：
Garavelli, Marco
影响因子：
56.9
作者：
WANG, Q;SCHOENLEIN, RW;SHANK, CV
通讯作者：
SHANK, CV
影响因子：
3.3
作者：
Weingart, Oliver;Schapiro, Igor;Buss, Volker
通讯作者：
Buss, Volker