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作 者:吴义室[1,2] 钟声[3] 艾希成[2] 胡坤生[3] 张建平[2]
机构地区:[1]中国科学院化学研究所,北京分子科学国家实验室,分子动态与稳态结构化学国家重点实验室,北京100080 [2]中国人民大学理学院化学系,北京100872 [3]中国科学院生物物理研究所,北京100101
出 处:《高等学校化学学报》2008年第1期140-143,共4页Chemical Journal of Chinese Universities
基 金:国家自然科学基金(批准号:20433010,20673144)资助
摘 要:利用飞秒时间分辨吸收光谱方法研究了菌紫质(BR)光循环中视黄醛超快异构化反应过程.发展了结合全局拟合的奇异值分解(SVD)分析方法,建立了超快异构化反应动力学模型,解析了几个重要的中间态I460,J625和K590的物种相关差异光谱(SADS)和布居动力学,确定了光致异构化反应过程.同时明确了700nm附近存在的受激荧光来自于弗兰克-康登跃迁态(H中间态)的贡献,其衰减寿命为0.04ps.这些结果对深入认识H态在超快异构化反应过程中的作用具有参考价值.The ultrafast photoisomerization process of retinal in Bacteriorhodpsin's(BR) photocycle was investigated via femtosecond time-resolved absorption spectroscopy. Singular value decomposition(SVD) combined with model-based global fitting was employed to analyze the time-resolved spectra, and the related difference spectra(SADS) and the population dynamics of I460, J625 and K590 intermediates were derived on the basis of our proposed reaction scheme. The detailed photoisomerization pathways were discussed. Moreover, the SADS of Franck-Condon state (H intermediate) , radiative transition of which accounts for the stimulated emission around 700 nm, was also detected, and its time constant was 0. 04 ps. Our results prove the involvement of the H-intermediate in ultra:fast photoisomerization process of retinal in BR.
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