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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Picosecond Time-Resolved Stokes and Anti-Stokes Raman Studies on the Photochromic Reactions of Diarylethene Derivatives
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Picosecond Time-Resolved Stokes and Anti-Stokes Raman Studies on the Photochromic Reactions of Diarylethene Derivatives

机译：二芳基乙烯衍生物的光致变色反应的皮秒时间分辨斯托克斯和反斯托克斯拉曼研究

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摘要

The cyclization and cycloreversion reactions of diarylethene derivatives have been studied with picosecond time-resolved Stokes and anti-Stokes Raman spectroscopies. The cyclization reaction of 1,2-bis(2,5-dimethyl-3-thienyl) perfluorocyclopentene (DMTF) is found to occur within 4 ps to produce the vibrationally excited closed forms in the ground electronic (S_0) state. The time constant of the vibrational relaxation toward a thermal equilibrium with solvent molecules is estimated to be about 10 ps. The cycloreversion reaction of 1,2-bis(3,4-dimethyl-5-phenyl-2-thienyl) perfluorocyclopentene (DMPTF) also generates the vibrationally excited open forms in the S_0 state within 4 ps, which decay on a picosecond time scale. The picosecond time-resolved anti-Stokes Raman spectra of DMPTF show two vibrational bands assignable to the C＝C stretching modes of the cyclopentene and thiophene moieties of the generated open forms. The Raman intensity arising from the cyclopentene moiety relative to that from the thiophene moiety becomes smaller with the delay time, indicating that part of the excess energy generated via the cycloreversion reaction is localized on the C＝C stretching mode of the cyclopentene moiety. This result suggests that the C＝C stretching mode of the cyclopentene moiety is one of the promoting or the accepting modes in the cycloreversion reaction.
机译：已经用皮秒时间分辨的斯托克斯和反斯托克斯拉曼光谱学研究了二芳基乙烯衍生物的环化和环还原反应。发现1,2-双（2,5-二甲基-3-噻吩基）全氟环戊烯（DMTF）的环化反应在4 ps内发生，从而以基态电子（S_0）的状态产生振动激发的闭合形式。朝着与溶剂分子的热平衡的振动弛豫的时间常数估计为约10 ps。 1,2-双（3,4-二甲基-5-苯基-2-噻吩基）全氟环戊烯（DMPTF）的环还原反应还会在4 ps内以S_0状态产生振动激发的开放形式，其在皮秒级的时间内衰减。 DMPTF的皮秒时间分辨反斯托克斯拉曼光谱显示出两个振动带，分别对应于所生成开放形式的环戊烯和噻吩部分的C ＝ C拉伸模式。环戊烯部分的拉曼强度相对于噻吩部分的拉曼强度随延迟时间而变小，表明通过环还原反应产生的过量能量的一部分位于环戊烯部分的C ＝ C拉伸模式上。该结果表明，环戊烯部分的C ＝ C拉伸模式是环还原反应中的促进或接受模式之一。

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