高压下香豆素7分子内电荷转移过程的实验与理论研究
详细信息 查看官网全文
- 英文论文题名：High Pressure controlled ultrafast intramolecular charge transfer process of Coumarin 7:An experimental and theoretical study
- 论文作者：李慧 ; 尹航 ; 刘晓春 ; 石英 ; 金明星 ; 丁大军
- 英文论文作者：Hui Li ; Hang Yin ; Xiaochun Liu ; Ying Shi ; Mingxing Jin ; Dajun Ding ; Institute of Atomic and Molecular Physics ; Jilin University
- 年：2016
- 作者机构：吉林大学原子与分子物理研究所;
- 论文关键词：飞秒瞬态吸收光谱 ; 高压技术 ; 含时密度泛函 ; 电荷转移过程
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第四十四分会：化学动力学
- 语种：中文
- 分类号：O641
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第四十四分会 ; 化学动力学
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：166k
- 原文格式：D
- 会议级别：全国
摘要
我们结合飞秒瞬态吸收光谱技术和高压技术,研究了压力对Coumarin 7(C7)分子的激发态超快过程的调控作用。动力学拟合结果表明:常压下(1atm),C7分子在第一电子激发态会经历两个弛豫过程,分别为39.95 ps的快过程与0.9 ns的相对较慢的过程;高压下(0.1 GPa~0.3 GPa),随着压力的提高,C7分子快过程增加到137 ps,慢过程增加至3.6 ns。在此基础上,采用TDDFT理论方法对该分子进行了计算,获得了垂直激发能、电荷分布、几何构型等相关信息。结合理论结果,我们把上述快过程归属为分子内的电荷转移过程(ICT)过程;通过时间尺度分析与发射峰位置的比较,我们将相对较慢的过程归属为ICT态荧光辐射过程。综上,压力能有效调控C7分子的激发态动力学过程,具体体现在迟滞ICT过程与延长ICT荧光寿命。
The effects of pressure on the ultrafast processes of excited states of Coumarin 7(C7) molecules by combining femtosecond transient absorption spectroscopy and high pressure technology have been investigated. The fitted results showed that, under 1atm, C7 undergoes a fast and a relatively slow relaxation process, 39,95 ps and 0.9ns respectively. Under high pressure(0.1 GPa~0.3 GPa), however, the fast process increased to 137 ps and slow process increased to 3.6 ns as pressure increased. Combining with the time-dependent density functional theory(TDDFT) method, we obtained the information of frontier molecular orbital and geometric structures. The fast process was attributed to the intramolecular charge transfer process(ICT), the fluorescence radiation process was responsible for the long-lived one. To sum up, pressure can regulate the dynamics process in excited state of C7 molecular. The specific expression is that the pressure can make the ICT slower and the life time of ICT fluorescence longer.
The effects of pressure on the ultrafast processes of excited states of Coumarin 7(C7) molecules by combining femtosecond transient absorption spectroscopy and high pressure technology have been investigated. The fitted results showed that, under 1atm, C7 undergoes a fast and a relatively slow relaxation process, 39,95 ps and 0.9ns respectively. Under high pressure(0.1 GPa~0.3 GPa), however, the fast process increased to 137 ps and slow process increased to 3.6 ns as pressure increased. Combining with the time-dependent density functional theory(TDDFT) method, we obtained the information of frontier molecular orbital and geometric structures. The fast process was attributed to the intramolecular charge transfer process(ICT), the fluorescence radiation process was responsible for the long-lived one. To sum up, pressure can regulate the dynamics process in excited state of C7 molecular. The specific expression is that the pressure can make the ICT slower and the life time of ICT fluorescence longer.
引文
[1]Satpati.A.K.;Kumbhakar.M.;Nath S.;Pal.H.,Photochem.Photobiol.2009,85:119.
© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号 地址：北京市海淀区学院路29号 邮编：100083 电话：办公室：(+86 10)66554848；文献借阅、咨询服务、科技查新：66554700 |