利用动态Stark效应开展对多原子分子非绝热光解过程的控制研究
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- 英文论文题名：Dynamic Stark Control of Nonadiabatic Photodissociation of Polyatomic Molecules
- 论文作者：唐颖 ; 凌丰姿 ; 蒿巧利 ; 宋辛黎 ; 胡春龙 ; 李帅 ; 邓绪兰 ; 张冰
- 英文论文作者：Ying Tang ; Fengzi Ling ; Qiaoli Hao ; Xinli Song ; Chunlong Hu ; Shuai Li ; Xulan Deng ; Bing Zhang ; State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics ; Wuhan Institute of Physics and Mathematics ; Chinese Academy of Sciences
- 年：2016
- 作者机构：中国科学院武汉物理与数学研究所;
- 论文关键词：动态Stark效应 ; 多原子分子 ; 光解 ; 飞秒激光
- 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：O644.1
- 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：147k
- 原文格式：D
- 会议级别：全国
摘要
飞秒激光具有能量超强、时间超快的优点;纳秒激光对产物探测具有高选择性的特点。我们将两者结合起来提出了飞秒-纳秒相结合的超快控制方法:泵浦光与控制光使用飞秒激光脉冲,通过改变泵浦-控制延迟时间,利用控制光产生的动态Stark效应改变分子激发态的演化途径,使演化过程及结果发生变化;探测光使用纳秒激光,通过共振增强多光子电离对演化产物进行态选择的精密探测。目前,我们已将该方法成功用于对简单三原子分子OCS以及复杂多原子分子碘苯的光解反应及产物通道的控制。在对OCS分子的光解控制研究中,我们观察到在泵浦-控制延迟时间为435fs处,解离产物S(~1D)的产率被明显抑制,同时解离产物S(~3P)的产率明显增强。此外,在对碘苯分子的相关研究中,我们发现红外飞秒控制激光在延迟时间为380和720fs处对解离产物基态I原子和激发态I*原子的产率具有明显的控制作用。研究表明,该方法对多原子分子非绝热光解过程的控制研究具有一定的普适性。
We present a simple experimental approach for controlling the outcome of photochemical reactions by combining the advantages of ultrafast femtosecond laser and high spectral resolution nanosencond laser. A precisely timed infrared femtosecond pulse is introduced to modify the reaction barriers via dynamic Stark effect during a chemical reaction. A nanosecond laser sensitively detects the products via resonance enhanced multiphoton ionization(REMPI) scheme. It has been successfully demonstrated for dynamic Stark control(DSC) of photodissociation of OCS, observing obvious suppress of S(~1D) and enhancement of S(~3P) yield at 435 fs. We further applied it to the photodissociation of iodobenzene, and observed the remarkable modifications of I* and I yields at 380 and 720 fs, which are perfect consistent with the time constants measured under field-free conditions. It strongly proved the universal applicability of our approach, and also the advantages in precisely clocking wavepacket movement and positioning the intersections of potential surfaces.
We present a simple experimental approach for controlling the outcome of photochemical reactions by combining the advantages of ultrafast femtosecond laser and high spectral resolution nanosencond laser. A precisely timed infrared femtosecond pulse is introduced to modify the reaction barriers via dynamic Stark effect during a chemical reaction. A nanosecond laser sensitively detects the products via resonance enhanced multiphoton ionization(REMPI) scheme. It has been successfully demonstrated for dynamic Stark control(DSC) of photodissociation of OCS, observing obvious suppress of S(~1D) and enhancement of S(~3P) yield at 435 fs. We further applied it to the photodissociation of iodobenzene, and observed the remarkable modifications of I* and I yields at 380 and 720 fs, which are perfect consistent with the time constants measured under field-free conditions. It strongly proved the universal applicability of our approach, and also the advantages in precisely clocking wavepacket movement and positioning the intersections of potential surfaces.
引文