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利用千兆瓦激光脉冲光解的金属有机团簇的质谱和电荷密度研究。

Mass spectrometric and charge density studies of organometallic clusters photoionized by gigawatt laser pulses.

机构信息

Chemistry Division, Bhabha Atomic Research Centre, Mumbai, 400 085, India.

出版信息

Mass Spectrom Rev. 2017 Mar;36(2):188-212. doi: 10.1002/mas.21469. Epub 2015 May 11.

Abstract

Clusters on exposure to nanosecond laser pulses of gigawatt intensity exhibit a variety of photo-chemical processes such as fragmentation, intracluster reaction, ionization, Coulomb explosion, etc. Present article summarizes the experimental results obtained in our laboratory utilizing time-of-flight mass spectrometer which deal with one such aspect of cluster photochemistry related to generation of multiply charged atomic ions upon excessive ionization of cluster constituents (Coulomb explosion) at low intensity laser field (∼10  W/cm ). To understand the mechanism of laser-cluster interaction, laser as well as cluster parameters were varied. Mass spectrometric studies were carried out at different laser wavelength as well as varying the nature of cluster constituents, backup pressure, nozzle diameter, etc. In addition, charge density measurements were also preformed to get information about the total number of ions generated upon laser-cluster interaction as a function of laser wavelength. In case of pure molecular clusters, the charge state of atomic ions as well as charge density was observed to enhance with increasing laser wavelength, signifying efficient coupling of the cluster medium with nanosecond laser pulse at longer wavelength. While in case of clusters doped with species having comparatively lower ionization energy, the efficiency of laser-cluster interaction was less, in contrast to studies carried out using femtosecond lasers. Results obtained in the present work have been rationalized on the basis of proposed three-stage cluster ionization mechanism, that is, multiphoton ionization ignited-inverse Bremsstrahlung heating and electron ionization. © 2015 Wiley Periodicals, Inc. Mass Spec Rev. 36:188-212, 2017.

摘要

纳秒激光脉冲的千兆瓦强度照射下的团簇会表现出多种光化学反应过程,如碎裂、团簇内反应、电离、库仑爆炸等。本文总结了我们实验室利用飞行时间质谱仪获得的实验结果,该质谱仪涉及与团簇光化学的一个方面有关,即在低强度激光场(约 10 W/cm)下,团簇成分过度电离(库仑爆炸)时产生多重价态原子离子。为了理解激光-团簇相互作用的机制,我们改变了激光和团簇的参数。在不同的激光波长以及改变团簇成分、背压、喷嘴直径等条件下进行了质谱研究。此外,还进行了电荷密度测量,以获取有关激光-团簇相互作用产生的总离子数随激光波长变化的信息。在纯分子团簇的情况下,原子离子的电荷态和电荷密度随着激光波长的增加而增加,这表明在较长波长下,团簇介质与纳秒激光脉冲的有效耦合。而在掺杂具有相对较低电离能的物种的团簇中,激光-团簇相互作用的效率较低,与使用飞秒激光进行的研究相反。本文工作的结果是基于提出的三阶段团簇电离机制进行合理化的,即多光子电离引发-逆韧致辐射加热和电子电离。©2015Wiley Periodicals,Inc. Mass Spec Rev. 36:188-212, 2017.

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