飞秒光电子影像技术对氯丙烯分子的光电离/解离机理的研究

J4 ›› 2016, Vol. 33 ›› Issue (4): 385-391.

• 光谱 • 下一篇

飞秒光电子影像技术对氯丙烯分子的光电离/解离机理的研究

沈环¹,华林强²

1 华中农业大学理学院，湖北武汉 430070； 2 华中农业大学应用物理研究所，湖北武汉 430070；3 中国科学院武汉物理与数学研究所波谱与原子分子物理国家重点实验室，湖北武汉 430071

收稿日期:2016-03-01 修回日期:2016-03-18 出版日期:2016-07-28 发布日期:2016-07-28
通讯作者: 沈环（1982-），女，安徽人，博士，讲师，主要从事激光光谱的研究。 E-mail:shenhuan@mail.hzau.edu.cn

Study of the photoionization/photodissociation mechanisms of allyl chloride by femtosecond photoelectron imaging

Shen Huan, Hua Linqiang

Received:2016-03-01 Revised:2016-03-18 Published:2016-07-28 Online:2016-07-28

摘要/Abstract

摘要： 飞秒光电子影像技术结合飞行时间质谱对氯丙烯（C3H5Cl）在200 nm、400 nm、800 nm飞秒脉冲下的光电离/解离机理进行了研究。实验结果表明氯丙烯的光电离/解离机理与激光波长存在依赖关系。分析发现，在短波长200 nm时，母体分子C3H5Cl以双光子电离为主要通道，而其他的碎片离子则来源于C3H5Cl+的解离。当波长向长波方向变化时，例如800 nm时，C3H5Cl中间态的解离就开始占主导地位，碎片离子的信号也相应增强。此外，光电子能谱进一步证实了在400 nm和800 nm时存在来源于中性碎片的光电子，而这些中性碎片又是由C3H5Cl的中间态直接解离而产生的。这意味着，在长波400 nm和800 nm时，母体分子可能被激发到寿命较短的中间解离态，从而解离产生中性碎片，导致光解离过程在长波段占有重要角色。

关键词: 飞秒激光

Abstract: Femtosecond photoeletron imaging technique coupled with time-of-flight mass spectroscopy have been used to study the photoionization/photodissociation mechanisms of allyl chloride with 200 nm, 400 nm and 800 nm femtosecond laser pulses. The results show a wavelength dependent photoionization/photodissociation behavior. It is found that at short wavelength, i.e., 200 nm, two-photon ionization of the parent molecule is the dominant channel, while other fragment ions are generated by dissociation of C3H5Cl+. As we shift to longer wavelength, i.e., 800 nm, dissociation from intermediates states starts to play an important role. Furthermore, the spectra of photoelectron kinetic energy also confirm that photoelectron peaks resulted from the neutral fragments and they are generated from dissociation of the intermediate states of C3H5Cl. This implies that photodissociation starts to play a significant role at longer wavelength since neutral fragments are supposed to be generated on the intermediate states that reached by 400 nm or 800 nm photons.

Key words: femtosecond laser

中图分类号:

O433
O561

沈环华林强. 飞秒光电子影像技术对氯丙烯分子的光电离/解离机理的研究[J]. J4, 2016, 33(4): 385-391.

Shen Huan, Hua Linqiang. Study of the photoionization/photodissociation mechanisms of allyl chloride by femtosecond photoelectron imaging[J]. J4, 2016, 33(4): 385-391.

参考文献

[1]Buff D R, Parr C A, Jason J A.The photoionization of allyl chloride from onset to 20 eV[J].International Journal of Mass Spectrometry and ion physics, 1981, 40(1):31-34 [2] Traeger C J.A study of the allyl cation thermochemistry by photoionzation mass spectrometry[J].International Journal of Mass Spectrometry and ion processes, 1984, 58:259-271 [3]Castillejo M, Martin M, de Nalda R, Couris S, Koudoumas E.Dissociative ionization of halogenated ethylenes in intense femtosecond laser pulses[J].Chemical Physics Letters, 2002, 353(3):295-303 [4]Shen Huan, Hua Linqiang, Cao Zhenzhou, Bing Zhang.C-Br bond fission dynamics in ultraviolet photodissociation of propargyl bromide[J].Optics Communications, 2009, 282(3):287-291 [5] Shen Huan(沈环), Zhang Bing(张冰).Photoionization/photodissociation mechanism of allyl chloride with a femtosecond laser pulse[J].Chinese journal of quantum electronics (量子电子学报), 2016, 33:- [6]Fan H, Pratt S T.Determination of spin-orbit branching fractions in the photodissociation of halogenated hydrocarbons[J].Journal of Physical Chemistry A, 2007, 111(19):3901-3906 [7]Myers T L, Kitchen D C, Hu B, Butler L J.Investigating Conformation Dependence and Non-Adiabatic Effects in the Photodissociation of Allyl Chloride at 193 nm[J].Journal of chemical physics, 1996, 104(14):5446-5456 [8]Morton M L, Butler L J, Stephenson T A.C-Cl bond fission,HCl elimination,and secondary radical decomposition in the 193 nm photodissociation of allyl chloride[J].Journal of Chemical Physics, 2002, 116(7):2763-2775 [9]Park M S, Lee K W, Jung K H.Br(2pj) and Cl(2pj) Atom Formation Dynamics of Allyl Bromide and Chloride at 234 nm[J].Journal of Chemical Physics, 2001, 114(5):10368-10374 [10]Liu Y, Bulter L J.C-Cl Bond Fission Dynamics and Angular Momentum Recoupling in the 235 nm Photodissociation of Allyl Chloride[J].Journal of Chemical Physics, 2004, 121(22):11016-11022 [11]Fischer I, Schutler T, Deyerl H J, Elhanine M, Alcaraz C.Photoionization and dissociative photoionization of the allyl radical,C3H5[J].International Journal of Mass Spectrometry, 2007, 261(2-3):227-233 [12]Gilbert T, Pfab R, Fischer I, Chen P.The zero kinetic energy photoelectron spectrum of the propargyl radical,C3H3[J].Journal of Chemical Physics, 2000, 112(6):2575-2578 [13]Gilbert T, Fischer I, Chen P.Zero kinetic energy photoelectron spectra of the allyl radical,C3H5[J].Journal of Chemical Physics, 2000, 113(2):561-566 [14]Jin Bae Yong, Lee Mina, Kim Soo Myung.One-photon mass-analyzed threshold ionization spectroscopy of 2-chloropropene,2-C3H5CL and its vibrational assignment based on the density-functional theory calculations[J].Journal of Chemical Physics, 2005, 123(4):044306-1-044306-8 [15]吴成印, 龚旗煌.分子的飞秒强光电离[J].物理, 2006, 35(08):666-672 [16]Shen H, Chen JJ, Hua LQ, Zhang B.Photodissociation Dynamics of Allyl Chloride at 200 and 266 nm Studied by Time-resolved Mass Spectrometry and Photoelectron Imaging[J].Journal of Physical Chemistry A, 2014, 118(25):4444-4450 [17]Hua LQ, Shen H, Hu CJ, Zhang B.Photoelectron imaging of atomic chlorine and bromine following photolysis of CH2BrCl[J].Journal of Chemical Physics, 2008, 129(24):244308-1-244308-7 [18]Shen H, Hua LQ, Hu CJ, Zhang B.Photoelectron imaging of 8p Rydberg states of atomic iodine following methyl iodide A-band decomposition[J].Journal of Molecular Spectroscopy, 2009, 257(2):200-204 [19]Dribinski V, Ossadtchi A, Mandelshtam V A, Reisler H.Reconstruction of abel-transformable images: The Gaussian basis-set expansion abel transform method,Rev[J].Sci. Instrum., 2002, 73(7):2634-2642 [20]Gentry W R, Giese C F.Ten-microsecond pulsed molecular beam source and a fast ionization detector[J].Rev. Sci. Instrum., 1978, 49(5):595-602 [21] Worrell C W.The photoelectron and absorption spectra of allyl halides[J].Journal of Electron Spectroscopy and Related Phenomema, 1974, 3:359-367 [22]Roeterdink W G, Janssen M H M.Femtosecond velocity map imaging of dissociative ionization dynamics in CF3I[J].Physical Chemistry Chemical Physics, 2002, 4(4):601-612 [23]Torres I, Martinez R, Castano F.Electron-impact dissociative ionization of fluoromethanes CHF3 and CF4[J].Journal of physics B-atomic molecular and optical physics, 2002, 35(11):2423-2436 [24] Elshakre M.Dissociative ionization of methanol in medium intense femtosecond laser field using time-of-flight mass spectrometry[J].Radiation Physics and Chemistry, 2015, 112:49-55 [25]Farmanara P, Steinkellner O, Wick M T, Wittmann M, Korn G, Radloff W.Ultrafast internal conversion and photodissociation of molecules excited by femtosecond 155 nm laser pulses[J].Journal of Chemical Physics, 1999, 111(14):6264-6270

飞秒光电子影像技术对氯丙烯分子的光电离/解离机理的研究

Study of the photoionization/photodissociation mechanisms of allyl chloride by femtosecond photoelectron imaging

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