Multiphoton ionization and dissociation dynamics of Freon-113 induced by femtosecond laser pulse

Liu Yu-Zhu; Chen Yun-Yun; Zheng Gai-Ge; Jin Feng; Gregor Knopp

doi:10.7498/aps.65.053302

Abstract

The ozone layer which absorbs harmful solar UV radiation is an essential umbrella for human. However, a large number of exhausts of Freon released by human activity into the atmosphere pose a great threat to the ozone layer. The UV sunlight radiation induced Freon dissociation produces chlorine radicals, which are found to be the main culprit for destroying the atmospheric ozone. In this paper, multiphoton ionization and dissociation dynamics of Freon-113 (CF2ClCFCl2) induced by femtosecond laser pulse are studied by time-of-flight mass spectrometry coupled with velocity map imaging technique. Fragment mass spectra of Freon-113 are measured by time-of-flight mass spectrometry. No parent ions are discovered in the time-of-flight mass spectra, and all the detected ions are from the fragmentation induced by the laser pulse. Daughter ions CFCl2+, CF2Cl+, C2F3Cl2+ are found to be the three major fragmentation ions in the multi-photon ionization and dissociation. Several photodissociation channels are discussed and concluded by further analysis and calibration (via the ratio of mass to charge) of the measured time-of-flight mass spectra. Three main photodissociation mechanisms are found as follows: 1) C2F3Cl3+→C2F3Cl2++Cl with breaking C--Cl bond and directly producing the Cl radical; 2) C2F3Cl3+ →CFCl2++CF2Cl with breaking the C--C; 3) C2F3Cl3+ →CF2Cl++CFCl2 with breaking the C--C bond. Ion images of the three main fragments C2F3Cl2+, CFCl2+ and CF2Cl+ are measured by the velocity map imaging setup. The speed distributions of these three fragment ions are obtained from the velocity map imaging. The speed distribution of C2F3Cl2+ with breaking C--Cl bond can be fitted by two Gaussian distributions while the speed distributions of both CFCl2+ and CF2Cl+ with breaking the C--C bond can be well fitted by one Gaussian distribution. The different fittings reflect different production channels. The detailed photodissociation dynamics is obtained by analyzing the kinetic energy distribution and angular distribution of the fragment ions. Additionally, density functional theory calculations on high-precision level are also performed on photodissociation dynamics for further analysis and discussion. An in-depth understanding of dissociation dynamics of freon can provide theoretical reference and experimental basis for further controlling the dissociation process that can do destruction to the ozone layer.

Keywords:

Authors and contacts

1.
School of Physics and Opto-electronics Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, China;
2.
Jiangsu Collaborative Innovation Center on Atmospheric Environment and Equipment Technology (CICAEET), Nanjing 210044, China;
3.
C. Eugene Benett Department of Chemistry, West Virginia University, Morgantown WV 26506, USA;
4.
Paul Scherrer Institute, Villigen 5232, Switzerland

Corresponding author: Liu Yu-Zhu, yuzhu.liu@gmail.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 11304157) and the Six Talent Peaks Project in Jiangsu Province, China (Grant No. JNHB-011).

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Cited By

[1]	Sinreich R, Merten A, Molina L, Volkamer R 2013 Atmos. Meas. Tech. 6 1521
[2]	Liu J, Zou Y, Si F Q, Zhou H J, Dou K, Wang Y, Liu W Q 2015 Acta Phys. Sin. 64 164209 (in Chinese) [刘进, 邹莹, 司福祺, 周海金, 窦科, 王煜, 刘文清 2015 物理学报 64 164209]
[3]	Wu F C, Li A, Xie P H, Chen H, Ling L Y, Xu J, Mou F S, Zhang J, Shen J C, Liu J G, Liu W Q 2015 Acta Phys. Sin. 64 114211 (in Chinese) [吴丰成, 李昂, 谢品华, 陈浩, 凌六一, 徐晋, 牟福生, 张杰, 申进朝, 刘建国, 刘文清 2015 物理学报 64 114211]
[4]	Hendick F, Muller J F, Clemer K, Wang P, de Maziere M, Fayt C, Gielen C, Hermans C, Ma J Z, Pinardi G, Stavrakou T, Vlemmix T, van Roozendael M 2014 Atmos. Chem. Phys. 14 765
[5]	Shen J, Tan H, Wang J, Wang J, Lee S 2015 J. Internet Technol. 16 171
[6]	Chang J, Wang T, Zhang C, Ge Y, Tao Z 2013 Chin. Phys. Lett. 30 114206
[7]	Zheng J, Yang D, Ma Y, Chen M, Chang J, Li S, Wang M 2015 Atmosph. Environ. 119 167
[8]	Zhu B 2012 Trans. Atmosph. Sci. 35 513 (in Chinese) [朱彬 2012 大气科学学报 35 513]
[9]	Xiao S R, Shi L F, Huang B 2015 Laser & Optoelectronics Progress 52 071206 (in Chinese) [肖韶荣, 石刘峰, 黄彪 2015 激光与光电子学进展 52 071206]
[10]	Farman J C, Gardiner B G, Shanklin J D 1985 Nature 315 207
[11]	Molina M J, Rowland F S 1974 Nature 249 810
[12]	Wang D S, Kim M S, Choe J C, Ha T K 2001 J. Chem. Phys. 115 5454
[13]	Butler J H, Battle M, Bender M L, Montzka S A, Clarke A D, Saltzman E S, Sucher C M, Severinghaus J P, Elkins J W 1999 Nature 399 749
[14]	Chen H Y, Lien C Y, Lin W Y, Lee Y T, Lin J J 2009 Science 324 781
[15]	Hobe M 2007 Science 318 1878
[16]	Schiermeier Q 2007 Nature 449 382
[17]	Pope F D, Hansen J C, Bayes K D, Friedl R R, Sander S P 2007 J. Phys. Chem. A 111 4322
[18]	Hobe M, Salawitch R J, Canty T, Keller-Rudek H, Moortgat G K, Grooß J U, Mller R, Stroh F 2007 Atmos. Chem. Phys. 7 3055
[19]	Lokhman V N, Ryabov E A, Ogurok D D 2004 Tech. Phys. Lett. 30 345
[20]	Scully S W J, Mackie R A, Browning R, Dunn K F, Latimer C J 2004 Phys. Rev. A 70 042707
[21]	Liu Y Z, Xiao S R, Zhang C Y, Zheng G G, Chen Y Y 2012 Acta Phys. Sin. 61 193301 (in Chinese) [刘玉柱, 肖韶荣, 张成义, 郑改革, 陈云云 2012 物理学报 61 193301]
[22]	Nachbor M D, Giese C F, Gentry W R 1995 J. Phys. Chem. 99 15400
[23]	Hippler M, Quack M, Bumewes B 1997 Phys. Chem. 101 356
[24]	Wang S K, Tsai W C, Chou L C, Chen J, Wu Y H, He T M, Feng K S, Wen C R 2012 Surf. Sci. 606 1062
[25]	Harvey J, Tuckett R P, Bodi A 2012 J. Phys. Chem. A 116 9696
[26]	Crolin D, Piancastelli M N, Stolte W C, Lindle D W 2009 J. Chem. Phys. 131 244301
[27]	Chen L L, Tian S X, Xu Y F, Chu G B, Liu F Y, Shan X B, Sheng L S 2011 Int. J. Mass Spectrom. 305 20
[28]	Zuiderweg A, Kaiser J, Laube J C, Rockmann T, Holzinger R 2011 Atmos. Chem. Phys. Discuss. 11 33173
[29]	Eppink A T J B, Parker D H 1997 Rev. Sci. Instrum. 68 3477
[30]	Parker D H, Eppink A T J B 1997 J. Chem. Phys. 107 2357
[31]	Liu Y Z, Gerber T, Knopp G 2014 Acta Phys. Sin. 63 244208 (in Chinese) [刘玉柱, Gerber T, Knopp G 2014 物理学报 63 244208]
[32]	Frisch M J, Trucks G W, Schlegel H B et al. 2004 Gaussian 03, Revision D.01, Pittsburgh, PA Gaussian Inc
[33]	Watanabe K, Nakayama T, Mottl J 1962 J. Quant. Spectry. Radiative Transfer 2 369

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Vol. 65, Issue 5 - 2016-03-05

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