关键词: 氟利昂/
光解离/
飞行时间质谱/
离子速度成像
English Abstract
Multi-photon dissociation dynamics of Freon 1110 induced by femtosecond laser pulse
Liu Yu-Zhu1,2,Xiao Shao-Rong1,2,
Wang Jun-Feng1,
He Zhong-Fu1,
Qiu Xue-Jun3,
Gregor Knopp
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, Nanjing 210044, China;
3.College of Electronics and Information, South-Central University for Nationalities, Wuhan 430074, China;
4.Paul Scherrer Institute, Villigen 5232, Switzerland
Fund Project:Project supported by the National Natural Science Foundation of China (Grant Nos. 11304157, 11504175, 11404411) and Six Talent Peaks Project in Jiangsu Province (Grant No. 2015-JNHB-011).Received Date:03 February 2016
Accepted Date:15 March 2016
Published Online:05 June 2016
Abstract:The ozone layer which absorbs harmful solar UV radiation is an essential umbrella for human beings. However, a large number of exhausts of chlorine compounds including freon released by people in the atmosphere pose a great threat to the ozone layer. Freon dissociates into the product of chlorine radicals induced by UV sunlight radiation, which are found to be the main culprit for the destruction of atmospheric ozone. In this paper, time-of-flight mass spectrometry and velocity map imaging technique are coupled for investigating the multiphoton dissociation dynamics of Freon 1110 (C2Cl4, Tetrachloroethylene) induced by ultrafast short laser pulse on a femtosecond time scale at 800 nm. Fragments mass spectra of C2Cl4 are measured by time-of-flight mass spectrometry. Together with the parent ion C2Cl4+, two dominant fragment ions C2Cl3+ and C2Cl2+ are discovered in the multi-photon ionization and dissociation process in the experiment. By analyzing the above mass spectra, two corresponding photodissociation mechanisms are discussed and listed as follows: 1) C2Cl4+C2Cl3+ +Cl with single CCl bond breaking and direct production of Cl radical; 2) C2Cl4+C2Cl2+ +2Cl with double CCl bonds breaking and production of two Cl radicals. Also, ion images of these two observed fragment ions C2Cl3+ and C2Cl2+ are measured by velocity map imaging apparatus. The kinetic energy distributions of these two fragment ions are determined from the measured velocity map images. The kinetic energy distributions of both C2Cl3+ and C2Cl2+ can be well fitted by two Gaussion distributions. It indicates that both fragments C2Cl3+ and C2Cl2+ are from two production channels. The peak energies for each channel are fitted. More detailed photodissociation dynamics is obtained by analyzing the angular distribution of the generated fragment ions. The anisotropy parameter values are measured to be 0.46 (low energy channel) and 0.52 (high energy channel) for the fragment C2Cl3+, and 0.41 (low energy channel) and 0.66 (high energy channel) for the fragment C2Cl2+, respectively. The ratios between parallel transition and perpendicular transition are determined for all the observed channels for producing fragments C2Cl3+ and C2Cl2+. In addition, density functional theory calculations at a high-precision level are also performed on photodissociation dynamics for further analysis and discussion. The optimized geometries of ground state and ionic state of C2Cl4 are obtained and compared with density functional theory calculation at the level of B3LYP/6-311G++(d,p). The different structures of the ground and ionic states are given and discussed. The calculated information about ionic states of C2Cl4, including energy level and oscillator strength for the ionic excited states, is also given for analyzing the photodissociation dynamics of the C2Cl4 ions.
Keywords: freon/
photodissociation/
time-of-flight mass spectra/
velocity map imaging
