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Crossed Beam Experiment on the validity of Born-Oppenheimer Approximation in Cl (2P) + D2 →DCl + D reaction
Xiao Chun-lei
State key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Abstract:
The reaction of chlorine atom Cl(2P) [Cl(2P3/2) and Cl*(2P1/2)] with D2 was investigated at collision energy from 4.5 to 6.5 kcal/mol with a high resolution crossed molecular beam apparatus using the technique of D-atom Rydberg tagging detection. The contribution from the spin-orbit excited reaction Cl*(2P1/2) +D2, which is prohibited by Born-Oppenheimer (BO) approximation, was observed. Collision-energy dependence of differential cross sections (DCSs) near the backward scattering direction was measured. The BO-forbidden reaction Cl*+ D2 was found to be dominant at lower collision energy. As collision energy increases, reactivity of BO-allowed reaction Cl+D2 increases much faster than that of BO-forbidden reaction and becomes dominant at higher collision energy. Our experiment indicates that the additional energy of spin-orbit excitation in Cl* facilitates BO-forbidden reaction to pass through the barrier at lower collision energy, while BO approximation is still valid at collision energy above barrier. This tendency of reactivity of Cl/ Cl* + D2 is similar to its isotopic reaction of Cl/Cl*+H2.
Key words:  spin-orbit state, Born-Oppenheimer approximation,crossed beam experiment
FundProject:
Crossed Beam Experiment on the validity of Born-Oppenheimer Approximation in Cl (2P) + D2 →DCl + D reaction
肖春雷
2) State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023, China
摘要:
The reaction of chlorine atom Cl(2P) [Cl(2P3/2) and Cl*(2P1/2)] with D2 was investigated at collision energy from 4.5 to 6.5 kcal/mol with a high resolution crossed molecular beam apparatus using the technique of D-atom Rydberg tagging detection. The contribution from the spin-orbit excited reaction Cl*(2P1/2) +D2, which is prohibited by Born-Oppenheimer (BO) approximation, was observed. Collision-energy dependence of differential cross sections (DCSs) near the backward scattering direction was measured. The BO-forbidden reaction Cl*+ D2 was found to be dominant at lower collision energy. As collision energy increases, reactivity of BO-allowed reaction Cl+D2 increases much faster than that of BO-forbidden reaction and becomes dominant at higher collision energy. Our experiment indicates that the additional energy of spin-orbit excitation in Cl* facilitates BO-forbidden reaction to pass through the barrier at lower collision energy, while BO approximation is still valid at collision energy above barrier. This tendency of reactivity of Cl/ Cl* + D2 is similar to its isotopic reaction of Cl/Cl*+H2.
关键词:  spin-orbit state, Born-Oppenheimer approximation,crossed beam experiment
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