We report a newly constructed laser ablation crossed molecular beam apparatus, equipped with time-sliced velocity map imaging technique, to study state-to-state metal atom reaction dynamics. Supersonic metal atomic be...We report a newly constructed laser ablation crossed molecular beam apparatus, equipped with time-sliced velocity map imaging technique, to study state-to-state metal atom reaction dynamics. Supersonic metal atomic beam is generated by laser vaporization of metal rod, and free expansion design without gas flow channel has been employed to obtain a good quality of metal atomic beam. We have chosen the crossed-beam reaction Al＋O2 to test the performance of the new apparatus. Two-rotational-states selected AIO（X^2∑＋, v=0, N and N＋I4） products can be imaged via P（N） and R（N＋14） branches of the Av=l band at the same wavelength, during （1＋1） resonance-enhanced multi-photon ionization through the AIO（D2E＋） intermediate state. In our experiment at 244.145 nm for simultaneous transitions of P（15） and R（29） branch, two rings in slice image were clearly distinguishable, corresponding to the AiO（v=0, N=IS） and AIO（v=0, N=29） states respectively. The energy difference between the two rotational levels is 403 cm^-1. The success of two states resolved in our apparatus suggests a better collisional energy resolution compared with the recent research study [J. Chem. Phys. 140, 214304 （2014）].展开更多
The reaction dynamics of yttrium atoms with sulfur dioxide molecules at a high collision energy of 36 kcal/mol was studied using time-sliced velocity map ion imaging,crossed molecular beam and laser-ablation method.Th...The reaction dynamics of yttrium atoms with sulfur dioxide molecules at a high collision energy of 36 kcal/mol was studied using time-sliced velocity map ion imaging,crossed molecular beam and laser-ablation method.The product YO was detected via multiphoton ionization at various wavelengths in the region of 482-615 nm.The slice images of YO show a broad velocity distribution and forward-backward peaking angular distribution.The forward scattering signal is stronger than its backward distribution.This indicates that the reaction proceeds via an intermediate complex and the lifetime of the intermediate state is less than one rotational period.The formation of complex suggests that electron transfer occurs in the oxidation reaction.展开更多
One of the themes of modern molecular reac tion dynamics is to charac terize elementary chemical reactions from“quan tum state to quan tum stat e”,and the study of molecular reaction dynamics in excited states can h...One of the themes of modern molecular reac tion dynamics is to charac terize elementary chemical reactions from“quan tum state to quan tum stat e”,and the study of molecular reaction dynamics in excited states can help test the validi ty of modern chemical t heories and provide met hods to cont rol chemical reactions.The subject of this review is to describe the recent experimental techniques used to study the reaction dynamics of metal atoms in the gas phase.Through these techniques,information such as the internal energy distribution and angular distribution of the nascent products or the three-dimensional stereodynamic reactivity can be obtained.In addition,by preparing metal at oms wi th specific exci ted elec tronic states or orbi tal arrangemen ts,information about the reactivity of the electronic states enriches the relevant understanding of the electron transfer mechanism in metal reaction dynamics.展开更多
A two-dimensional single-mode laser model with cross-correlation between the real and imaginary parts of the colored quadric pump noise is investigated. A novel laser amplitude Langevin equation is obtained, in which ...A two-dimensional single-mode laser model with cross-correlation between the real and imaginary parts of the colored quadric pump noise is investigated. A novel laser amplitude Langevin equation is obtained, in which the cross-correlation λp between the real and imaginary parts of the pump noise appears. The mean, variance, and skewness of first-passage-time are calculated. It is shown that the mean, variance, and skewness of first-passage-time are strongly affected by λp.展开更多
基金We are indebted to Prof. Kopin Liu （IAMS, Taipei） for stimulating discussions on going experiments, to Prof. Ming-fei Zhou and Assoc. Prof. Guan-jun Wang （Fudan University, Shanghai） for assistance in building machine, to Prof. Uzi. Even （Tel Aviv University, Tel Aviv） for discussions oil E1 valve employnmnt in laser ablation, and to Prof. Xue-ming Yang＇s group （DICP, Dalian） for new Iaser system. This work was supported by the National Natural Science Foundation of China （No.21322309） and the Program for Professor of Special Appointment （Eastern Scholar） at Shanghai Institutions of Higher Learning.
文摘We report a newly constructed laser ablation crossed molecular beam apparatus, equipped with time-sliced velocity map imaging technique, to study state-to-state metal atom reaction dynamics. Supersonic metal atomic beam is generated by laser vaporization of metal rod, and free expansion design without gas flow channel has been employed to obtain a good quality of metal atomic beam. We have chosen the crossed-beam reaction Al＋O2 to test the performance of the new apparatus. Two-rotational-states selected AIO（X^2∑＋, v=0, N and N＋I4） products can be imaged via P（N） and R（N＋14） branches of the Av=l band at the same wavelength, during （1＋1） resonance-enhanced multi-photon ionization through the AIO（D2E＋） intermediate state. In our experiment at 244.145 nm for simultaneous transitions of P（15） and R（29） branch, two rings in slice image were clearly distinguishable, corresponding to the AiO（v=0, N=IS） and AIO（v=0, N=29） states respectively. The energy difference between the two rotational levels is 403 cm^-1. The success of two states resolved in our apparatus suggests a better collisional energy resolution compared with the recent research study [J. Chem. Phys. 140, 214304 （2014）].
基金supported by the National Natural Science Foundation of China (No.21673047,No.21327901and No.21573047)the Shanghai Key Laboratory Foundation of Molecular Catalysis and Innovative Materialsthe Program for Professor of Special Appointment(Eastern Scholar) at Shanghai Institutions of Higher Learning.
文摘The reaction dynamics of yttrium atoms with sulfur dioxide molecules at a high collision energy of 36 kcal/mol was studied using time-sliced velocity map ion imaging,crossed molecular beam and laser-ablation method.The product YO was detected via multiphoton ionization at various wavelengths in the region of 482-615 nm.The slice images of YO show a broad velocity distribution and forward-backward peaking angular distribution.The forward scattering signal is stronger than its backward distribution.This indicates that the reaction proceeds via an intermediate complex and the lifetime of the intermediate state is less than one rotational period.The formation of complex suggests that electron transfer occurs in the oxidation reaction.
基金The work was supported by the National Natural Science Foundation of China(No.21673047 and No.22073019)the Shanghai Key Laboratory Foundation of Molecular Catalysis and Innovative Materialsthe Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning.
文摘One of the themes of modern molecular reac tion dynamics is to charac terize elementary chemical reactions from“quan tum state to quan tum stat e”,and the study of molecular reaction dynamics in excited states can help test the validi ty of modern chemical t heories and provide met hods to cont rol chemical reactions.The subject of this review is to describe the recent experimental techniques used to study the reaction dynamics of metal atoms in the gas phase.Through these techniques,information such as the internal energy distribution and angular distribution of the nascent products or the three-dimensional stereodynamic reactivity can be obtained.In addition,by preparing metal at oms wi th specific exci ted elec tronic states or orbi tal arrangemen ts,information about the reactivity of the electronic states enriches the relevant understanding of the electron transfer mechanism in metal reaction dynamics.
基金The project supported by National Natural Science Foundation of China under Grant No. 10275025 and the Education Foundation of Hebei Province under Grant No. 2004D006.
文摘A two-dimensional single-mode laser model with cross-correlation between the real and imaginary parts of the colored quadric pump noise is investigated. A novel laser amplitude Langevin equation is obtained, in which the cross-correlation λp between the real and imaginary parts of the pump noise appears. The mean, variance, and skewness of first-passage-time are calculated. It is shown that the mean, variance, and skewness of first-passage-time are strongly affected by λp.
