RESEARCH ON RECOMBINATION REACTIONS BETWEEN POSITIVE AND NEGATIVE IONS BY USING A CROSSED ION-BEAM METHOD

交叉离子束法研究正负离子复合反应

• 批准号: 09440201
• 负责人: TSUJI Masaharu
• 金额: $ 8.96万
• 依托单位: KYUSHU UNIVERSITY
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (B).
• 财政年份: 1997
• 资助国家: 日本
• 起止时间: 1997 至 2000
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-09440201/
• 关键词: ION BEAM; POSITIVE ION; NEGATIVE ION; EXCIMER; SPIN-ORBIT STATE; RARE GAS ION; EMISSION SPECTRUM; NEUTRALIZATION REACTION; 放電フロー法; 再結合反応; クラスタリング

A crossed ion-beam apparatus of positive and negative ions was constructed, and applied to the following neutralization reactions leading to rare gas halide excimers :Ar^+(^2P_<1/2,3/2>) + SF_6^-→ArF(B,C,D) + SF_5, (1)Kr^+(^2P_<1/2>) + C_6F_5Cl^- →KrCl(B,D) + C_6F_5, (2a)Kr^+(^2P_<3/2>) + C_6F_5Cl^- →KrCl(B,C) + C_6F_5. (2b)ArF(B-X,C-A) and KrCl(B-X,C-A,D-X) excimers are observed in reactions (1) and (2), respectively. No significant change in ArF((B-X,C-A) excimers was found, when the Ar^+(^2P_<1/2>) spin-orbit component was removed by the addition of N_2 to Ar. This suggests that the Ar^+(^2P_<1/2>)/SF_6^- does not provide ArF^* excimer or it gives the same excimer band. The relative formation rates of KrCl(B : C : D) in reaction (2a) were 0.05 : 0.00 : 0.95, while those in reaction (2b) were 0.71 : 0.29 : 0.00. The formation rate of KrCl(C) was small in both reactions at low operating pressures below 10^<-3> Torr. It was therefore concluded that the small formation rate of KrCl(C) is not due to its relatively long radiative lifetime, but due to its intrinsic feature.In order to obtain detailed information on the reaction dynamics of recombination reactions, theoretical ab initio calculations have been carried out for the He_2^+/C_6F_6^- reaction leading to low lying He_2^* states.In a preliminary experiment of this research project, we discovered a number of new emissions from rare gas heterodimers and heterotrimers.

建立了正负离子交叉束装置，并应用于下列产生稀有气体卤化物准分子的中和反应：Ar^+（^2P_<1/2，3/2>）+ SF_6^-→ArF（B，C，D）+ SF_5，（1）Kr^+（^2P_<1/2>）+ C_6F_5Cl^- →KrCl（B，D）+ C_6F_5，（2a）Kr^+（^2P_<3/2>）+ C_6F_5Cl^- →KrCl（B，C）+ C_6F_5。（2）在反应（1）和（2）中分别观察到ArF（B-X，C-A）和KrCl（B-X，C-A，D-X）准分子。在Ar中加入N_2去除Ar^+（^2P_<1/2>）自旋轨道成分后，未发现ArF（（B-X，C-A））准分子有明显变化。这表明Ar^+（^2P_<1/2>）/SF_6^-不提供ArF^* 激基缔合物，或者它提供相同的激基缔合物带。反应（2a）中KrCl（B：C：D）的相对生成速率为0.05：0.00：0.95，而反应（2 B）中的那些为0.71：0.29：0.00。在低于10 μ Torr的低操作压力下，两个反应中KrCl（C）的形成速率都很小<-3>。因此，KrCl（C）的小生成速率不是由于其相对较长的辐射寿命，而是由于其固有的特性。为了获得复合反应动力学的详细信息，本文对He_2^+/C_6F_6^-反应进行了理论从头计算，得到了低能级的He_2^* 在该研究项目的初步实验中，我们发现了一些来自稀有气体异二聚体和异三聚体的新排放。

项目成果

Y.Tanaka,M.Tsuji,and Y.Nishimura: "Mass-Spectormetric Study on Ion-Molecule Reactions of CH_5^+, C_2H_5^+, and C_3H_5^+ with C_8-C_<18> n-Paraffins in an Ion Trap"Bulletin of the Chemical Society of Japan. 73・12. 2703-2712 (2000)

Y. Tanaka、M. Tsuji 和 Y. Nishimura：“离子阱中 CH_5^+、C_2H_5^+ 和 C_3H_5^+ 与 C_8-C_<18> 正构烷烃的离子分子反应的质谱研究“日本化学会会报。73・12.2703-2712（2000）

M.Tsuji et al.: "Decomposition of CO_2 into CO and O by a Microwave-Excited Discharge Flow of CO_2/He and CO_2/Ar Mixtures"Chemistry Letters. 1号. 22-23 (2001)

M.Tsuji等人：“通过CO_2/He和CO_2/Ar混合物的微波激发放电流将CO_2分解为CO和O”《化学快报》第1. 22-23号（2001）。

M.Tsuji, M.Aizawa, E.Oda, and Y.Nishimura: "Mass-Spectrometric Study on Ion-Molecule Reactions of CF_3^+ with PhX(X=F, Cl, Br, I) at Near-Thermal Energies"Bull.Chem.Soc.Jpn.. 70-5. 1179-1183 (1997)

M.Tsuji、M.Aizawa、E.Oda 和 Y.Nishimura：“CF_3^ 与 PhX(X=F、Cl、Br、I) 在近热能下离子分子反应的质谱研究”公牛

M.Tsuji, E.Oda, and Y.Nishimura: "Chemical Ionization Mass Spectra of Benzene and Toluene at Low CH_4 Pressures"Chem.Lett.. 8. 781-782 (1997)

M.Tsuji、E.Oda 和 Y.Nishimura：“低 CH_4 压力下苯和甲苯的化学电离质谱”Chem.Lett.. 8. 781-782 (1997)

M.Tsuji, M.Tanaka, and Y.Nishimura: "Emission Spectra of NeRg_2^+ (Rg=Ar, Kr, Xe), ArRg_2^+ (Rg=Kr, Xe), and KrXe_2^+ Heterotrimer Ions Produced in Rare Gas Flowing Afterglowsat High Stagnation Pressures"J.Chem.Phys.. 107-13. 4852-4863 (1997)

M.Tsuji、M.Tanaka 和 Y.Nishimura：“稀有气体流动余辉卫星中产生的 NeRg_2^ (Rg=Ar, Kr, Xe)、ArRg_2^ (Rg=Kr, Xe) 和 KrXe_2^ 异三聚体离子的发射光谱