Selective Production and Kinetic Analysis of Singlet-state Metastable Molecular Nitrogen

单线态亚稳态氮分子的选择性生产及动力学分析

• 批准号: 14540469
• 负责人: UMEMOTO Hironobu
• 金额: $ 2.11万
• 依托单位: Japan Advanced Institute of Science and Technology
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (C)
• 财政年份: 2002
• 资助国家: 日本
• 起止时间: 2002 至 2003
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-14540469/
• 关键词: molecular nitrogen; metastable state; reactive process; atomic hydrogen; quantum yield; two-photon excitation; intersystem crossing; isotope effect; キセノン原子; 増幅自然放出; メタン; 水分子

The reactive processes of metastable molecular nitrogen were investigated.N_2(a^1Πg) was produced by laser two-photon excitation of ground-state molecular nitrogen.The near-by N_2(a'^1Σu)state can be produced by collisional relaxation of this N_2(a)state.H(D) atoms were identified by a two-photon laser-induced fluorescence technique as products of these metastable nitrogen molecules with some simple hydride(deuteride)compounds.The following results were obtained.(1)N_2(a')can be deactivated efficiently by hydrogen, methane, and water molecules and the production of H atoms is one of the major exit channels.(2)In the reaction of N_2(a') with CH_2D_2 and HOD, the yields of H and D atoms are the same, implying that, the reaction proceeds via intermediate complexes.(3)O_2 and Xe deactivate N_2(a')efficiently to produce triplet-state molecular nitrogen, while such intersystem crossing is inefficient in the collisional processes with N_2 and Ar.In addition to these, it was revealed that N_2(B^3Πg)and N_2(W^3Δu)states are produced selectively in the energy transfer from Xe(6s[3/2]_1) to N_2(X ^1Σg^+).The rate constants for the overall quenching of N_2(B^3 Πg, υ=0)are one order of magnitude smaller than those for the quenching of N_2(B^3 Πg, υ≧1). By choosing the amount of H(D) atoms produced in the reaction of Xe(6s[3/2]_1,) with H_2(D_2) as a standard, it was revealed that the production of H(D) atoms is one of the most important exit channels in the reaction of N_2(B^3 Πg, υ=0) with H_2(D_2), while the relaxation to N_2(A)is minor.These results are important not only in the field of basic science but also in the applied fields such as plasma technology.

研究了亚稳分子氮的反应过程。用激光双光子激发基态分子氮产生了N_2(a‘1Πg)。这种N_2(A)态的碰撞弛豫可以产生邻近的N_2(a’1Σu)态。用双光子激光诱导荧光技术鉴定了H(D)原子是这些亚稳态氮分子与一些简单的氢化物(氢化物)化合物的产物。结果表明：(1)N_2(a‘)可以被氢、甲烷、氢气和氢化物有效地失活。(2)在N_2(a‘)与CH_2D_2和HOD的反应中，H原子和D原子的产率相同，表明反应是通过中间体络合物进行的。(3)O_2和Xe能有效地钝化N_2(a’)生成三重态分子氮，而这种跨系反应在与N_2和Ar的碰撞过程中效率较低。此外，O_2和Xe能有效地钝化N_2(a‘)生成三重态分子氮。结果表明，在从Xe(6s[3/2]_1)到N_2(X^1Πg^+)的能量转移过程中，选择性地产生了N_2(B^3Δg)和N_2(W^3Σu)态，N_2整体猝灭(B^3Πg，υ=0)的速率常数比N_2(B^3Πg，υ≧1)猝灭的速率常数小一个数量级。通过选择Xe(6S[3/2]1)与H_2(D_2)反应产生的H(D)原子量作为标准，揭示了H(D)原子的产生是N_2(B^3Πg，υ=0)与H_2(D_2)反应中最重要的出射通道之一，而对N_2(A)的驰豫很小。这一结果不仅在基础科学领域具有重要意义，而且在等离子体技术等应用领域也具有重要意义。

项目成果

H.Matsumura: "Cat-CVD (Hot-wire CVD) ; How Different from PECVD in Preparing Amorphous Silicon"J.Non-Cryst.Solids. (In press). (2004)

H.Matsumura：“Cat-CVD（热线 CVD）；制备非晶硅与 PECVD 有何不同”J.Non-Cryst.Solids。

H.Umemoto: "Collisional Intersystem Crossing of N_2(a' ^1Σ_u^-) to Produce Triplet-state Molecular Nitrogen"J.Chem.Phys.. 118[22]. 10006-10011 (2003)

H.Umemoto：“N_2(a ^1Σ_u^-) 的碰撞系间交叉产生三重态分子氮”J.Chem.Phys.. 118[22] (2003)。

H.Umemoto: "Effects of Atomic Hydrogen in Gas Phase on a-Si : H and poly-Si Growth by Cat-CVD"J.Non-Cryst.Solids. 299-302,[Pt1]. 9-13 (2002)

H.Umemoto：“气相中的原子氢对 Cat-CVD 的 a-Si : H 和多晶硅生长的影响”J.Non-Cryst.Solids。

H.Umemoto: "Production Yields of H(D) atoms in the Reactions of N_2(a' ^1Σu^-) with H_2O, D_2O, and HOD"Bull.Chem.Soc.Jpn.. 76[2]. 291-294 (2003)

H.Umemoto：“N_2(a ^1Σu^-) 与 H_2O、D_2O 和 HOD 反应中 H(D) 原子的产率”Bull.Chem.Soc.Jpn.. 76[2]。 294（2003）

H.Matsumura et al.: "Recent Progress of Cat-CVD Research in Japan-Bridging between the First and Second Cat-CVD Conferences"Thin Solid Films. 430,[1,2]. 7-14 (2003)

H.Matsumura 等人：“日本 Cat-CVD 研究的最新进展 - 第一届和第二届 Cat-CVD 会议之间的桥梁”固体薄膜。