Theoretical Chemistry of Molecular Processes in Atmospheric Environment

大气环境中分子过程的理论化学

• 批准号: 11166270
• 负责人: IWATA Suehiro
• 金额: $ 11.52万
• 依托单位: National Institution for Academic Degrees (2001)Hiroshima University (2000)Okazaki National Research Institutes (1999)
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research on Priority Areas (A)
• 财政年份: 1999
• 资助国家: 日本
• 起止时间: 1999 至 2001
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-11166270/
• 关键词: carbon monoxide; vibration rotation spectra; water cluster anion; group 1 metal atom; hydroxyl radical; hydrocarbon; basis set superposition error; perturbation theory; 量子化学計算; 飽和炭化水素; イソプレン; 一酸化窒素; オキソニウム; 水和クラスター; 計算化学; 理論化学; 遷移確率; 大気化学

Computational chemistry now not only helps to analyze the experimental data but also provides original data and information on chemical and physical problems. The atmospheres of the earth, the sun and planets consist mostly of simple molecules. The molecular species involved in the chemical processes in the troposphere and stratosphere of the earth are also not large molecules except for biological substances. Therefore, computational chemistry has a extremely large potentiality in the research of the atmospheric environment. Lt is, however, not much explored yet. Under this project, we have studied the following subjects to demonstrate it.1) Accurate calculations of some spectroscopic properties of the basic molecules such as N_2 and CO.2) Structures and spectroscopic characteristics of water cluster anions and hydrated group 1 metal clusters. The finding of a new type of bonding, electron-hydrogen bond.3) The reactions of saturated hydrocarbons with a hydroxyl radical.4)A series of reactions initiated by the reaction of isoprene with a hydroxyl rqadical.5) The formation reactions of H_3O^+ at the D region of the ionosphere.6) The development of the BSSE free molecular orbital theories with projection operator formalism.7) Structures and stability of a Group 1 metal ion solvated with rare gas atoms.

计算化学现在不仅有助于分析实验数据，而且为化学和物理问题提供原始数据和信息。地球、太阳和行星的大气层主要由简单分子组成。地球对流层和平流层中参与化学过程的分子种类，除生物物质外，也都不是大分子。因此，计算化学在大气环境的研究中具有极大的潜力。然而，这方面的探索还不多。在这个项目中，我们研究了以下科目来证明它。1)准确计算了N_2和co等碱性分子的一些光谱性质；2)水簇阴离子和水合1族金属簇的结构和光谱特性。发现了一种新型键，电子-氢键。饱和烃与羟基自由基的反应。异戊二烯与羟基自由基反应引发的一系列反应。5)电离层D区H_3O^+的生成反应。6)基于投影算符形式的BSSE自由分子轨道理论的发展。1族金属离子与稀有气体原子溶剂化的结构和稳定性。

项目成果

E.O.Sako, Y.Kanameda, E.Ikenaga, M.Mitani, O.Takahashi, K.Saito, S.Iwata, S.Wada, T.Sekitani, K.Tanaka: "Mechanism of ion desorption reaction of PMMA thin film induced by core excitation,"J.Electron Spectrosc.Relat.Phenom.. 114-116. 591-596 (2001)

E.O.Sako、Y.Kanameda、E.Ikenaga、M.Mitani、O.Takahashi、K.Saito、S.Iwata、S.Wada、T.Sekitani、K.Tanaka：“PMMA 薄膜诱导的离子解吸反应的机理

K.Okada: "Ab initio MO study of A,D and third ^2Π states of CO^+,"J.Electron Spectroscopy and Related Phenomena. 108. 225-234 (2000)

K.Okada：“A、D 和 CO^+ 的第三 ^2Π 态的从头 MO 研究”，J. 电子谱学和相关现象。 108. 225-234 (2000)

T.Hashimoto, S.Iwata: "Theoretical study on the weakly-bound complexes in the reactions of hydroxyl radical with saturated hydrocarbons (methane, ethane and propane)"J. Phys. Chem. (In press). (2002)

T.Hashimoto，S.Iwata：“羟基自由基与饱和烃（甲烷、乙烷和丙烷）反应中弱结合配合物的理论研究”J。

K.Okada: "Accurate potential energy and transition dipole moment curves of several electronic states of CO^+"J.Chemical Physics. 112. 1804-1808 (2000)

K.Okada：“CO^ 几种电子态的准确势能和跃迁偶极矩曲线”J.ChemicalPhysics。

O.Takahashi, M.Mitani, M.Joyabu, K.Saito, S.Iwata: "Theoretical studies on the molecular dependence of the bond dissociation after the core excitations : CH_3OCO(CH_2)_nCN, n=0,1,2"J. Electron Spectrosc. Relat. Phenom. 120. 137-148 (2001)

O.Takahashi、M.Mitani、M.Joyabu、K.Saito、S.Iwata：“核心激发后键解离的分子依赖性的理论研究：CH_3OCO(CH_2)_nCN，n=0,1,2”