1999 年度実績報告書

大気中の原子・分子過程計算システム

研究課題

研究課題/領域番号	11166270
研究機関	岡崎国立共同研究機構
研究代表者	岩田末廣岡崎国立共同研究機構, 分子科学研究所, 教授 (20087505)
研究分担者	池上努岡崎国立共同研究機構, 分子科学研究所, 助手 (80245612)
キーワード	振動回転スペクトル / 計算化学 / 理論化学 / 遷移確率 / 大気化学 / ヒドロキシラジカル / イソプレン / 揮発性有機化合物
研究概要	1)一酸化炭素CO分子基底状態のポテンシャルエネルギー曲線と双極子モーメント関数を量子化学計算により精密に計算し、振動回転準位間の遷移確率をもとめた。この結果を用いて、NASAが人工衛星上で観測した太陽大気中のCOの赤外吸収スペクトルを再現し、太陽大気のCOが5000Kから5500Kの温度域に分布していることを明らかにした。 2)CO^+のいくつかの電子状態のポテンシャルエネルギー曲線と遷移双極子モーメント関数を計算し、最新の実験データを解析した。X,A,B状態の高い振動準位まで実験と一致し、電子振動準位間の相互作用によってボルン・オッペンハイマー近似が破れる状況を例示することに成功した。特に、D状態の振動プログレッションと帰属されているスペクトルの解析には、二つの透熱的状態間の相互作用によって2^2Πと3^2Π状態に分かれていることを考えに入れなければならないことを示した。 3)大気中の揮発性有機化合物(VOC)であるメタン、エタン、アセチレンとOHラジカルの反応を量子化学的に追跡し、反応中間体の同定、反応の律速段階・反応障壁を定量的にもとめた。 4)植物起源のVOCの中で最も重要なイソプレンの酸化過程のモデルを量子化学計算によって検証した。初期過程はOHとの反応であるが、最終生成物であるアルデヒドやケトンにまで反応が進むには、NOやO_3などの関与が必要となることを確認することができた。

研究成果
(18件)

すべてその他

すべて文献書誌 (18件)

[文献書誌] Seiichiro Ten-no, Suehiro Iwata, Sourav Pal and Debashis Mukherjee: "Generalization of the coupled-cluster response theory to multireference expansion spaces: an application of the coupled-cluster singles and doubles effective Hamiltonian"Theor. Chem. Accounts. 102. 252 (1999)
[文献書誌] Tadayoshi Suzuki, Tsutomu Ikegami, Masaaki Fujii and Suehiro Iwata: "Theoretical studies of internal methyl rotations in m-xylene: Comparison of Franck-Condon factors with the experimental spectra"J. Molec. Struc. (THEOCHEM). 461-462. 79-90 (1999)
[文献書誌] Tsutomu Ikegami and Suehiro Iwata: "Photodissociation dynamics of argon cluster ions"J. Chem. Phys.. 110. 8492-8500 (1999)
[文献書誌] Petr Nachtigall, Jan Hrusak, Ota Bludsky and Suehiro Iwata: "Investigation of the potential energy surfaces for the ground X^1A_1 and excited C^1B_2 electronic states of SO_2"Chem. Phys. Letters. 303. 441-1446 (1999)
[文献書誌] Kyoung K. Baeck, Heechol Choi and Suehiro Iwata: "Theoretical study on spectroscopic properties of positive, neutral and negative species of BCl_2 and AlCl_2 : The stability of the neative species"J. Phys. Chem.. A103. 6772-6777 (1999)
[文献書誌] Jan Hrusak, Zdenek Herman and Suehiro Iwata: "The heat of formation of the SiF_2 ^<++> dication: A theoretical prediction"Int. J. Mass Spectr. 192. 165-171 (1999)
[文献書誌] Nooru Watanabe, Seiichiro Ten-no, Sourav Pal, Suehiro Iwata and Yasuo Udagawa: "Size-extensive calculations of static structure factors from the coupled cluster singles and doubles model"J. Chem. Phys.. 111. 827-832 (1999)
[文献書誌] Pradipta Bandyopadhyay, Seiichiro Ten-no and Suehiro Iwata: "Structures and photoelectron spectroscopies of Si_2 C_2 studied with ab initio multicanonical Monte Carlo simulation"J. Phys. Chem.. 103. 6442-6447 (1999)
[文献書誌] Seiichiro Tenno and Suehiro Iwata: "On connection between the reference interaction site model integral equation theory and the partial wave expansion of molecular Orstein-Zernike equation"J. Chem. Phys. 111. 4865-4868 (1999)
[文献書誌] Wen-Ning Wang, Hai-Rong Tan, Kang-Nian Fan and Suehiro Iwata: "Theoretical studies of [Si_4 NO]^- with ab initio MO and DFT methods"Chem. Phys. Letters. 310. 313-322 (1999)
[文献書誌] Takeshi Tsurusawa and Suehiro Iwata: "Theoretical studies of structures and ionization threshold energies of water cluster complexes with a group 1 metal, M(H_2 O)_n (M=Li and Na)"J. Phys. Chem. A103. 6134-6141 (1999)
[文献書誌] Morihisa Saeki, Tatsuya Tsukuda, Suehiro Iwata and Takashi Nagata: "Electronic Isomers in [(CO_2 )_n ROH]^- cluster anions. II. Ab initio calculations"J. Chem. Phys. 111. 6333-6343 (1999)
[文献書誌] Katsuhiko Satoh and Suehiro Iwata: "Theoretical study of vibrational spectra for Cl^- (H_2 O): Temperature dependence and the influenced of Ar_0 (n=1-3)"Chem. Phys. Letters. 312. 522-529 (1999)
[文献書誌] Kazutoshi Okada and Suehiro Iwata: "Accurate potential energy and transition dipole moment curves of several electronic states of CO^+"J. Chem. Phys. 112. 1804-1808 (2000)
[文献書誌] Takeshi Tsurusawa and Suehiro Iwata: "Theoretical studies of the water cluster anions containing the OH{e}HO structure: energies and harmonic frequencies"Chem. Phys. Letters. 315. 433-440 (2000)
[文献書誌] Kazutoshi Okada and Suehiro Iwata: "Ab initio studies of several excited states of CO^+"J. Elect. Spectr. (in press). (2000)
[文献書誌] Takeshi Tsurusawa and Suehiro Iwata: "The electron-hydrogen bonds and the OH harmonic frequency shifts in water cluster complexes with a group 1 metal atom, M(H_2 O)_n (M=Li and Na)"J. Chem. Phys. (in press). (2000)
[文献書誌] Tsutomu Ikegami and Suehiro Iwata: "Spectral density calculation by using the Chebyshev expansion"J. Chem. Phys.. (submitted). (2000)

1999 年度 実績報告書

大気中の原子・分子過程計算システム

研究代表者

岩田 末廣 岡崎国立共同研究機構, 分子科学研究所, 教授 (20087505)

研究成果

[文献書誌] Seiichiro Ten-no, Suehiro Iwata, Sourav Pal and Debashis Mukherjee: "Generalization of the coupled-cluster response theory to multireference expansion spaces: an application of the coupled-cluster singles and doubles effective Hamiltonian"Theor. Chem. Accounts. 102. 252 (1999)

[文献書誌] Tadayoshi Suzuki, Tsutomu Ikegami, Masaaki Fujii and Suehiro Iwata: "Theoretical studies of internal methyl rotations in m-xylene: Comparison of Franck-Condon factors with the experimental spectra"J. Molec. Struc. (THEOCHEM). 461-462. 79-90 (1999)

[文献書誌] Tsutomu Ikegami and Suehiro Iwata: "Photodissociation dynamics of argon cluster ions"J. Chem. Phys.. 110. 8492-8500 (1999)

[文献書誌] Petr Nachtigall, Jan Hrusak, Ota Bludsky and Suehiro Iwata: "Investigation of the potential energy surfaces for the ground X^1A_1 and excited C^1B_2 electronic states of SO_2"Chem. Phys. Letters. 303. 441-1446 (1999)

[文献書誌] Kyoung K. Baeck, Heechol Choi and Suehiro Iwata: "Theoretical study on spectroscopic properties of positive, neutral and negative species of BCl_2 and AlCl_2 : The stability of the neative species"J. Phys. Chem.. A103. 6772-6777 (1999)

[文献書誌] Jan Hrusak, Zdenek Herman and Suehiro Iwata: "The heat of formation of the SiF_2 ^<++> dication: A theoretical prediction"Int. J. Mass Spectr. 192. 165-171 (1999)

[文献書誌] Nooru Watanabe, Seiichiro Ten-no, Sourav Pal, Suehiro Iwata and Yasuo Udagawa: "Size-extensive calculations of static structure factors from the coupled cluster singles and doubles model"J. Chem. Phys.. 111. 827-832 (1999)

[文献書誌] Pradipta Bandyopadhyay, Seiichiro Ten-no and Suehiro Iwata: "Structures and photoelectron spectroscopies of Si_2 C_2 studied with ab initio multicanonical Monte Carlo simulation"J. Phys. Chem.. 103. 6442-6447 (1999)

[文献書誌] Seiichiro Tenno and Suehiro Iwata: "On connection between the reference interaction site model integral equation theory and the partial wave expansion of molecular Orstein-Zernike equation"J. Chem. Phys. 111. 4865-4868 (1999)

[文献書誌] Wen-Ning Wang, Hai-Rong Tan, Kang-Nian Fan and Suehiro Iwata: "Theoretical studies of [Si_4 NO]^- with ab initio MO and DFT methods"Chem. Phys. Letters. 310. 313-322 (1999)

[文献書誌] Takeshi Tsurusawa and Suehiro Iwata: "Theoretical studies of structures and ionization threshold energies of water cluster complexes with a group 1 metal, M(H_2 O)_n (M=Li and Na)"J. Phys. Chem. A103. 6134-6141 (1999)

[文献書誌] Morihisa Saeki, Tatsuya Tsukuda, Suehiro Iwata and Takashi Nagata: "Electronic Isomers in [(CO_2 )_n ROH]^- cluster anions. II. Ab initio calculations"J. Chem. Phys. 111. 6333-6343 (1999)

[文献書誌] Katsuhiko Satoh and Suehiro Iwata: "Theoretical study of vibrational spectra for Cl^- (H_2 O): Temperature dependence and the influenced of Ar_0 (n=1-3)"Chem. Phys. Letters. 312. 522-529 (1999)

[文献書誌] Kazutoshi Okada and Suehiro Iwata: "Accurate potential energy and transition dipole moment curves of several electronic states of CO^+"J. Chem. Phys. 112. 1804-1808 (2000)

[文献書誌] Takeshi Tsurusawa and Suehiro Iwata: "Theoretical studies of the water cluster anions containing the OH{e}HO structure: energies and harmonic frequencies"Chem. Phys. Letters. 315. 433-440 (2000)

[文献書誌] Kazutoshi Okada and Suehiro Iwata: "Ab initio studies of several excited states of CO^+"J. Elect. Spectr. (in press). (2000)

[文献書誌] Takeshi Tsurusawa and Suehiro Iwata: "The electron-hydrogen bonds and the OH harmonic frequency shifts in water cluster complexes with a group 1 metal atom, M(H_2 O)_n (M=Li and Na)"J. Chem. Phys. (in press). (2000)

[文献書誌] Tsutomu Ikegami and Suehiro Iwata: "Spectral density calculation by using the Chebyshev expansion"J. Chem. Phys.. (submitted). (2000)

1999 年度実績報告書

岩田末廣岡崎国立共同研究機構, 分子科学研究所, 教授 (20087505)