Formation of hydrous silicate by photochemical reaction between ice and amorphous silicate at low temperatures

• Project/Area Number: 19K21887
• Research Category: Grant-in-Aid for Challenging Research (Exploratory)
• Allocation Type: Multi-year Fund
• Review Section: Medium-sized Section 17:Earth and planetary science and related fields
• Research Institution: Hokkaido University
• Principal Investigator: Kouchi Akira 北海道大学, 低温科学研究所, 教授 (60161866)
• Project Period (FY): 2019-06-28 – 2022-03-31
• Project Status: Completed (Fiscal Year 2021)
• Budget Amount: ¥6,370,000 (Direct Cost: ¥4,900,000、Indirect Cost: ¥1,470,000); Fiscal Year 2021: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000); Fiscal Year 2020: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000); Fiscal Year 2019: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000)
• Keywords: 非晶質珪酸塩 / 含水鉱物 / 氷 / 紫外線 / 低温 / 光化学反応 / 結晶化 / 非晶質ケイ酸塩 / 紫外線照射 / 含水ケイ酸塩

Outline of Research at the Start

低温の星間分子雲から原始太陽系外縁部に存在する，氷で覆われた非晶質ケイ酸塩を核とする微粒子は、紫外線の照射により氷の水分子が分解され反応性に富む OHラジカルができる．このOHラジカルは大きなエネルギーを持ち，10-150Kの低温でも非晶質ケイ酸塩と容易に反応して含水ケイ酸塩を作ると考えられる．これを透過型電子顕微鏡および高感度赤外分光装置を用いたその場観察法で調べる．非晶質ケイ酸塩としてはMg2SiO4およびMgSiO3組成の超微粒子および薄膜を用い，これらの超微粒子または薄膜を10-150Kに冷却，その上に氷を作製して紫外線を照射，構造，組織，赤外線吸収スペクトルの変化を観察する．

Outline of Final Research Achievements

To understand the formation mechanism of OH-bearing silicate at low temperatures, UV-irradiation experiments onto amorphous ice-covered amorphous silicate using a cryogenic transmission electron microscope. Three kind of amorphous silicate fine particles (Mg2SiO4, MgSiO3, and GEMS composition) were made by thermal plasma method. The formation of crystals was observed only when Mg2SiO4 particles were used at 82 K. None of formation was observed when MgSiO3 and GEMS particles were used. Crystals formed from amorphous Mg2SiO4 particles was identified using another high-resolution transmission electron microscope to be forsterite. It has been suggested that OH radicals formed by the photolysis of water molecules plays an essential role on the formation of forsterite.

Academic Significance and Societal Importance of the Research Achievements

原始惑星系における含水鉱物の生成は，地球型惑星の水の起源と関連するので，大変重要な課題である．これまでは非晶質珪酸塩と水蒸気の反応によって高温で含水鉱物が生成されると考えられてきた．今回の研究では，氷に紫外線を照射して生成されるOHラジカルによって，82Kという低温にもかかわらず非晶質珪酸塩が結晶化することが見出された．このことはOHラジカルと非晶質珪酸塩が反応して低温でも含水鉱物が生成される可能性があることを示したもので，今後の研究の展開に大きな期待を持たせる成果である．

Research Products

• [Journal Article] Measurements of ortho-to-para nuclear spin conversion of H2 on low-temperature carbonaceous grain analogs: Diamond-like carbon and graphite (2021)
  • Author(s): Tsuge Masashi、 Kouchi Akira、 Watanabe Naoki
  • Journal Title: The Astrophysical Journal Volume: 923 Issue: 1 Pages: 71-71
  • DOI: 10.3847/1538-4357/ac2a33
  • Peer Reviewed / Open Access
• [Journal Article] UV-induced formation of ice XI observed using an ultra-high vacuum cryogenic transmission electron microscope and its implications for planetary science (2021)
  • Author(s): Kouchi Akira、Kimura Yuki、Kitajima Kensei、Katsuno Hiroyasu、Hidaka Hiroshi、Oba Yasuhiro、Tsuge Masashi、Yamazaki Tomoya、Fujita Kazuyuki、Hama Tetsuya、Takahashi Yukihiro、Nakatsubo Shunichi、Watanabe Naoki
  • Journal Title: Frontiers in Chemistry Volume: 9 Pages: 799851-799851
  • DOI: 10.3389/fchem.2021.799851
  • Peer Reviewed / Open Access
• [Journal Article] Successive H-atom Addition to Solid OCS on Compact Amorphous Solid Water (2021)
  • Author(s): Nguyen Thanh、Oba Yasuhiro、Sameera W. M. C.、Kouchi Akira、Watanabe Naoki
  • Journal Title: The Astrophysical Journal Volume: 922 Issue: 2 Pages: 146-146
  • DOI: 10.3847/1538-4357/ac2238
  • Peer Reviewed / Open Access
• [Journal Article] Efficient formation pathway of methyl formate: The role of OH radicals on ice dust (2021)
  • Author(s): Ishibashi Atsuki、Hidaka Hiroshi、Oba Yasuhiro、Kouchi Akira、Watanabe Naoki
  • Journal Title: The Astrophysical Journal Letters Volume: 921 Issue: 1 Pages: L13-L13
  • DOI: 10.3847/2041-8213/ac3005
  • Peer Reviewed / Open Access
• [Journal Article] Experimental and Computational Studies on the Physicochemical Behavior of Phosphine Induced by Reactions with H and D Atoms on Interstellar Ice Grains (2021)
  • Author(s): Nguyen Thanh、Oba Yasuhiro、Sameera W. M. C.、Kouchi Akira、Watanabe Naoki
  • Journal Title: The Astrophysical Journal Volume: 918 Issue: 2 Pages: 73-73
  • DOI: 10.3847/1538-4357/ac0cf4
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Transmission Electron Microscopy Study of the Morphology of Ices Composed of H2O, CO2, and CO on Refractory Grains (2021)
  • Author(s): Kouchi, A., Tsuge, M., Hama, T., Oba, Y., Okuzumi, S., Sirono, S.-. iti ., Momose, M., Nakatani, N., Furuya, K., Shimonishi, T., Yamazaki, T., Hidaka, H., Kimura, Y., Murata, K.-. ichiro ., Fujita, K., Nakatsubo, S., Tachibana, S., & Watanabe, N.
  • Journal Title: The Astrophysical Journal Volume: 918 Issue: 2 Pages: 45-45
  • DOI: 10.3847/1538-4357/ac0ae6
  • Peer Reviewed / Open Access
• [Journal Article] Formation of chiral CO polyhedral crystals on icy interstellar grains (2021)
  • Author(s): Kouchi, A., Tsuge, M., Hama, T., Niinomi, H., Nakatani, N., Shimonishi, T., Oba, Y., Kimura, Y., Sirono, S.-. iti ., Okuzumi, S., Momose, M., Furuya, K., & Watanabe, N.
  • Journal Title: Monthly Notices of the Royal Astronomical Society Volume: 505 Issue: 1 Pages: 1530-1542
  • DOI: 10.1093/mnras/stab1173
  • NAID: 120007132042
  • Peer Reviewed / Open Access
• [Journal Article] Rapid Ortho-to-para Nuclear Spin Conversion of H2 on a Silicate Dust Surface (2021)
  • Author(s): Tsuge M., Namiyoshi T., Furuya K., Yamazaki T., Kouchi A., Watanabe N.
  • Journal Title: The Astrophysical Journal Volume: 908 Issue: 2 Pages: 234-234
  • DOI: 10.3847/1538-4357/abd9c0
  • Peer Reviewed / Open Access
• [Journal Article] CH3O radical binding on hexagonal water ice and amorphous solid water (2021)
  • Author(s): W. M. C. Sameera, B. Senevirathne, S. Andersson, M. Al-lbadi, H. Hidaka, A. Kouchi, G. Nyman, N. Watanabe
  • Journal Title: J. Phy. Chem. A Volume: 125 Issue: 1 Pages: 387-393
  • DOI: 10.1021/acs.jpca.0c09111
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Delivery of electrons by proton-hole transfer in ice at 10 K: Role of surface OH radicals (2021)
  • Author(s): K. Kitajima, Y. Nakai, W. M. C. Sameera, M. Tsuge, A. Miyazaki, H. Hidaka, A. Kouchi, N. Watanabe
  • Journal Title: J. Phys. Chem. Lett. Volume: 12 Issue: 1 Pages: 704-710
  • DOI: 10.1021/acs.jpclett.0c03345
  • Peer Reviewed
• [Journal Article] Photostimulated desorption of OH radicals from amorphous solid water: Evidence for the interaction of visible light with an OH-ice complex (2020)
  • Author(s): A. Miyazaki, N. Watanabe, W. M. C. Sameera, Y. Nakai, M. Tsuge, T. Hama, H. Hidaka, A. Kouchi
  • Journal Title: Phys. Rev. A Volume: 102 Issue: 5 Pages: 052822-052822
  • DOI: 10.1103/physreva.102.052822
  • Peer Reviewed
• [Journal Article] Diffusive hydrogenation reactions of CO embedded in amorphous solid water at elevated temperatures ～70K (2020)
  • Author(s): Tsuge M., Hidaka H., Kouchi A., Watanabe N.
  • Journal Title: The Astrophysical Journal Volume: 900 Issue: 2 Pages: 187-187
  • DOI: 10.3847/1538-4357/abab9b
  • Peer Reviewed
• [Journal Article] UV-ray irradiation never causes amorphization of crystalline CO2: A transmission electron microscopy study (2020)
  • Author(s): Tsuge M., Nguyen T., Oba Y., Hama T., Kouchi A., Watanabe N.
  • Journal Title: Chemical Physics Letters Volume: 760 Pages: 137999-137999
  • DOI: 10.1016/j.cplett.2020.137999
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Quantitative Anisotropic Analysis of Molecular Orientation in Amorphous N2O at 6 K by Infrared Multiple-Angle Incidence Resolution Spectrometry (2020)
  • Author(s): Hama T., Ishibashi A., Kouchi A., Watanabe N., Shioya N., Shimoaka T., Hasegawa T.
  • Journal Title: The Journal of Physical Chemistry Letters Volume: 11 Issue: 18 Pages: 7857-7866
  • DOI: 10.1021/acs.jpclett.0c01585
  • Peer Reviewed
• [Journal Article] In vivo characterization of the structures of films of a fatty acid and an alcohol adsorbed on the skin surface (2020)
  • Author(s): Hama T., Kouchi A., Watanabe N., Shioya N., Shimoaka T., Hasegawa T.
  • Journal Title: Biophysical Chemistry Volume: 266 Pages: 106459-106459
  • DOI: 10.1016/j.bpc.2020.106459
  • Peer Reviewed
• [Journal Article] An Experimental Study of Chemical Desorption for Phosphine in Interstellar Ice (2020)
  • Author(s): Nguyen T., Oba Y., Shimonishi T., Kouchi A., Watanabe N.
  • Journal Title: The Astrophysical Journal Letters Volume: 898, Issue: 2 Pages: L52-L52
  • DOI: 10.3847/2041-8213/aba695
  • Peer Reviewed / Open Access
• [Journal Article] High-density liquid water at a water-ice interface (2020)
  • Author(s): Niinomi H., Yamazaki T., Nada H., Hama T., Kouchi A., Okada J.T., Nozawa J., Uda S., Kimura Y.
  • Journal Title: The Journal of Physical Chemistry Letters Volume: 11 Pages: 6779-6784
  • Peer Reviewed
• [Journal Article] Precometary organic matter: A hidden reservoir of water inside the snow line (2020)
  • Author(s): Nakano Hideyuki、Hirakawa Naoki、Matsubara Yasuhiro、Yamashita Shigeru、Okuchi Takuo、Asahina Kenta、Tanaka Ryo、Suzuki Noriyuki、Naraoka Hiroshi、Takano Yoshinori、Tachibana Shogo、Hama Tetsuya、Oba Yasuhiro、Kimura Yuki、Watanabe Naoki、Kouchi Akira
  • Journal Title: Scientific Reports Volume: 10 Issue: 1 Pages: 7755-7755
  • DOI: 10.1038/s41598-020-64815-6
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Direct Measurements of Activation Energies for Surface Diffusion of CO and CO2 on Amorphous Solid Water Using In Situ Transmission Electron Microscopy (2020)
  • Author(s): A. Kouchi, K. Furuya , T. Hama , T. Chigai, T. Kozasa , and N. Watanabe
  • Journal Title: The Astrophysical Journal Letters Volume: 891 Issue: 1 Pages: L22-L22
  • DOI: 10.3847/2041-8213/ab78a2
  • Peer Reviewed / Open Access
• [Journal Article] DESHIMA on ASTE: On-Sky Responsivity Calibration of the Integrated Superconducting Spectrometer (2020)
  • Author(s): T. Takekoshi, ..., A. Kouchi, ..., Pieter J. de Visser
  • Journal Title: Journal of Low Temperature Physics Volume: - Issue: 1-2 Pages: 231-239
  • DOI: 10.1007/s10909-020-02338-0
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Ultraviolet-photon exposure stimulates negative current conductivity in amorphous ice below 50 K (2019)
  • Author(s): N. Watanabe, W. M. C. Sameera, H. Hidaka, A. Miyazaki, A. Kouchi
  • Journal Title: Chemical Physics Letters Volume: 737 Pages: 136820-136820
  • DOI: 10.1016/j.cplett.2019.136820
  • Peer Reviewed
• [Journal Article] First light demonstration of the integrated superconducting spectrometer (2019)
  • Author(s): A. Endo, ..., A. Kouchi, ... J. A. Baselmans
  • Journal Title: Nature Astronomy Volume: 3 Issue: 11 Pages: 989-996
  • DOI: 10.1038/s41550-019-0850-8
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Nucleobase synthesis in interstellar ices (2019)
  • Author(s): Y. Oba, Y. Takano, H. Naraoka, N. Watanabe and A. Kouchi
  • Journal Title: Nature Communications Volume: 10 Issue: 1 Pages: 4413-4413
  • DOI: 10.1038/s41467-019-12404-1
  • Peer Reviewed / Open Access
• [Journal Article] Probing the Molecular Structure and Orientation of the Leaf Surface of Brassica oleracea L. by Polarization Modulation-Infrared Reflection-Absorption Spectroscopy (2019)
  • Author(s): T. Hama, K. Seki, A. Ishibashi, A. Miyazaki, A. Kouchi, N. Watanabe, T. Shimoaka, T. Hasegawa
  • Journal Title: Plant Cell Physiology Volume: 60 Issue: 7 Pages: 1567-1580
  • DOI: 10.1093/pcp/pcz063
  • Peer Reviewed
• [Journal Article] Physico-chemical Behavior of Hydrogen Sulfide Induced by Reactions with H and D Atoms on Different Types of Ice Surfaces at Low Temperature (2019)
  • Author(s): Y. Oba, T.Tomaru, A. Kouchi, N. Naoki
  • Journal Title: The Astrophysical Journal Volume: 874 Issue: 2 Pages: 124-124
  • DOI: 10.3847/1538-4357/ab0961
  • Peer Reviewed / Open Access
• [Presentation] 低温氷表面上に存在する微量ラジカルの非破壊検出装置の開発 (2020)
  • Author(s): 石橋篤季, 日高宏, 大場康弘, 羽馬哲也, 香内晃, 渡部直樹
  • Organizer: 日本物理学会第75回年次大会
• [Presentation] Surface diffusion of OH radical on amorphous solid water (2019)
  • Author(s): Miyazaki, A. , Watanabe, N., Sameera, W.M.C, Hama, T. , Hidaka, H. , Kouchi, A.
  • Organizer: IAU Symposium 350
  • Int'l Joint Research
• [Presentation] Liquid-like behavior of water ice induced by vacuum ultraviolet irradiation at low temperatures (2019)
  • Author(s): HAMA, Tetsuya; TACHIBANA, Shogo; KOUCHI, Akira; OBA, Yasuhiro; PIANI, Laurette; HIDAKA, Hiroshi; KIMURA, Yuki; MURATA, Ken-ichiro; YURIMOTO, Hisayoshi; WATANABE, Naoki
  • Organizer: 35th Symposium on Chemical Kinetics and Dynamics
  • Int'l Joint Research
• [Presentation] Probing the molecular structure of the intact leaf cuticle by polarization modulation-infrared reflection-absorption spectroscopy (2019)
  • Author(s): T.HAMA,K.SEKI, A.ISHIBASHI,A. MIYAZAKI, A.KOUCHI,N.WATANABE, T.SHIMOAKA, T.HASEGAWA
  • Organizer: 35th Symposium on Chemical Kinetics and Dynamics
  • Int'l Joint Research
• [Presentation] H2 formation on a low-temperature diamondlike carbon surface (2019)
  • Author(s): TSUGE, Masashi; HAMA, Tetsuya; KIMURA, Yuki; KOUCHI, Akira; WATANABE, Naoki
  • Organizer: 35th Symposium on Chemical Kinetics and Dynamics
  • Int'l Joint Research
• [Presentation] Synthesis of Nitrogen Heterocycles of Astrobiologial Interest in Interstellar Ice Analogs (2019)
  • Author(s): Y.Oba,Y.Takano,H.Naraoka,N.Watanabe,A.Kouchi
  • Organizer: 2019 Astrobiology Science Conference
  • Int'l Joint Research
• [Presentation] Reactive desorption of methanol from amorphous solid water at 10K (2019)
  • Author(s): H.Hidaka, Y. Yarnall, A. Kouchi, N.Watanabe, The 12the meeting on cosmic dust
  • Organizer: The 12the meeting on cosmic dust
  • Int'l Joint Research / Invited
• [Presentation] Detection of nucleobases dipeptides in organic residues formed by photochemical reactions in interstellar ice analogs (2019)
  • Author(s): Y.Oba, Y.Takano,H.Naraoka,N.Watanabe,A. Kouchi
  • Organizer: Goldschmidt 2019
  • Int'l Joint Research
• [Presentation] Inversion of surface voltage on H2O films affection sublimation of CO underlayer (2019)
  • Author(s): A. Ishibashi, Y.Oba,T.Hama,A.kouchi,N.Watanabe
  • Organizer: ACS National Meeting & Expo
  • Int'l Joint Research
• [Presentation] Activation energy of OH-radical diffusion on water ice surface (2019)
  • Author(s): A. Miyazaki, N.Watanabe, W. Sameera, T.Hama, H.Hidaka, A.Kouchi
  • Organizer: ACS National Meeting & Expo
  • Int'l Joint Research
• [Presentation] アモルファスMg2SiO4微粒子を覆った氷の光化学反応によるフォルステライト結晶の生成 (2019)
  • Author(s): 香内晃,木村勇気,場康弘,羽馬哲也,渡部直樹,橘省吾,土山明,延寿里美,大坪貴文
  • Organizer: 日本地球惑星科学連合2019年大会
• [Presentation] 星間分子雲における化学進化：単純分子から核酸塩基生成へ (2019)
  • Author(s): 大場康弘,高野淑識,奈良岡浩,渡部直樹,香内晃
  • Organizer: 第37回有機地球化学シンポジウム
• [Presentation] 低温氷表面吸着物質の高感度非破壊質量分析装置の開発 (2019)
  • Author(s): 石橋篤季, 日高宏, 大場康弘, 羽馬哲也, 香内晃, 渡部直樹
  • Organizer: 原子衝突学会第 44 回年会
• [Presentation] 模擬星間塵氷の光化学反応による核酸塩基生成 (2019)
  • Author(s): 大場 康弘,高野 淑識,奈良岡 浩,渡部 直樹 ,香内 晃
  • Organizer: 日本地球化学会第66回年会
• [Remarks] 北海道大学低温科学研究所 宇宙物質科学・宇宙雪氷学グループHP
  • URL: http://www.lowtem.hokudai.ac.jp/astro/index.html
• [Remarks] 宇宙物質科学・宇宙雪氷学グループ
  • URL: http://www.lowtem.hokudai.ac.jp/astro/index.html