Exploring general nature of interfacial melting on ice crystals: in situ approach by optical microscopy

• Project/Area Number: 21H01824
• Research Category: Grant-in-Aid for Scientific Research (B)
• Allocation Type: Single-year Grants
• Section: 一般
• Review Section: Basic Section 30010:Crystal engineering-related
• Research Institution: Hokkaido University
• Principal Investigator: Murata Kenichiro 北海道大学, 低温科学研究所, 助教 (60646272)
• Co-Investigator(Kenkyū-buntansha): 佐崎 元 北海道大学, 低温科学研究所, 教授 (60261509)
• Project Period (FY): 2021-04-01 – 2024-03-31
• Project Status: Completed (Fiscal Year 2023)
• Budget Amount: ¥17,680,000 (Direct Cost: ¥13,600,000、Indirect Cost: ¥4,080,000); Fiscal Year 2023: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000); Fiscal Year 2022: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000); Fiscal Year 2021: ¥13,520,000 (Direct Cost: ¥10,400,000、Indirect Cost: ¥3,120,000)
• Keywords: 氷の界面融解 / 擬似液体層 / 結晶成長 / 光学顕微鏡その場観察 / 不純物 / 潮解 / 疑似液体層

Outline of Research at the Start

本研究では, これまで精力的に研究されてきた気相に接した裸の氷の表面融解を越えて, 金属, 誘電体, 有機液体等に接した, より広義な氷界面での表面融解（氷の界面融解）の包括的理解を目指している. 特に, 光学顕微鏡法をベースにした非侵襲的なその場観察システムを新たに提案することで, 長年の懸案であった擬似液体層の厚みの精密測定を行う. 更に, 界面により誘起/抑制された擬似液体層の新たな熱力学的存在条件を探索することで, 一般化された氷の界面融解の普遍的性質を探求する. 加えて, 界面により誘起された擬似液体層を介した氷の新たな結晶成長機構を提案する.

Outline of Final Research Achievements

We focus on micro(nano)particles attached on ice crystal surfaces as a model of interfacial melting of ice crystals. We consider (i) roles of microparticles (or the interface between microparticles and ice crystal surfaces) for the generation of quasi-liquid layers (QLLs) and (ii) competition between microparticles and step dynamics on ice crystal surfaces. We reveal that microparticles are involved in the generation of QLLs through defects and dislocations induced by the microparticles themselves. We also demonstrate that surface elastic distortion, induced by the microparticles embedded in the ice crystal, affects the step dynamics.
In addition, we revisit deliquescence of sodium clorides to explore general nature of surface melting of ice crystals. We find similarities of wetting behavior between deliquescent liquid films and QLLs, which offer the possibility to understand the surface melting and the deliquescence in a unified manner.

Academic Significance and Societal Importance of the Research Achievements

本研究により，微粒子が結晶成長ダイナミクスや擬似液体層の生成に関与していることが明らかになった．本研究は特に上空での氷結晶とエアロゾルやブラックカーボンなどの不純物との関連を意識しているが，本成果を通じて，結晶成長学的視点から不純物を介した雲形成の新たな素過程を提示できる可能性がある．また，ごく最近，白金（111）面において，ステップが誘起する結晶表面の歪みが触媒活性を増強させるとの報告がある．本研究で示唆されるように，微粒子を介して結晶表面の歪みを制御できれば，触媒活性の更なる向上を狙った材料設計の可能性が開かれると考えられる．

Research Products

• [Journal Article] Step-bunching Instability of Growing Interfaces between Ice and Supercooled Water (2023)
  • Author(s): MURATA Ken-ichiro、SAZAKI Gen
  • Journal Title: Vacuum and Surface Science Volume: 66 Issue: 4 Pages: 221-226
  • DOI: 10.1380/vss.66.221
  • ISSN: 2433-5835, 2433-5843
  • Year and Date: 2023-04-10
  • Peer Reviewed
• [Journal Article] Microscopic ordering of supercooled water on the ice basal face (2023)
  • Author(s): Mochizuki Kenji、Murata Ken-ichiro、Zhang Xuan
  • Journal Title: Communications Materials Volume: 4 Issue: 1 Pages: 33-33
  • DOI: 10.1038/s43246-023-00359-2
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] <i>In situ</i> cryogenic transmission electron microscopy observation on the formation of hydrogen-ordered hexagonal ices and its astrophysical implications (2023)
  • Author(s): Yamazaki Tomoya、Kouchi Akira、Murata Ken-ichiro、Katsuno Hiroyasu、Nada Hiroki、Hama Tetsuya、Kimura Yuki
  • Journal Title: Monthly Notices of the Royal Astronomical Society Volume: 527 Issue: 2 Pages: 2858-2868
  • DOI: 10.1093/mnras/stad3401
  • Peer Reviewed / Open Access
• [Journal Article] The emergence of drop-type and thin-layer-type quasi-liquid layers on ice crystal surfaces and their thermodynamic origin (2022)
  • Author(s): Sazaki Gen、Murata Ken-ichiro、Asakawa Harutoshi、Nagashima Ken、Nakatsubo Shunichi、Furukawa Yoshinori
  • Journal Title: Journal of Crystal Growth Volume: 597 Pages: 126853-126853
  • DOI: 10.1016/j.jcrysgro.2022.126853
  • Peer Reviewed
• [Journal Article] Growth Kinetics of Elementary Spiral Steps on Ice Prism Faces Grown in Vapor and Their Temperature Dependence (2022)
  • Author(s): Miyamoto Genki、Kouchi Akira、Murata Ken-ichiro、Nagashima Ken、Sazaki Gen
  • Journal Title: Crystal Growth & Design Volume: 22 Issue: 11 Pages: 6639-6646
  • DOI: 10.1021/acs.cgd.2c00851
  • Peer Reviewed
• [Journal Article] Step-bunching instability of growing interfaces between ice and supercooled water (2022)
  • Author(s): Murata Ken-ichiro、Sato Masahide、Uwaha Makio、Saito Fumiaki、Nagashima Ken、Sazaki Gen
  • Journal Title: Proceedings of the National Academy of Sciences Volume: 119 Issue: 10
  • DOI: 10.1073/pnas.2115955119
  • Peer Reviewed
• [Journal Article] In-situ optical microscopy observation of elementary steps on ice crystals grown in vapor and their growth kinetics (2021)
  • Author(s): Sazaki Gen、Inomata Masahiro、Asakawa Harutoshi、Yokoyama Etsuro、Nakatsubo Shunichi、Murata Ken-ichiro、Nagashima Ken、Furukawa Yoshinori
  • Journal Title: Progress in Crystal Growth and Characterization of Materials Volume: 67 Issue: 4 Pages: 100550-100550
  • DOI: 10.1016/j.pcrysgrow.2021.100550
  • Peer Reviewed
• [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] 高分解光学顕微鏡で見る氷結晶のミクロな成長ダイナミクス (2021)
  • Author(s): 村田憲一郎
  • Journal Title: 化学と工業 Volume: 74(5) Pages: 360-362
  • Peer Reviewed
• [Presentation] 氷の表面融解における不純物効果 (2024)
  • Author(s): 村田 憲一郎
  • Organizer: 日本物理学会2024年春季大会
• [Presentation] Structure and dynamics of growing interfaces between ice and supercooled water: A link between molecular ordering and step-bunching instability (2023)
  • Author(s): Ken-ichiro Murata
  • Organizer: The 9th International Discussion Meeting on Relaxations in Complex Systems (9 IDMRCS)
  • Int'l Joint Research / Invited
• [Presentation] Step-bunching instability of growing interfaces between ice and supercooled water (2023)
  • Author(s): Ken-ichiro Murata
  • Organizer: The 15th International Conference on the Physics and Chemistry of Ice (PCI-2023)
  • Int'l Joint Research / Invited
• [Presentation] Microscopic Ordering of Supercooled Water on the Ice Basal Face (2023)
  • Author(s): Ken-ichiro Murata
  • Organizer: The 15th International Conference on the Physics and Chemistry of Ice (PCI-2023)
  • Int'l Joint Research
• [Presentation] 潮解再訪：濡れと結晶成長・融解ダイナミクスの競合 (2023)
  • Author(s): 村田 憲一郎
  • Organizer: 日本物理学会第78回年次大会
• [Presentation] 潮解再訪：濡れと結晶成長・溶解ダイナミクスの競合 (2023)
  • Author(s): 村田 憲一郎
  • Organizer: 第52回結晶成長国内会議
• [Presentation] 氷の融液成長界面における秩序形成と成長ダイナミクス (2022)
  • Author(s): 村田憲一郎
  • Organizer: 日本物理学会 2022年秋季大会
• [Presentation] 氷の融液成長界面における秩序形成と成長ダイナミクス (2022)
  • Author(s): 村田憲一郎
  • Organizer: 第51回結晶成長国内会議