Growth mechanism of surface ice flakes at the initial stage of freezing of water-based organic solvent liquid film

SUN Yuyang; NIU Yuying; ZONG Xiaoxiao; ZHAO Yugang

doi:10.7498/aps.74.20250902

Abstract

Freezing of multicomponent droplets and thin films is ubiquitous in natural environments and engineered settings. Previous studies on multicomponent droplets, including Marangoni-driven self-lifting droplets and soap-bubble freezing, have identified the roles of interfacial flow and solute redistribution, often exhibiting a snow-globe effect of migrating ice particles. Curvature and field-of-view constraints in droplet systems hinder continuous observation of a single object. Here, utilizing the comparability of interfacial heat and mass transfer between droplets and films, we employ a flat isopropanol-water binary film on a cooled substrate to achieve high-resolution, time-resolved in-situ microscopy observation of individual separated ice flakes within a supercooling (ΔT) range of the substrate. Experiments show that with the increase of ΔT, the external shape of ice flakes evolves from hexagonal pyramid to dodecagonal pyramid and ultimately to a nearly-conical form, accompanied by the decrease of transparency. We quantify morphological evolution by using a shape factor β and qualitatively distinguish crystal-structure differences by combining bright-field and dark-field microscopy. A minimal model that couples solute and thermal diffusion with Marangoni stress rationalizes the observations: solute-concentration gradients primarily drive structural evolution, while the competition between advection and diffusion governs anisotropic growth. These results provide mechanistic insight into interfacial freezing dynamics of multi-component liquid films and establish flat-film microscopy as a platform for single-flake kinetics.

Keywords:

Authors and contacts

1.
Shanghai Key Laboratory of Multiphase Flow and Heat Transfer in Power Engineering, School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China
2.
Key Laboratory of Icing and Anti/De-Icing, China Aerodynamics Research and Development Center, Mianyang 621000, China

Corresponding author: ZHAO Yugang, ygzhao@usst.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 52276079).

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References

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Cited By

图 1 (a) 实验装置示意图; (b) 硅片处理前后接触角对比; (c) $\Delta T = \left( {5.5 \pm 0.1} \right)$ ℃时异丙醇-水液膜冻结过程; (d), (e) 对单个冰片的显微观察的时间起点和终点

Figure 1. (a) Schematic diagram of the experimental setup; (b) comparison of contact angles before and after plasma treatment of monocrystalline silicon wafers; (c) freezing process of isopropanol-water liquid film at $\Delta T = \left( {5.5 \pm 0.1} \right)$ ℃; (d), (e) the beginning and ending of microscopic observation of a single ice flake.

DownLoad: Full-Size Img PowerPoint

图 2 (a), (b) 不同过冷度下冰片生长动力学过程　(a) $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃; (b) $\Delta T = \left( {12.6 \pm 0.1} \right)$ ℃. (c), (d) 不同过冷度下冰片轮廓的变化 (c) $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃; (d) $\Delta T = \left( {12.6 \pm 0.1} \right)$ ℃

Figure 2. (a), (b) Kinetic processes of ice flakes growth at different supercooling degrees: (a) $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃; (b) $\Delta T = $$ \left( {12.6 \pm 0.1} \right)$ ℃. (c), (d) Changes of ice flake profiles at different supercooling degrees: (c) $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃; (d) $\Delta T = $$ \left( {12.6 \pm 0.1} \right)$ ℃.

DownLoad: Full-Size Img PowerPoint

图 3 明场以及暗场观察对比　(a) 明场观察示意图; (b) 暗场观察示意图; (c) $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃暗场下无法观察到冰片, 冰片几乎透明; (d) $\Delta T = \left( {12.6 \pm 0.1} \right)$ ℃暗场下观察到冰片为白色且不透明

Figure 3. Comparison of bright-field as well as dark-field observation: (a) Schematic of bright-field observation; (b) schematic of dark-field observation; (c) ice flakes could not be observed in the dark-field at $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃, and the ice flakes were almost transparent; (d) ice flakes were observed to be white and opaque in the dark-field at $\Delta T = \left( {12.6 \pm 0.1} \right)$ ℃.

DownLoad: Full-Size Img PowerPoint

图 4 (a) 不同过冷度下分离冰片形貌; (b) 形状因子定义; (c) 形状因子随过冷度变化规律

Figure 4. (a) Morphology of separated ice flakes at different supercooling degrees; (b) definition of shape factor; (c) variation rule of shape factor with supercooling degree.

DownLoad: Full-Size Img PowerPoint

图 5 物理机制示意图　(a) 低过冷度下结冰偏析与马兰戈尼流的产生; (b) 过冷度增加溶质扩散减弱, 浓度差增加马兰戈尼流增强, 冰片加速生长; (c) 大过冷度下马兰戈尼流减弱导致溶质富集

Figure 5. Schematic diagram of the physical mechanism: (a) Icing segregation and production of Marangoni flow at low subcooling; (b) weakened solute diffusion, enhanced Marangoni flow, and accelerated growth of ice flakes at increasing subcooling; (c) weakened Marangoni flow at large subcooling leading to solute enrichment.

DownLoad: Full-Size Img PowerPoint

图 6 (a) 冰片水平方向生长速度定义; (b) 冰片水平方向生长速度随过冷度变化

Figure 6. (a) Definition of the horizontal growth velocity of the ice flakes; (b) horizontal growth velocity versus supercooling.

DownLoad: Full-Size Img PowerPoint

图 7 冰片生长不同生长模式相图

Figure 7. Phase diagram of different growth modes of ice flakes.

DownLoad: Full-Size Img PowerPoint

map

[1]	Wu X M, Chu F Q, Ma Q, Zhu B 2017 Appl. Therm. Eng. 118 448 Google Scholar
[2]	Li L Y, Liu Z L, Li Y X, Dong Y W 2017 Int. J. Heat Mass Transfer 113 166 Google Scholar
[3]	Li K, Miao Y M, Xia D Y, Liu N, Zhang H, Dou B L, He Q Z, Zhao Y G, Li C, Mohtaram S 2024 Appl. Therm. Eng. 248 123282 Google Scholar
[4]	Wang P, Zhou W S, Bao Y Q, Li H 2018 Struct Control Health Monit. 25 e2138 Google Scholar
[5]	Wei K X, Yang Y, Zuo H Y, Zhong D Q 2020 Wind Energy 23 433 Google Scholar
[6]	Cebeci T, Kafyeke F 2003 Annu. Rev. Fluid Mech. 35 11 Google Scholar
[7]	Cao Y, Wu Z, Su Y, Xu Z 2015 Prog. Aeronaut. Sci. 74 62 Google Scholar
[8]	Hu H B, He Q, Yu S X, Zhang Z Z, Song D 2016 Acta Phys. Sin. 65 104703 [胡海豹, 何强, 余思潇, 张招柱, 宋东 2016 65 104703]Google Scholar Hu H B, He Q, Yu S X, Zhang Z Z, Song D 2016 Acta Phys. Sin. 65 104703 Google Scholar
[9]	He Z W, Zhuo Y Z, Wang F, He J Y, Zhang Z L 2019 Soft Matter 15 2905 Google Scholar
[10]	Ji K P, Rui X M, Li L, Leblond A, McClure G 2015 Comput. Struct. 157 153 Google Scholar
[11]	Gurganus C, Kostinski A B, Shaw R A 2011 J. Phys. Chem. Lett. 2 1449 Google Scholar
[12]	Gurganus C, Kostinski A B, Shaw R A 2013 J. Phys. Chem. C 117 6195 Google Scholar
[13]	Inada T, Tomita H, Koyama T 2014 Int. J. Refrig. 40 294 Google Scholar
[14]	Fletcher N H 1958 J. Chem. Phys. 29 572 Google Scholar
[15]	Wildeman S, Sterl S, Sun C, Lohse D 2017 Phys. Rev. Lett. 118 084101 Google Scholar
[16]	Jung S, Tiwari M K, Doan N V, Poulikakos D 2012 Nat. Commun. 3 615 Google Scholar
[17]	Wang Y, Cheng Y 2019 Int. J. Heat Mass Transfer 140 1023 Google Scholar
[18]	Peppin S S L, Elliott J A W, Worster M G 2006 J. Fluid Mech. 554 147 Google Scholar
[19]	Zhao Y, Yan Z, Zhang H, Yang C, Cheng P 2021 Int. J. Heat Mass Transfer 165 120609 Google Scholar
[20]	Marín A G, Enríquez O R, Brunet P, Colinet P, Snoeijer J H 2014 Phys. Rev. Lett. 113 054301 Google Scholar
[21]	Yan X, Au S C Y, Chan S C, Chan Y L, Leung N C, Wu W Y, Sin D T, Zhao G L, Chung C H Y, Mei M, Yang Y C, Qiu H H, Yao S S 2024 Nat. Commun. 15 1567 Google Scholar
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[23]	Fang W Z, Zhu F Q, Zhu L L, Tao W Q, Yang C 2022 Commun. Phys. 5 51 Google Scholar
[24]	Jin P H, Yan X, Hoque M J, Rabbi K F, Sett S, Ma J C, Li J Q, Fang X L, Carpenter J, Cai S J, Tao W Q, Miljkovic N 2022 Cell Rep. Phys. Sci. 3 100894 Google Scholar
[25]	张旋, 刘鑫, 吴晓敏, 闵敬春 2020 工程热 41 402 Zhang X, Liu X, Wu X M, Min J C 2020 J. Eng. Thermophys. 41 402
[26]	董琪琪, 胡海豹, 陈少强, 何强, 鲍路瑶 2018 67 054702 Google Scholar Dong Q Q, Hu H B, Chen S Q, He Q, Bao L Y 2018 Acta Phys. Sin. 67 054702 Google Scholar
[27]	Ivall J, Hachem M, Coulombe S, Servio P 2015 Cryst. Growth Des. 15 3969 Google Scholar
[28]	Zhao Y, Yang C, Cheng P 2021 Appl. Phys. Lett. 118 14 Google Scholar
[29]	Jiang Y P, Zhao Y G, Zhang H, Yang C, Cheng P 2024 Cell Rep. Phys. Sci. 5 4 Google Scholar
[30]	Zeng H, Wakata Y, Chao X, Li M B, Sun C 2023 J. Colloid and Interf. Sci. 648 736 Google Scholar
[31]	Dang Q, Song M L, Dang C B, Zhan T Z, Zhang L 2022 Langmuir 38 7846 Google Scholar
[32]	Miao Y M, Zhao Y G, Gao M, Yang L, Yang C 2022 Appl. Phys. Lett. 120 091602 Google Scholar
[33]	Chu F Q, Li S X, Zhao C J, Feng Y H, Lin Y K, Wu X M, Yan X, Miljkovic N 2024 Nat. Commun. 15 2249 Google Scholar
[34]	Schutzius T M, Jung S, Maitra T, Graeber G, Köhme M, Poulikakos D 2015 Nature 527 82 Google Scholar
[35]	Graeber G, Schutzius T M, Eghlidi H, Poulikakos D 2017 Proc. Natl. Acad. Sci. 114 11040 Google Scholar
[36]	Zhuo Y H, Xiao S B, Håkonsen V, He J Y, Zhang Z L 2020 ACS Mater. Lett. 2 616 Google Scholar
[37]	Zhu Z B, Zhang X, Zhao Y G, Huang X Y, Yang C 2022 Int. J. Therm. Sci. 171 107241 Google Scholar
[38]	Lambley H, Graeber G, Vogt R, Gaugler L C, Baumann E, Schutzius T M, Poulikakos D 2023 Nat. Phys. 19 649 Google Scholar
[39]	褚福强, 吴晓敏, 朱毅 2017 工程热 38 352 Chu F Q, Wu X M, Zhu Y 2017 J. Eng. Thermophys. 38 352
[40]	Chen R H, Phuoc T X, Martello D 2011 Int. J. Heat Mass Transfer 54 2459 Google Scholar
[41]	Bhuiyan M H U, Saidur R, Amalina M A, Mostafizur R M, Islam A 2015 Procedia Eng. 105 431 Google Scholar
[42]	Ahmadi S F, Nath S, Kingett C M, Yue P, Boreyko J B 2019 Nat. Commun. 10 2531 Google Scholar
[43]	Wang F, Chen L, Li Y Q, Huo P, Gu X, Hu M, Deng D S 2024 Phys. Rev. Lett. 132 014002 Google Scholar
[44]	Wang F, Zeng H, Du Y, Tang X, Sun C 2024 arXiv: 2407.20555v1 [physics. flu-dyn]
[45]	Moore M R, Mughal M S, Papageorgiou D T 2017 J. Fluid Mech. 817 455 Google Scholar
[46]	Thiévenaz V, Josserand C, Séon T 2020 Phys. Rev. Fluids 5 041601 Google Scholar
[47]	Schremb M, Campbell J M, Christenson H K, Tropea C 2017 Langmuir 33 4870 Google Scholar
[48]	Campbell J M, Sandnes B, Flekkøy E G, Måløy K J 2022 Cryst. Growth Des. 22 2433 Google Scholar
[49]	Babich A, Bashkatov A, Yang X, Mutschke G, Eckert K 2023 Int. J. Heat Mass Transfer 215 124466 Google Scholar
[50]	Tokgoz S, Geisler R, van Bokhoven L J A, Wieneke B 2012 Meas. Sci. Technol. 23 115302 Google Scholar
[51]	Zhang M K, Gao C, Ye B, Tang J C, Jiang B 2019 Cryobiology 86 47 Google Scholar
[52]	Li J Q, Rahman M, Patel S, Bogner R H, Fan T H 2022 Cryst. Growth Des. 22 6917 Google Scholar
[53]	Kurz W, Fisher D J 1992 Fundamentals of Solidification 5th Edition (Switzerland: Trans Tech Publication Ltd) pp56–59
[54]	Libbrecht K 2017 Annu. Rev. Mater. Res. 47 271 Google Scholar
[55]	Zhao Y, Guo Q, Lin T, Cheng P 2020 Int. J. Heat Mass Transfer 159 120074 Google Scholar
[56]	Lohse D, Zhang X 2020 Nat. Rev. Phys. 2 426 Google Scholar
[57]	Kitahata H, Yoshinaga N 2018 J. Chem. Physi. 148 134906 Google Scholar
[58]	Mullins W W, Sekerka R F 1964 J. Appl. Phys. 35 444 Google Scholar
[59]	Dehaoui A, Issenmann B, Caupin F 2015 Proc. Natl. Acad. Sci. 112 12020 Google Scholar
[60]	Pothoczki S, Pethes I, Pusztai L, Temleitner L, Csókás D, Kohara S, Ohara K, Bakó I 2021 J. Mol. Liq. 329 115592 Google Scholar

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Vol. 74, Issue 22 - 2025-11-20

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