Supersaturation, Nucleation, and Phase Separation of Mesoscopic Systems

Supersaturation, nucleation, and phase separation are ubiquitous phenomena of great interest in both science and industry. However, a unified, quantitative understanding of these phenomena has yet to be achieved for mesoscopic systems. Here, we present a set of general equations that determine the monomer saturation degree, the size distribution, and the free energy of mesoscopic systems, as well as their phase-transition conditions. These equations reveal that, under supersaturation, the largest cluster size (LCS) is an important state variable; the supersaturation degree decreases with the LCS, approaching unity in the macroscopic limit. We identify the critical supersaturation, at which the nuclei undergo the phase transition to form large crystals. Below this critical supersaturation, the nucleus size distribution is either a unimodal function or a monotonically decreasing function of size, depending on the system and temperature. We also predict the most probable nucleus size and the direction of spontaneous changes of the LCS. Our theory provides a unified, quantitative explanation of the nucleus-size-distribution across six different systems, including nanoparticles and biological condensates. This work serves as a general theoretical framework useful for understanding and designing nucleation and phase transitions of mesoscopic systems.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2025-12-03
DOI
https://doi.org/10.1021/jacs.5c10868
Primary Topic
nanoparticles nucleation surface interactions
Type
article
Field-Weighted Citation Impact
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article

Supersaturation, Nucleation, and Phase Separation of Mesoscopic Systems

Jaeyoung Sung, Donghee Kim, Jingyu Kang, Sanggeun Song et al.
Journal of the American Chemical Society
nanoparticles nucleation surface interactions
article

Supersaturation, Nucleation, and Phase Separation of Mesoscopic Systems

Jaeyoung Sung, Donghee Kim, Jingyu Kang, Sanggeun Song, Taeghwan Hyeon, Yongwon Jung, Joonkyung Jang, Sungjee Kim, Byung Hyo Kim, Mino Yang, Jeong‐Mo Choi, Sangwoon Yoon, Ji‐Hyun Kim, Jungwon Park, Jonghwa Han, Youngjae Ryu
article en

Abstract

Supersaturation, nucleation, and phase separation are ubiquitous phenomena of great interest in both science and industry. However, a unified, quantitative understanding of these phenomena has yet to be achieved for mesoscopic systems. Here, we present a set of general equations that determine the monomer saturation degree, the size distribution, and the free energy of mesoscopic systems, as well as their phase-transition conditions. These equations reveal that, under supersaturation, the largest cluster size (LCS) is an important state variable; the supersaturation degree decreases with the LCS, approaching unity in the macroscopic limit. We identify the critical supersaturation, at which the nuclei undergo the phase transition to form large crystals. Below this critical supersaturation, the nucleus size distribution is either a unimodal function or a monotonically decreasing function of size, depending on the system and temperature. We also predict the most probable nucleus size and the direction of spontaneous changes of the LCS. Our theory provides a unified, quantitative explanation of the nucleus-size-distribution across six different systems, including nanoparticles and biological condensates. This work serves as a general theoretical framework useful for understanding and designing nucleation and phase transitions of mesoscopic systems.

Journal of the American Chemical SocietyVol. 147(51)
Pohang University of Science and Technology (KR), Seoul National University (KR), Soongsil University (KR), Lawrence Berkeley National Laboratory (US), Korea Advanced Institute of Science and Technology (KR), Chungbuk National University (KR), National University (SD), Creative Research (GB), Institute for Basic Science (KR), Advanced Institute of Convergence Technology (KR), Center for Global Health (US), NOAA Chemical Sciences Laboratory (US), State Research Institute of Mechanical Engineering (RU), Pusan National University (KR), Chung-Ang University (KR), University of California, Berkeley (US)
Openalex Percentile: Top 58%
nanoparticles nucleation surface interactions
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