Multiphasic size-dependent growth dynamics of nanoparticle ensembles

• 成果类型: Article
• 署名作者: Kim, Ji- Hyun; Kim, Joodeok; Kim, Byung Hyo; Song, Sanggeun; Kang, Jingyu; Rhee, Jinho; Kim, Donghee; Chun, Hoje; Choi, Hyesung; Cho, Hyungjin; Kim, Yongjoon; Jung, Jae Won; Son, Youngju; Jung, Junhyeok; Park, Kunwoo; Jeon, Sungho; Lee, Minho; Han, Byungchan; Lee, Won Chul; Kim, Dongjun; Hyeon, Taeghwan; Sung, Jaeyoung; Park, Jungwon
• 署名单位: Chung Ang University; Chung Ang University; Chung Ang University; Institute for Basic Science - Korea (IBS); Seoul National University (SNU); Seoul National University (SNU); Soongsil University; University of California System; University of California Berkeley; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; Chung Ang University; Yonsei University; Hanyang University; Seoul National University (SNU); Seoul National University (SNU)
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-10114
• DOI: 10.1073/pnas.2424950122
• 发表日期: 2025-06-10
• 关键词: nanocrystal growth; homogeneous nucleation; bimolecular reactions; kinetics; mechanisms; microscopy; formalism; prospects

摘要

Colloidal nanoparticles are of great interest in modern science and industry. However, the thermodynamic mechanism and dynamics of nanoparticle growth have yet to be understood. Addressing these issues, we tracked hundreds of in-situ growth trajectories of a nanoparticle ensemble using liquid-phase TEM and found that the nanoparticle growth, including coalescence, exhibits nanoparticle size-dependent multiphasic dynamics, unexplainable by current theories. Motivated by this finding, we developed a model and theory for an ensemble of growing nanoparticles, providing a unified, quantitative understanding of the time-dependent mean and fluctuation of nanoparticle size and size-dependent growth rate profiles across various nanoparticle systems and experimental conditions. Our work reveals that the chemical potential in a small nanoparticle strongly deviates from the Gibbs-Thomson equation, shedding light on how it governs the size-dependent growth dynamics of nanoparticles.