Journal: PNAS 122.23 (2025): e2424950122.
Author: Ji-Hyun Kima,b,c,1, Joodeok Kimd,e,1, Byung Hyo Kimd,e,f,1, Sanggeun Songg,h,1, Jingyu Kanga,b,c,i, Jinho Rheed,e, Donghee Kima,b,c,i, Hoje Chunj, Hyesung Choid,e, Hyungjin Chof, Yongjoon Kimf, Jae Won Jungf, Youngju Sohnd,e, Junhyeok Jungd,e, Kunwoo Parkd,e, Sungho Jeonk, Minho Leea,b,c,i, Byungchan Hanj, Won Chul Leek, Dongjun Kimd,e,
Taeghwan Hyeond,e,2, Jaeyoung Sunga,b,c,i,2, Jungwon Parkd,e,l,m,2
a Global Science Research Center for Systems Chemistry, Chung-Ang University; Seoul 06974, Republic of Korea.
b Creative Research Initiative Center for Chemical Dynamics in Living Cells, Chung-Ang University; Seoul 06974, Republic of Korea.
c Department of Chemistry, Chung-Ang University; Seoul 06974, Republic of Korea.
d Center for Nanoparticle Research, Institute for Basic Science (IBS); Seoul 08826, Republic of Korea.
e School of Chemical and Biological Engineering, and Institute of Chemical Process, Seoul National University; Seoul 08826, Republic of Korea.
f Department of Materials Science and Engineering, Soongsil University; Seoul 06978, Republic of Korea.
g Department of Chemical and Biomolecular Engineering, University of California, Berkeley, Berkeley, California 94720, USA.
h Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
i National Institute of Innovative Functional Imaging, Chung-Ang University; Seoul 06974, Republic of Korea.
j Department of Chemical and Biomolecular Engineering, Yonsei University; Seoul 03722, Republic of Korea.
k Department of Mechanical Engineering, BK21 FOUR ERICA-ACE Center, Hanyang University; Ansan, Gyeonggi 15588, Republic of Korea.
l Institute of Engineering Research, College of Engineering, Seoul National University; Seoul 08826, Republic of Korea.
m Advanced Institute of Convergence Technology, Seoul National University; Suwon, Gyeonggi 16229, Republic of Korea.
1 These authors contributed equally to this work.
2 Correspondence regarding experiment should be addressed to jungwonpark@snu.ac.kr (J.P.) and thyeon@snu.ac.kr (T.H.); Correspondence regarding theory should be addressed to jaeyoung@cau.ac.kr (J.S.)
DOI: https://doi.org/10.1073/pnas.2424950122
Colloidal nanoparticles are of great interest in modern science and industry. However, 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 discovered that the nanoparticle growth, including coalescence, exhibits nanoparticle size-dependent multiphasic dynamics, unexplainable by current theories. Motivated by this finding, we developed a new 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.