Reversible disorder-order transitions in atomic crystal nucleation

Sungho Jeon, Taeyeong Heo, Sang Yeon Hwang, Jim Ciston, Karen C. Bustillo, Bryan W. Reed, Jimin Ham, Sungsu Kang, Sungin Kim, Joowon Lim, Kitaek Lim, Ji Soo Kim, Min Ho Kang, Ruth S. Bloom, Sukjoon Hong, Kwanpyo Kim, Alex Zettl, Woo Youn Kim, Peter Ercius, Jungwon ParkWon Chul Lee

Research output: Contribution to journalArticlepeer-review

1 Citation (Scopus)

Abstract

Nucleation in atomic crystallization remains poorly understood, despite advances in classical nucleation theory. The nucleation process has been described to involve a nonclassical mechanism that includes a spontaneous transition from disordered to crystalline states, but a detailed understanding of dynamics requires further investigation. In situ electron microscopy of heterogeneous nucleation of individual gold nanocrystals with millisecond temporal resolution shows that the early stage of atomic crystallization proceeds through dynamic structural fluctuations between disordered and crystalline states, rather than through a single irreversible transition. Our experimental and theoretical analyses support the idea that structural fluctuations originate from size-dependent thermodynamic stability of the two states in atomic clusters. These findings, based on dynamics in a real atomic system, reshape and improve our understanding of nucleation mechanisms in atomic crystallization.

Original languageEnglish
Article numberaaz7555
JournalScience
Volume371
Issue number6528
DOIs
Publication statusPublished - 2021 Jan 29

Bibliographical note

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© 2021 American Association for the Advancement of Science. All rights reserved.

All Science Journal Classification (ASJC) codes

  • General

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