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Reversible disorder-order transitions in atomic crystal nucleation.

Sungho JeonTaeyeong HeoSang-Yeon HwangJim CistonKaren C BustilloBryan W ReedJimin HamSungsu KangSungin KimJoowon LimKitaek LimJi Soo KimMin-Ho KangRuth S BloomSukjoon HongKwanpyo KimAlex ZettlWoo Youn KimPeter ErciusJungwon ParkWon Chul Lee
Published in: Science (New York, N.Y.) (2021)
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.
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