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Abstract Physical unclonable functions (PUFs) are emerging as an alternative to information security by providing an advanced level of cryptographic keys with non‐replicable characteristics, yet the cryptographic keys of conventional PUFs are not reconfigurable from the ones assigned at the manufacturing stage and the overall authentication process slows down as the number of entities in the dataset or the length of cryptographic key increases. Herein, a supersaturated solution‐based PUF (S‐PUF) is presented that utilizes stochastic crystallization of a supersaturated sodium acetate solution to allow a time‐efficient, hierarchical authentication process together with on‐demand rewritability of cryptographic keys. By controlling the orientation and the average grain size of the sodium acetate crystals via a spatiotemporally programmed temperature profile, the S‐PUF now includes two global parameters, that is, angle of rotation and divergence of the diffracted beam, in addition to the speckle pattern to produce multilevel cryptographic keys, and these parameters function as prefixes for the classification of each entity for a fast authentication process. At the same time, the reversible phase change of sodium acetate enables repeated reconfiguration of the cryptographic key, which is expected to offer new possibilities for a next‐generation, recyclable anti‐counterfeiting platform. 

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.