Abstract

Experimental study of the atomic mechanism in melting and freezing processes remains a formidable challenge. We report herein on a unique material system that allows for in situ growth of bismuth nanoparticles from the precursor compound SrBi2Ta2O9 under an electron beam within a high-resolution transmission electron microscope (HRTEM). Simultaneously, the melting and freezing processes within the nanoparticles are triggered and imaged in real time by the HRTEM. The images show atomic-scale evidence for point defect induced melting, and a freezing mechanism mediated by crystallization of an intermediate ordered liquid. During the melting and freezing, the formation of nucleation precursors, nucleation and growth, and the relaxation of the system, are directly observed. Based on these observations, an interaction–relaxation model is developed towards understanding the microscopic mechanism of the phase transitions, highlighting the importance of cooperative multiscale processes.

Highlights

  • Experimental study of the atomic mechanism in melting and freezing processes remains a formidable challenge

  • Based on the direct observations, we prove that the two opposite processes of melting and freezing are controlled by the interaction–relaxation model, which might provide guidance for future theoretical investigation and for better control of the dynamics of the phase transition

  • The observed trajectories highlight the unique contributions of premelting/prefreezing states, which helps improve the understanding of microscopic mechanism of the phase transitions

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Summary

Introduction

Experimental study of the atomic mechanism in melting and freezing processes remains a formidable challenge. During the melting and freezing, the formation of nucleation precursors, nucleation and growth, and the relaxation of the system, are directly observed Based on these observations, an interaction–relaxation model is developed towards understanding the microscopic mechanism of the phase transitions, highlighting the importance of cooperative multiscale processes. Such large discrepancies highlight the need for more precise and detailed experimental results to justify the theoretical models and to further our understanding of the melting and freezing processes Experimentally studying these microscopic mechanisms remains a significant technical challenge as it demands an experimental system that enables manipulation between different phases, and allows for in situ imaging of the atomic structural change during phase transition. Based on the direct observations, we prove that the two opposite processes of melting and freezing are controlled by the interaction–relaxation model, which might provide guidance for future theoretical investigation and for better control of the dynamics of the phase transition

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