Liquid anomalies and fragility of supercooled antimony

• 成果类型: Article
• 署名作者: Giuliani, Flavio; Mattioli, Francesco Guidarelli; Chen, Yuhan; Baratella, Dario; Dragoni, Daniele; Bernasconi, Marco; Russo, John; Boeri, Lilia; Mazzarello, Riccardo
• 署名单位: Sapienza University Rome; University of Milano-Bicocca
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-8424; 1091-6490
• DOI: 10.1073/pnas.2531605123
• 发表日期: 2026-03-24
• 页码: e2531605123
• 关键词: monoatomic phase-change memories; neuromorphic computing; SUPERCOOLED LIQUIDS; fragility; liquid-liquid transition; PHASE-CHANGE MATERIALS; CRYSTALLIZATION KINETICS; TRANSITION; viscosity; crystal; water; ORDER; MODEL

摘要

Phase-change materials (PCMs) based on group IV, V, and VI elements, such as Ge, Sb, and Te, exhibit distinctive liquid-state features, including thermodynamic anomalies and unusual dynamical properties, which are believed to play a key role in their fast and reversible crystallization behavior. Antimony (Sb), a monoatomic PCM with ultrafast switching capabilities, stands out as the only elemental member of this group for which the properties of the liquid and supercooled states have so far remained unknown. In this work, we use large-scale molecular dynamics simulations with a neural network potential trained on first-principles data to investigate the liquid, supercooled, and amorphous phases of Sb across a broad pressure-temperature range. We uncover clear signatures of anomalous behavior, including a density maximum and nonmonotonic thermodynamic response functions, which are described by a two-state model based on the structural evolution of the liquid. Moreover, extrapolation of the viscosity to the glass transition, based on configurational and excess entropies, indicates that Sb is a highly fragile material. Our results present a compelling case for the connection between the liquid-state properties of PCMs and their unique ability to combine high amorphous-phase stability with ultrafast crystallization.