On the Role of Atomic Mobility in the Polyamorphism of Metallic Glasses
Abstract
Understanding the microscopic mechanisms underlying polyamorphic transitions requires simultaneous knowledge of thermodynamic and structural evolution, which has remained experimentally inaccessible. Here, we combine chip-based fast differential scanning calorimetry with high-energy synchrotron X-ray diffraction to simultaneously probe the thermodynamic and structural evolution during the polyamorphic transition of a Pd-Ni-P metallic glass. Correlating heat-flow signals with the corresponding structural evolution during both heating and cooling reveals a direct relationship between thermodynamic evolution and medium-range structural ordering. Based on this relationship, we identify two distinct transition mechanisms. In the glassy state, the transition proceeds continuously through progressive medium-range ordering, accompanied by enhanced thermal stability and strongly temperature-dependent kinetics. In contrast, in the equilibrium supercooled liquid, the transition proceeds through the coexistence of distinct amorphous states, with only a weak temperature dependence of the kinetics. These findings show that atomic mobility governs the transformation pathway by coupling thermodynamic evolution to structural ordering, providing new insights into polyamorphic transitions in nonequilibrium amorphous systems.
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BibTeX
@misc{shen2026role,
title = {{On the Role of Atomic Mobility in the Polyamorphism of Metallic Glasses}},
author = {Jie Shen and Antoine Cornet and Pei-Hao Sun and Valerio Di Lisio and Daniele Cangialosi and Klara Otto and Isabella Gallino and Martin Rosenthal and Eloi Pineda and Giulio Monaco and Marco Di Michiel and Yong-Hao Sun and Wei-Hua Wang and Ruta Beatrice},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.32434},
eprint = {2610.32434},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.32434},
note = {CC0},
}
RIS
TY - UNPB
TI - On the Role of Atomic Mobility in the Polyamorphism of Metallic Glasses
AU - Jie Shen
AU - Antoine Cornet
AU - Pei-Hao Sun
AU - Valerio Di Lisio
AU - Daniele Cangialosi
AU - Klara Otto
AU - Isabella Gallino
AU - Martin Rosenthal
AU - Eloi Pineda
AU - Giulio Monaco
AU - Marco Di Michiel
AU - Yong-Hao Sun
AU - Wei-Hua Wang
AU - Ruta Beatrice
PY - 2026
DA - 2026/10/23
PB - arXiv
DO - 10.48550/arxiv.2610.32434
UR - https://arxiv.org/abs/2610.32434
AB - Understanding the microscopic mechanisms underlying polyamorphic transitions requires simultaneous knowledge of thermodynamic and structural evolution, which has remained experimentally inaccessible. Here, we combine chip-based fast differential scanning calorimetry with high-energy synchrotron X-ray diffraction to simultaneously probe the thermodynamic and structural evolution during the polyamorphic transition of a Pd-Ni-P metallic glass. Correlating heat-flow signals with the corresponding structural evolution during both heating and cooling reveals a direct relationship between thermodynamic evolution and medium-range structural ordering. Based on this relationship, we identify two distinct transition mechanisms. In the glassy state, the transition proceeds continuously through progressive medium-range ordering, accompanied by enhanced thermal stability and strongly temperature-dependent kinetics. In contrast, in the equilibrium supercooled liquid, the transition proceeds through the coexistence of distinct amorphous states, with only a weak temperature dependence of the kinetics. These findings show that atomic mobility governs the transformation pathway by coupling thermodynamic evolution to structural ordering, providing new insights into polyamorphic transitions in nonequilibrium amorphous systems.
ER -