Quantifying the Kinetic and Thermodynamic Origins of the Glass-Forming Ability in Metals
Abstract
The glass-forming ability (GFA) of a metallic liquid can be quantified by the critical cooling rate Rc, below which it crystallizes upon cooling. Rc is determined by the competition between R and the crystallization rate 𝒦X. Here, we calculate Rc and 𝒦X in model pure metals and alloys with BCC/B2 and FCC equilibrium crystal structures. Using classical nucleation theory and independently calculated crystal growth rates, we evaluate 𝒦X=(IU3)1/4 at T=0.8Tm, where I and U are the nucleation and growth rates and Tm is the melting temperature. We find a strong positive correlation between 𝒦X and Rc over eleven orders of magnitude. We decompose 𝒦X into a product of a kinetic contribution, involving atomic cluster attachment and diffusion, and a thermodynamic contribution. We show that the thermodynamic contribution to 𝒦X dominates the kinetic contribution over the range of cooling rates that we consider. The nucleation barrier ΔGc ∼ γ̃3/Δμ̃2, where γ̃ is the reduced effective liquid--crystal interfacial free energy and Δμ̃ is the reduced bulk driving force, determines the magnitude of the thermodynamic contribution. The relative importance of γ̃ and Δμ̃ depends on the material: a large interfacial free energy can suppress nucleation in some systems, whereas a weak bulk driving force can inhibit crystallization in others. Analyses of the structural and chemical order show that better glass formers have enhanced structural frustration, more icosahedral-like and less crystal-like local environments, and a larger chemical-order mismatch between the supercooled liquid and crystal phases.
Related
- Crystal forming ability of amorphous refractory metals under nanoindentation: a molecular dynamics study
- Thermodynamic origins of multimode spinodal decomposition in multicomponent alloys
- Topological and kinetic origins of fractional thermal conductance at the topological insulator--superconductor interface
- Transport coefficients in hard-sphere fluids: thermodynamic versus kinetic descriptions
- Kinetic heterogeneity tightens thermodynamic bounds on spectra of Markov cycles
BibTeX
@misc{jin2026quantifying,
title = {{Quantifying the Kinetic and Thermodynamic Origins of the Glass-Forming Ability in Metals}},
author = {Weiwei Jin and Jinpeng Fan and Mark D. Shattuck and Corey S. O'Hern},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.24101},
eprint = {2610.24101},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.24101},
note = {CC BY-NC-SA 4.0},
}
RIS
TY - UNPB
TI - Quantifying the Kinetic and Thermodynamic Origins of the Glass-Forming Ability in Metals
AU - Weiwei Jin
AU - Jinpeng Fan
AU - Mark D. Shattuck
AU - Corey S. O'Hern
PY - 2026
DA - 2026/10/16
PB - arXiv
DO - 10.48550/arxiv.2610.24101
UR - https://arxiv.org/abs/2610.24101
AB - The glass-forming ability (GFA) of a metallic liquid can be quantified by the critical cooling rate R_c, below which it crystallizes upon cooling. R_c is determined by the competition between R and the crystallization rate 𝒦_X. Here, we calculate R_c and 𝒦_X in model pure metals and alloys with BCC/B2 and FCC equilibrium crystal structures. Using classical nucleation theory and independently calculated crystal growth rates, we evaluate 𝒦_X=(IU^3)^1/4 at T=0.8T_m, where I and U are the nucleation and growth rates and T_m is the melting temperature. We find a strong positive correlation between 𝒦_X and R_c over eleven orders of magnitude. We decompose 𝒦_X into a product of a kinetic contribution, involving atomic cluster attachment and diffusion, and a thermodynamic contribution. We show that the thermodynamic contribution to 𝒦_X dominates the kinetic contribution over the range of cooling rates that we consider. The nucleation barrier ΔG_c ∼ γ̃^3/Δμ̃^2, where γ̃ is the reduced effective liquid--crystal interfacial free energy and Δμ̃ is the reduced bulk driving force, determines the magnitude of the thermodynamic contribution. The relative importance of γ̃ and Δμ̃ depends on the material: a large interfacial free energy can suppress nucleation in some systems, whereas a weak bulk driving force can inhibit crystallization in others. Analyses of the structural and chemical order show that better glass formers have enhanced structural frustration, more icosahedral-like and less crystal-like local environments, and a larger chemical-order mismatch between the supercooled liquid and crystal phases.
ER -