First-principles transition-state tensorial cluster expansion of vacancy diffusion in Ta-W beyond the kinetically-resolved activation approximation
Abstract
Predicting diffusion in chemically complex alloys remains challenging due to the strong dependence of migration barriers on local atomic environments. Migration barriers computed using density functional theory and nudged elastic band calculations are represented via a tensorial cluster expansion including transition states and deployed in on-lattice kinetic Monte Carlo simulations. Applied to the Ta-W system, the framework captures nontrivial composition-dependent diffusion behavior arising from a crossover between solute trapping and percolated low-barrier transport pathways, yielding a maximum in the apparent activation energy near intermediate compositions. This approach establishes a general and scalable route for integrating first-principles transition-state energetics into mesoscale kinetic simulations, enabling predictive multiscale modeling of diffusion in chemically complex materials and providing a pathway for uncovering emergent transport phenomena.
Versions
Related
- Unbiased first-principles construction of complete tensorial spin Hamiltonians
- Localization Transition in Kinetically Deformed one-dimensional Aubry-André Model
- First-Principles Investigation of Ammonia Adsorption and N-H Activation on W-B Nanoclusters
- Pressure-Induced Phase Transition and Superconducting Properties of LiPdH2: A First-Principles Study
- Anisotropic electrical and thermal conductivity of TiH₂ across its crystalline phase transition: A first-principles study
BibTeX
@misc{jeffries2026firstprinciples,
title = {{First-principles transition-state tensorial cluster expansion of vacancy diffusion in Ta-W beyond the kinetically-resolved activation approximation}},
author = {Jacob Jeffries and Brianna Sebastian-Olazabal and Enrique Martinez},
howpublished = {arXiv},
year = {2026},
month = jun,
doi = {10.48550/arxiv.2605.23612},
eprint = {2605.23612},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2605.23612},
note = {CC BY-NC-ND 4.0},
}
RIS
TY - UNPB
TI - First-principles transition-state tensorial cluster expansion of vacancy diffusion in Ta-W beyond the kinetically-resolved activation approximation
AU - Jacob Jeffries
AU - Brianna Sebastian-Olazabal
AU - Enrique Martinez
PY - 2026
DA - 2026/06/05
PB - arXiv
DO - 10.48550/arxiv.2605.23612
UR - https://arxiv.org/abs/2605.23612
AB - Predicting diffusion in chemically complex alloys remains challenging due to the strong dependence of migration barriers on local atomic environments. Migration barriers computed using density functional theory and nudged elastic band calculations are represented via a tensorial cluster expansion including transition states and deployed in on-lattice kinetic Monte Carlo simulations. Applied to the Ta-W system, the framework captures nontrivial composition-dependent diffusion behavior arising from a crossover between solute trapping and percolated low-barrier transport pathways, yielding a maximum in the apparent activation energy near intermediate compositions. This approach establishes a general and scalable route for integrating first-principles transition-state energetics into mesoscale kinetic simulations, enabling predictive multiscale modeling of diffusion in chemically complex materials and providing a pathway for uncovering emergent transport phenomena.
ER -