Asymmetric Energy Landscapes Control Diffusion in Glasses
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arXiv
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| Autores principales: | , , , , |
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| Formato: | Preprint |
| Publicado: |
2026
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| _version_ | 1866914408614068224 |
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| author | Annamareddy, Ajay Wang, Bu Voyles, Paul M. Szlufarska, Izabela Morgan, Dane |
| author_facet | Annamareddy, Ajay Wang, Bu Voyles, Paul M. Szlufarska, Izabela Morgan, Dane |
| contents | While diffusion in crystalline solids is quantitatively understood through defect-mediated atomic hops, no comparable quantitative framework exists for glasses. In these systems, the origin of large diffusion activation energies remains puzzling, despite local rearrangements involving low barriers. Using molecular dynamics simulations of metallic glasses, we decompose diffusion into random-walk and correlation contributions and find that back-and-forth correlated motion, not local rearrangement barriers, dominates the activation energy, resolving how low-barrier rearrangements yield large macroscopic activation energies. These correlations arise from asymmetry between forward and reverse barriers, a generic feature of disordered energy landscapes. We find that the correlation-driven mechanism is active beyond metallic glass alloys, including SiO2 and a single-component Lennard-Jones glass. The latter demonstrates that the correlation originates from structural disorder rather than chemical complexity. The framework also explains accelerated surface diffusion, where reduced activation energies arise primarily from weaker correlations rather than changes in local rearrangement barriers. Our results establish a direct, quantitative link between atomic-scale dynamics and macroscopic transport, providing a predictive basis for kinetics in disordered materials. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2603_18317 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Asymmetric Energy Landscapes Control Diffusion in Glasses Annamareddy, Ajay Wang, Bu Voyles, Paul M. Szlufarska, Izabela Morgan, Dane Materials Science Disordered Systems and Neural Networks Statistical Mechanics While diffusion in crystalline solids is quantitatively understood through defect-mediated atomic hops, no comparable quantitative framework exists for glasses. In these systems, the origin of large diffusion activation energies remains puzzling, despite local rearrangements involving low barriers. Using molecular dynamics simulations of metallic glasses, we decompose diffusion into random-walk and correlation contributions and find that back-and-forth correlated motion, not local rearrangement barriers, dominates the activation energy, resolving how low-barrier rearrangements yield large macroscopic activation energies. These correlations arise from asymmetry between forward and reverse barriers, a generic feature of disordered energy landscapes. We find that the correlation-driven mechanism is active beyond metallic glass alloys, including SiO2 and a single-component Lennard-Jones glass. The latter demonstrates that the correlation originates from structural disorder rather than chemical complexity. The framework also explains accelerated surface diffusion, where reduced activation energies arise primarily from weaker correlations rather than changes in local rearrangement barriers. Our results establish a direct, quantitative link between atomic-scale dynamics and macroscopic transport, providing a predictive basis for kinetics in disordered materials. |
| title | Asymmetric Energy Landscapes Control Diffusion in Glasses |
| topic | Materials Science Disordered Systems and Neural Networks Statistical Mechanics |
| url | https://arxiv.org/abs/2603.18317 |