Critical role of phase-dependent properties in modeling photothermal sintering of LiCoO2 cathodes

Fuente: arXiv
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Main Authors: Hu, Yang, Sklénard, Benoit, Vels, Wouter, Romanyuk, Yaroslav E., Turlo, Vladyslav
Format: Preprint
Published: 2026
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author Hu, Yang
Sklénard, Benoit
Vels, Wouter
Romanyuk, Yaroslav E.
Turlo, Vladyslav
author_facet Hu, Yang
Sklénard, Benoit
Vels, Wouter
Romanyuk, Yaroslav E.
Turlo, Vladyslav
contents Photothermal (photonic) sintering crystallizes as-deposited amorphous LiCoO2 (LCO) cathodes for solid-state thin-film batteries using millisecond, surface-localized heating. However, process design often relies on 1D models with phase-averaged, temperature-independent properties, which can mispredict peak temperatures and thermal damage margins. Here we develop a multiscale, data-driven framework that provides phase- and grain size-resolved thermophysical inputs for stoichiometric LCO. We train an Allegro neural network potential with near-ab initio accuracy, enabling Green-Kubo calculations of thermal conductivity for crystalline and amorphous phases. The low, weakly density-dependent conductivity of amorphous LCO motivates its use as an effective intergranular phase in a thin-interface model that reproduces observed grain-size-dependent thermal transport. Combined with measured wavelength-resolved optical properties in 1D multiphysics simulations, we show amorphous LCO absorbs more strongly and reaches higher peak temperatures than crystalline LCO; thus crystalline, constant-property models systematically overestimate safe operating windows.
format Preprint
id arxiv_https___arxiv_org_abs_2604_21842
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Critical role of phase-dependent properties in modeling photothermal sintering of LiCoO2 cathodes
Hu, Yang
Sklénard, Benoit
Vels, Wouter
Romanyuk, Yaroslav E.
Turlo, Vladyslav
Materials Science
Photothermal (photonic) sintering crystallizes as-deposited amorphous LiCoO2 (LCO) cathodes for solid-state thin-film batteries using millisecond, surface-localized heating. However, process design often relies on 1D models with phase-averaged, temperature-independent properties, which can mispredict peak temperatures and thermal damage margins. Here we develop a multiscale, data-driven framework that provides phase- and grain size-resolved thermophysical inputs for stoichiometric LCO. We train an Allegro neural network potential with near-ab initio accuracy, enabling Green-Kubo calculations of thermal conductivity for crystalline and amorphous phases. The low, weakly density-dependent conductivity of amorphous LCO motivates its use as an effective intergranular phase in a thin-interface model that reproduces observed grain-size-dependent thermal transport. Combined with measured wavelength-resolved optical properties in 1D multiphysics simulations, we show amorphous LCO absorbs more strongly and reaches higher peak temperatures than crystalline LCO; thus crystalline, constant-property models systematically overestimate safe operating windows.
title Critical role of phase-dependent properties in modeling photothermal sintering of LiCoO2 cathodes
topic Materials Science
url https://arxiv.org/abs/2604.21842