A Hierarchical Synergistic Deep Learning Framework Integrating Composition, Structure, and Ionic Transport for Solid-State Electrolyte Discovery

Abstract:Inorganic solid-state electrolytes must combine high room-temperature ionic conductivity, a wide electrochemical window, excellent electronic insulation, and favorable mechanical compliance. Single models struggle to support reliable multi-objective screening across vast chemical spaces because of training-data distribution mismatch, cross-property dataset heterogeneity, and scarce kinetic transport data. To overcome these limitations, we develop a hierarchical synergistic deep-learning framework that sequentially coordinates efficiency, accuracy, and reliability through four complementary modules. The in-house-developed L-G-DCNN and a multi-fidelity implementation built on DenseGNN serve as compositional and structural experts for thermodynamic coarse screening and multi-property evaluation, respectively; MatterSim and system-specific DeePMD models provide transport pre-assessment and kinetic validation. Systematic benchmarks show that each module outperforms mainstream counterparts in its task, while retrospective validation establishes dual closed-loop verification of module-level accuracy and end-to-end workflow reliability. Applied to 30,364,908 Alex/ICSD-derived candidates, the framework identifies 97 high-performance candidates with room-temperature ionic conductivities of 0.109--59.0 mS/cm, including 94 halides, one borohydride, and two oxides. Consistency with independent experimental data confirms that 76 of the 94 halides fall within reported high-conductivity structural regions. Analysis reveals that Li$^{+}$ jump-network connectivity, rather than the number of geometric Li sites, is the core determinant of room-temperature ionic conductivity. Li-defect engineering effectively enhances oxide transport, whereas the inherent rigidity of the O$^{2-}$ framework suggests a potential upper limit on oxide electrolyte performance.

Materials Science (cond-mat.mtrl-sci); Artificial Intelligence (cs.AI); Machine Learning (cs.LG)

arXiv:2608.25592 [cond-mat.mtrl-sci]

(or arXiv:2608.25592v1 [cond-mat.mtrl-sci] for this version)

https://doi.org/10.48550/arXiv.2608.25592 Focus to learn more arXiv-issued DOI via DataCite (pending registration)

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