Integrating electronic structure into generative modeling of inorganic materials

Abstract: Recent advances in generative models have introduced a new paradigm for the inverse design of inorganic materials, enabling the discovery of new crystalline structures with desired properties. However, existing generative models focus solely on structural aspects of materials during generation, while overlooking the underlying electronic behavior that fundamentally governs materials' stability and functionality. In this work, we present ChargeDIFF, the first generative model for inorganic materials that explicitly incorporates electronic structure into the generation process. Specifically, ChargeDIFF leverages charge density, a direct spatial representation of a material's electronic structure, as an additional modality for generation. ChargeDIFF demonstrates exceptional performance in both unconditional and conditional generation tasks compared to baseline models, with ablation studies revealing that this improvement is directly due to its ability to capture the material's electronic structure during generation. Moreover, the ability to control charge density during generation allows ChargeDIFF to introduce a novel inverse design method based on three-dimensional charge density, illustrating the potential to generate lithium-ion battery cathode materials with desired ion migration pathways, as validated by physics-based simulations. By highlighting the importance of accounting for electronic characteristics during material generation, ChargeDIFF offers new possibilities in the generative design of stable and functional materials.