Generative Inversion of Spectroscopic Data for Amorphous Structure Elucidation

Abstract

Determining atomistic structures from characterization data is one of the most common yet intricate problems in materials science. Particularly in amorphous materials, proposing structures that balance realism and agreement with experiments requires expert guidance, good interatomic potentials, or both. Here, we introduce GLASS, a generative framework that inverts multi-modal spectroscopic measurements into realistic atomistic structures without knowledge of the potential energy surface. A score-based model learns a structural prior from low-fidelity data and samples out-of-distribution structures conditioned on differentiable spectral targets. Reconstructions using pair distribution functions (PDFs), X-ray absorption spectroscopy, and diffraction measurements quantify the complementarity between spectral modalities and demonstrate that PDFs is the most informative probe for our framework. We use GLASS to rationalize three contested experimental problems: paracrystallinity in amorphous silicon, a liquid-liquid phase transition in sulfur, and ball-milled amorphous ice. In each case, generated structures reproduce experimental measurements and reveal mechanisms inaccessible to diffraction analysis alone.