Boron-assisted synthesis of compositionally complex amorphous oxides via short-range-order-constrained generative design

Abstract

Engineering short-range atomic order in amorphous materials offers a promising yet still underexplored route to high-performance solids. Here, we establish a boron-assisted amorphization strategy through ApolloX, a theory-guided, short-range-order-constrained generative framework for identifying low-energy amorphous configurations in compositionally complex multimetal BOx systems. Using FeCoNiMoBOx as a representative model platform, ApolloX predicts an ensemble of candidate amorphous configurations across systematically varied boron contents. Ab initio molecular dynamics simulations based on these configurations show that increasing boron content suppresses atomic diffusion and disfavors crystallization, with the stabilization of BO3-centered local motifs emerging as a key structural feature associated with enhanced amorphization propensity. Guided by these predictions, we synthesize three representative FeCoNiMoBOx compositions with distinct boron contents and use synchrotron-based scattering and electron microscopy to verify compositional fidelity, structural homogeneity, and the targeted amorphous features, thereby experimentally validating the boron-regulated structural evolution predicted by theory. Beyond this representative system, the same strategy is extended to a broader library of multimetal BOx amorphous compositions spanning diverse metal combinations and boron loadings, demonstrating that the boron-assisted route is not limited to a single FeCoNiMoBOx family but is broadly transferable across compositionally complex amorphous oxides. Overall, our results establish boron incorporation as a practical design variable for tuning short-range order and amorphization in multicomponent oxides, and provide a general framework for the theory-guided discovery of compositionally complex amorphous materials with tunable properties.