Adaptable Method for Crystal Design across Diverse Constraints and Objectives with Pretrained Property Predictors

Abstract

Advanced crystal design can accelerate materials discovery across applications from photovoltaics to spintronics. Practical design must satisfy multiple properties and physical constraints, yet existing machine-learning-based approaches to such design often depend on large datasets, retraining, or task-specific generators. Here, we show that direct predictor-guided gradient optimization enables data-efficient, constraint-rich crystal design by combining off-the-shelf predictors with site-wise element masks, template initialization, and task-specific losses. In perovskites, it outperformed generative and Bayesian baselines under three targets -- band gap, formation energy, and tolerance factor -- and two hard constraints. DFT assessment further showed band-gap targeting competitive with a leading generative model despite using predictors trained on roughly one-tenth of the data. By flexibly combining pretrained predictors with application-oriented masks and custom losses, the same framework supported half-metal design. Such modularity could help researchers and engineers translate diverse application requirements directly into optimized candidate crystals with minimal computational cost.