Conditional Generative Models Enable Targeted Exploration of MAX Phase Design Space

Abstract

MAX phases (M${}_{n+1}$AX${}_n$), precursors to MXenes, span a vast compositional space, motivating efficient computational screening for synthesisable candidates. We employ CrystaLLM$-\ddot{I}€$, a large language model fine-tuned on 6,179 double transition-metal MAX phases, and demonstrate its ability to generate out-of-sample structures consistent with known experimental trends. Using a conditioning vector with two dimensions (a statistically derived MXene derivative count and a surrogate for A-site binding energy), the model was able to target MXene-favourable regions of phase space for generation. Specific condition vectors double novel stable structure generation rates versus unconditioned baselines. Of ten compositionally novel candidates, five exhibit DFT-validated stability ($E_{hull}<0.050$ eV/atom). This work showcases the potential for autoregressive generative models to explore targeted materials' spaces, offering a scalable framework for accelerated discovery in compositionally complex systems.