Abstract
The rapid advancement of deep learning is reshaping the hardware design landscape toward AI tasks, posing fundamental challenges for HPC workloads such as atomistic simulation. Here we present SMC-AI, a general algorithmic framework that extends the SMC-X method for efficient canonical Monte Carlo simulation on AI accelerators, including GPUs and NPUs, while maintaining extreme scalability. The implementation of SMC-AI on an NPU cluster reaches unprecedented performance, achieving MC simulation of 4 trillion atoms on 4096 NPU dies. This represents the largest ML-accelerated atomistic simulation reported, delivering 32X system size and 1.3X throughput than previous records, with a relatively small computational budget. Excellent strong and weak scaling efficiency are reached for both the NPU and GPU implementation. By decoupling ML models from simulation, SMC-AI creates an abstraction that facilitates integration and porting of diverse ML models, laying a foundation for the future development of scalable scientific software.