Implementation of the Multigrid Gaussian-Plane-Wave Algorithm with GPU Acceleration in PySCF

This is the authors' abstract. We don't add key points for this paper.

We introduce a GPU-accelerated multigrid Gaussian-Plane-Wave density fitting (FFTDF) approach for efficient Fock builds and nuclear gradient evaluations within Kohn–Sham density functional theory, as implemented in the GPU4PySCF module of PySCF. Our CUDA kernels employ a grid-based parallelization strategy for contracting Gaussian basis function pairs and achieve 50% to 80% of the FP64 peak performance on NVIDIA GPUs, with no loss of efficiency for high angular momentum (up to f-shell) functions. Benchmark calculations on molecules and solids with up to 1536 atoms and 20480 basis functions show up to 25 × speedup on an H100 GPU relative to the CPU implementation on a 28-core shared-memory node. For a 256-water cluster, the ground-state energy and nuclear gradients can be computed in ∼30 seconds on a single H100 GPU. This implementation serves as an open-source foundation for many applications, such as ab initio molecular dynamics and high-throughput calculations.