Large scale quantum chemistry with Tensor Processing Units

Abstract

We demonstrate the use of Google's cloud-based Tensor Processing Units (TPUs) to accelerate and scale up conventional (cubic-scaling) density functional theory (DFT) calculations. Utilizing 512 TPU cores, we accomplish the largest such DFT computation to date, with 247848 orbitals, corresponding to a cluster of 10327 water molecules with 103270 electrons, all treated explicitly. Our work thus paves the way towards accessible and systematic use of conventional DFT, free of any system-specific constraints, at unprecedented scales.

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• Self-Supervised Generative Models for Crystal Structures
• Subspace recursive Fermi-operator expansion strategies for large-scale DFT eigenvalue problems on HPC architectures