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.
@article{arxiv.2202.01255,
title = {Large scale quantum chemistry with Tensor Processing Units},
author = {Ryan Pederson and John Kozlowski and Ruyi Song and Jackson Beall and Martin Ganahl and Markus Hauru and Adam G. M. Lewis and Yi Yao and Shrestha Basu Mallick and Volker Blum and Guifre Vidal},
journal= {arXiv preprint arXiv:2202.01255},
year = {2022}
}