Distributed Implementation of Full Configuration Interaction for One Trillion Determinants.

Abstract

Full configuration interaction (FCI) can provide an exact molecular ground-state energy within a given basis set and serve as a benchmark for approximate methods in quantum chemical calculations, including the emerging variational quantum eigensolver. However, its exponential computational and memory requirements easily exceed the capability of a single server and limit its applicability to large molecules. In this paper, we present a distributed FCI implementation employing a hybrid parallelization scheme with multithreading and multiprocessing to expand FCI's applicability. We optimize this scheme to minimize the bottlenecks arising from interprocess communications and interthread data management. Our implementation achieves higher scalability than the naive combination of prior works and successfully calculates the exact energy of C3H8/STO-3G with 1.31 trillion determinants, which is the largest FCI calculation to the best of our knowledge. Furthermore, we provide a comprehensive list of FCI results with 136 combinations of molecules and basis sets for future evaluation and development of approximate methods.