Toward an extreme-scale electronic structure system

Jorge L. Galvez Vallejo, Calum Snowdon, Ryan Stocks, Fazeleh Kazemian, Fiona Chuo Yan Yu, Christopher Seidl, Zoe Seeger, Melisa Alkan, David Poole, Bryce M. Westheimer, Mehaboob Basha, Marco De La Pierre, Alistair Rendell, Ekaterina I. Izgorodina, Mark S. Gordon, Giuseppe M.J. Barca

Research output: Contribution to journalArticlepeer-review


Electronic structure calculations have the potential to predict key matter transformations for applications of strategic technological importance, from drug discovery to material science and catalysis. However, a predictive physicochemical characterization of these processes often requires accurate quantum chemical modeling of complex molecular systems with hundreds to thousands of atoms. Due to the computationally demanding nature of electronic structure calculations and the complexity of modern high-performance computing hardware, quantum chemistry software has historically failed to operate at such large molecular scales with accuracy and speed that are useful in practice. In this paper, novel algorithms and software are presented that enable extreme-scale quantum chemistry capabilities with particular emphasis on exascale calculations. This includes the development and application of the multi-Graphics Processing Unit (GPU) library LibCChem 2.0 as part of the General Atomic and Molecular Electronic Structure System package and of the standalone Extreme-scale Electronic Structure System (EXESS), designed from the ground up for scaling on thousands of GPUs to perform high-performance accurate quantum chemistry calculations at unprecedented speed and molecular scales. Among various results, we report that the EXESS implementation enables Hartree-Fock/cc-pVDZ plus RI-MP2/cc-pVDZ/cc-pVDZ-RIFIT calculations on an ionic liquid system with 623 016 electrons and 146 592 atoms in less than 45 min using 27 600 GPUs on the Summit supercomputer with a 94.6% parallel efficiency.

Original languageEnglish
Article number044112
Number of pages24
JournalJournal of Chemical Physics
Issue number4
Early online date27 Jul 2023
Publication statusPublished - 28 Jul 2023


  • Quantum chemistry
  • Moller-Plesset perturbation theory
  • Electronic structure
  • Correlation-consistent basis sets
  • Ionic liquids
  • Drug discovery
  • High performance computing
  • Graphics processing units
  • Supercomputer


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