Content area

Abstract

Hybrid density functional approximations (DFAs) offer compelling accuracy for ab initio electronic-structure simulations of molecules, nanosystems, and bulk materials, addressing some deficiencies of computationally cheaper, frequently used semilocal DFAs. However, the computational bottleneck of hybrid DFAs is the evaluation of the non-local exact exchange contribution, which is the limiting factor for the application of the method for large-scale simulations. In this work, we present a drastically optimized resolution-of-identity-based real-space implementation of the exact exchange evaluation for both non-periodic and periodic boundary conditions in the all-electron code FHI-aims, targeting high-performance CPU compute clusters. The introduction of several new refined Message Passing Interface (MPI) parallelization layers and shared memory arrays according to the MPI-3 standard were the key components of the optimization. We demonstrate significant improvements of memory and performance efficiency, scalability, and workload distribution, extending the reach of hybrid DFAs to simulation sizes beyond ten thousand atoms. As a necessary byproduct of this work, other code parts in FHI-aims have been optimized as well, e.g., the computation of the Hartree potential and the evaluation of the force and stress components. We benchmark the performance and scaling of the hybrid DFA based simulations for a broad range of chemical systems, including hybrid organic-inorganic perovskites, organic crystals and ice crystals with up to 30,576 atoms (101,920 electrons described by 244,608 basis functions).

Details

1009240
Identifier / keyword
Title
Efficient All-electron Hybrid Density Functionals for Atomistic Simulations Beyond 10,000 Atoms
Publication title
arXiv.org; Ithaca
Publication year
2024
Publication date
Mar 15, 2024
Section
Condensed Matter
Publisher
Cornell University Library, arXiv.org
Source
arXiv.org
Place of publication
Ithaca
Country of publication
United States
University/institution
Cornell University Library arXiv.org
e-ISSN
2331-8422
Source type
Working Paper
Language of publication
English
Document type
Working Paper
Publication history
 
 
Online publication date
2024-07-15
Milestone dates
2024-03-15 (Submission v1)
Publication history
 
 
   First posting date
15 Jul 2024
ProQuest document ID
2962943979
Document URL
https://www.proquest.com/working-papers/efficient-all-electron-hybrid-density-functionals/docview/2962943979/se-2?accountid=208611
Full text outside of ProQuest
Copyright
© 2024. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.
Last updated
2024-07-16
Database
ProQuest One Academic