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Title: Efficient Treatment of Large Active Spaces through Multi-GPU Parallel Implementation of Direct Configuration Interaction

Abstract

In this study, we have extended our graphical processing unit (GPU)-accelerated direct configuration interaction program to multiple devices, reducing iteration times for configuration spaces of 165 million determinants to only 3 s using NVIDIA P100 GPUs. Similar improvements in the one- and two-particle reduced density matrix formation allow for fast analytical energy gradients and electronic properties. Our parallel algorithm enables the calculation of arbitrarily large configuration spaces (limited only by available system memory), with iteration times of 13 min for an active space of 18 electrons in 18 orbitals (2.4 billion determinants) using six consumer grade NVIDIA 1080Ti GPUs. These advances enable routine molecular dynamics simulations, geometry optimizations, and absorption spectrum calculations for molecules with large configuration spaces, a task that has heretofore required massive computational effort. In this work, we demonstrate the utility of our program by generating the absorption spectrum for diphenyl acetylene at the floating occupation molecular orbital complete active space configuration interaction level of theory. Lastly, several active spaces were investigated to assess the dependence of spectral features on orbital space dimension.

Authors:
ORCiD logo [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR). Scientific Discovery through Advanced Computing (SciDAC); Extreme Science and Engineering Discovery Environment; National Science Foundation (NSF)
OSTI Identifier:
1617039
Grant/Contract Number:  
AC02-76SF00515; TG-CHE140101; ACI-1429830
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Theory and Computation
Additional Journal Information:
Journal Volume: 16; Journal Issue: 3; Journal ID: ISSN 1549-9618
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
97 MATHEMATICS AND COMPUTING; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Fales, B. Scott, and Martínez, Todd J. Efficient Treatment of Large Active Spaces through Multi-GPU Parallel Implementation of Direct Configuration Interaction. United States: N. p., 2020. Web. doi:10.1021/acs.jctc.9b01165.
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Fales, B. Scott, & Martínez, Todd J. Efficient Treatment of Large Active Spaces through Multi-GPU Parallel Implementation of Direct Configuration Interaction. United States. https://doi.org/10.1021/acs.jctc.9b01165
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Fales, B. Scott, and Martínez, Todd J. Wed . "Efficient Treatment of Large Active Spaces through Multi-GPU Parallel Implementation of Direct Configuration Interaction". United States. https://doi.org/10.1021/acs.jctc.9b01165. https://www.osti.gov/servlets/purl/1617039.
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@article{osti_1617039,
title = {Efficient Treatment of Large Active Spaces through Multi-GPU Parallel Implementation of Direct Configuration Interaction},
author = {Fales, B. Scott and Martínez, Todd J.},
abstractNote = {In this study, we have extended our graphical processing unit (GPU)-accelerated direct configuration interaction program to multiple devices, reducing iteration times for configuration spaces of 165 million determinants to only 3 s using NVIDIA P100 GPUs. Similar improvements in the one- and two-particle reduced density matrix formation allow for fast analytical energy gradients and electronic properties. Our parallel algorithm enables the calculation of arbitrarily large configuration spaces (limited only by available system memory), with iteration times of 13 min for an active space of 18 electrons in 18 orbitals (2.4 billion determinants) using six consumer grade NVIDIA 1080Ti GPUs. These advances enable routine molecular dynamics simulations, geometry optimizations, and absorption spectrum calculations for molecules with large configuration spaces, a task that has heretofore required massive computational effort. In this work, we demonstrate the utility of our program by generating the absorption spectrum for diphenyl acetylene at the floating occupation molecular orbital complete active space configuration interaction level of theory. Lastly, several active spaces were investigated to assess the dependence of spectral features on orbital space dimension.},
doi = {10.1021/acs.jctc.9b01165},
journal = {Journal of Chemical Theory and Computation},
number = 3,
volume = 16,
place = {United States},
year = {Wed Jan 29 00:00:00 EST 2020},
month = {Wed Jan 29 00:00:00 EST 2020}
}
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https://doi.org/10.1021/acs.jctc.9b01165
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