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Title: Double-buffered, heterogeneous CPU + GPU integral digestion algorithm for single-excitation calculations involving a large number of excited states

Journal Article · · Journal of Computational Chemistry
DOI:https://doi.org/10.1002/jcc.25531· OSTI ID:1604460
 [1];  [2]; ORCiD logo [3]
  1. The Ohio State Univ., Columbus, OH (United States); Q‐Chem Inc., Pleasanton, CA (United States)
  2. Q‐Chem Inc., Pleasanton, CA (United States)
  3. The Ohio State Univ., Columbus, OH (United States)
+ Show Author Affiliations

The most widely used quantum-chemical models for excited states are single-excitation theories, a category that includes configuration interaction with single substitutions, time-dependent density functional theory, and also a recently developed ab initio exciton model. When a large number of excited states are desired, these calculations incur a significant bottleneck in the “digestion” step in which two-electron integrals are contracted with density or density-like matrices. We present an implementation that moves this step onto graphical processing units (GPUs), and introduce a double-buffer scheme that minimizes latency by computing integrals on the central processing units (CPUs) concurrently with their digestion on the GPUs. An automatic code generation scheme simplifies the implementation of high-performance GPU kernels. For the exciton model, which requires separate excited-state calculations on each electronically coupled chromophore, the heterogeneous implementation described here results in speedups of 2–6× versus a CPU-only implementation. For traditional time-dependent density functional theory calculations, we obtain speedups of up to 5× when a large number of excited states is computed.

Research Organization:
The Ohio State Univ., Columbus, OH (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
Grant/Contract Number:
SC0008850; SC0008550
OSTI ID:
1604460
Alternate ID(s):
OSTI ID: 1479532
Journal Information:
Journal of Computational Chemistry, Vol. 39, Issue 26; ISSN 0192-8651
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 5 works
Citation information provided by
Web of Science

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Cited By (2)

GPU‐Accelerated Large‐Scale Excited‐State Simulation Based on Divide‐and‐Conquer Time‐Dependent Density‐Functional Tight‐Binding journal August 2019
How will quantum computers provide an industrially relevant computational advantage in quantum chemistry? preprint January 2020

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