Accelerating Correlated Quantum Chemistry Calculations Using Graphical Processing Units and a Mixed Precision Matrix Multiplication Library

 Title: Accelerating Correlated Quantum Chemistry Calculations Using Graphical Processing Units and a Mixed Precision Matrix Multiplication Library Author: Olivares-Amaya, Roberto; Watson, Mark A.; Edgar, Richard G; Vogt, Leslie Ann; Shao, Yihan; Aspuru-Guzik, Alan Note: Order does not necessarily reflect citation order of authors. Citation: Olivares-Amaya, Roberto, Mark A. Watson, Richard G. Edgar, Leslie Vogt, Yihan Shao, and Alán Aspuru-Guzik. 2010. Accelerating correlated quantum chemistry calculations using graphical processing units and a mixed-precision matrix multiplication library. Journal of Chemical Theory and Computation 6(1): 135-144. Full Text & Related Files: Accelerating_correlated_quantum_chemistry.pdf (193.7Kb; PDF) Abstract: Two new tools for the acceleration of computational chemistry codes using graphical processing units (GPUs) are presented. First, we propose a general black-box approach for the efficient GPU acceleration of matrix−matrix multiplications where the matrix size is too large for the whole computation to be held in the GPU’s onboard memory. Second, we show how to improve the accuracy of matrix multiplications when using only single-precision GPU devices by proposing a heterogeneous computing model, whereby single- and double-precision operations are evaluated in a mixed fashion on the GPU and central processing unit, respectively. The utility of the library is illustrated for quantum chemistry with application to the acceleration of resolution-of-the-identity second-order Møller−Plesset perturbation theory calculations for molecules, which we were previously unable to treat. In particular, for the 168-atom valinomycin molecule in a cc-pVDZ basis set, we observed speedups of 13.8, 7.8, and 10.1 times for single-, double- and mixed-precision general matrix multiply (SGEMM, DGEMM, and MGEMM), respectively. The corresponding errors in the correlation energy were reduced from −10.0 to −1.2 kcal mol$$^{-1}$$ for SGEMM and MGEMM, respectively, while higher accuracy can be easily achieved with a different choice of cutoff parameter. Published Version: doi:10.1021/ct900543q Terms of Use: This article is made available under the terms and conditions applicable to Open Access Policy Articles, as set forth at http://nrs.harvard.edu/urn-3:HUL.InstRepos:dash.current.terms-of-use#OAP Citable link to this page: http://nrs.harvard.edu/urn-3:HUL.InstRepos:5344469 Downloads of this work: