Exploiting graphical processing units to enable quantum chemistry calculation of large solvated molecules with conductor-like polarizable continuum models |
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Authors: | Fang Liu David M. Sanchez Heather J. Kulik Todd J. Martínez |
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Affiliation: | 1. Department of Chemistry and The PULSE Institute, Stanford University, Stanford, California;2. Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts |
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Abstract: | The conductor-like polarizable continuum model (C-PCM) with switching/Gaussian smooth discretization is a widely used implicit solvation model in quantum chemistry. We have previously implemented C-PCM solvation for Hartree-Fock (HF) and density functional theory (DFT) on graphical processing units (GPUs), enabling the quantum mechanical treatment of large solvated biomolecules. Here, we first propose a GPU-based algorithm for the PCM conjugate gradient linear solver that greatly improves the performance for very large molecules. The overhead for PCM-related evaluations now consumes less than 15% of the total runtime for DFT calculations on large molecules. Second, we demonstrate that our algorithms tailored for ground state C-PCM are transferable to excited state properties. Using a single GPU, our method evaluates the analytic gradient of the linear response PCM time-dependent density functional theory energy up to 80× faster than a conventional central processing unit (CPU)-based implementation. In addition, our C-PCM algorithms are transferable to other methods that require electrostatic potential (ESP) evaluations. For example, we achieve speed-ups of up to 130× for restricted ESP-based atomic charge evaluations, when compared to CPU-based codes. We also summarize and compare the different PCM cavity discretization schemes used in some popular quantum chemistry packages as a reference for both users and developers. |
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Keywords: | excited state graphical processing unit nonequilibrium solvation polarizable continuum |
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