Improving the Performance of Hybrid Functional-Based Molecular Dynamics Simulation through Screening of Hartree–Fock Exchange ForcesClick to copy article linkArticle link copied!
Abstract
Density functional theory-based molecular dynamics calculations of condensed phase systems often benefit from the use of hybrid functionals. However, their use is computationally very demanding and severely limits the system size and time scale that can be simulated. Several methods have been introduced to accelerate hybrid functional molecular dynamics including Schwarz screening and the auxiliary density matrix method (ADMM). Here we present a simple screening scheme that can be applied in addition to these methods. It works by examining Hartree–Fock exchange (HFX) integrals and subsequently excluding those that contribute very little to any nuclear force component. The resultant force error is corrected by a history-dependent extrapolation scheme. We find that for systems where the calculation of HFX forces is a major bottleneck, a large fraction of the integrals can be neglected without introducing significant errors in the nuclear forces. For instance, for a 2 × 2 × 2 unit cell of CoO, 92% of the HFX integrals that have passed Schwarz screening within the ADMM approach can be neglected leading to a performance gain of a factor of 3 at a negligible error in nuclear forces (≤5 × 10–4 H bohr–1). We also show that total energy conservation and solvation structures are not adversely affected by the screening method.
Cited By
Smart citations by scite.ai include citation statements extracted from the full text of the citing article. The number of the statements may be higher than the number of citations provided by ACS Publications if one paper cites another multiple times or lower if scite has not yet processed some of the citing articles.
This article is cited by 9 publications.
- Ritama Kar, Sagarmoy Mandal, Vaishali Thakkur, Bernd Meyer, Nisanth N. Nair. Speeding-up Hybrid Functional-Based Ab Initio Molecular Dynamics Using Multiple Time-stepping and Resonance-Free Thermostat. Journal of Chemical Theory and Computation 2023, 19
(22)
, 8351-8364. https://doi.org/10.1021/acs.jctc.3c00964
- Bhaskar Rana, John M. Herbert. Hidden Hemibonding in the Aqueous Hydroxyl Radical. The Journal of Physical Chemistry Letters 2021, 12
(33)
, 8053-8060. https://doi.org/10.1021/acs.jpclett.1c02283
- Sagarmoy Mandal, Vaishali Thakkur, Nisanth N. Nair. Achieving an Order of Magnitude Speedup in Hybrid-Functional- and Plane-Wave-Based Ab Initio Molecular Dynamics: Applications to Proton-Transfer Reactions in Enzymes and in Solution. Journal of Chemical Theory and Computation 2021, 17
(4)
, 2244-2255. https://doi.org/10.1021/acs.jctc.1c00009
- Sagarmoy Mandal, Ritama Kar, Tobias Klöffel, Bernd Meyer, Nisanth N. Nair. Improving the scaling and performance of multiple time stepping‐based molecular dynamics with hybrid density functionals. Journal of Computational Chemistry 2022, 43
(9)
, 588-597. https://doi.org/10.1002/jcc.26816
- Guido Falk von Rudorff. Arbitrarily accurate quantum alchemy. The Journal of Chemical Physics 2021, 155
(22)
https://doi.org/10.1063/5.0073941
- Bhaskar Rana, John M. Herbert. Role of hemibonding in the structure and ultraviolet spectroscopy of the aqueous hydroxyl radical. Physical Chemistry Chemical Physics 2020, 22
(47)
, 27829-27844. https://doi.org/10.1039/D0CP05216G
- Christina Apostolidou. Vibrational Spectra of the OH Radical in Water: Ab Initio Molecular Dynamics Simulations and Quantum Chemical Calculations Using Hybrid Functionals. Advanced Theory and Simulations 2020, 3
(12)
https://doi.org/10.1002/adts.202000174
- Sagarmoy Mandal, Nisanth N. Nair. Speeding-up
ab initio
molecular dynamics with hybrid functionals using adaptively compressed exchange operator based multiple timestepping. The Journal of Chemical Physics 2019, 151
(15)
https://doi.org/10.1063/1.5125422
- Christina Apostolidou. OH radical in water from
ab initio
molecular dynamics simulation employing hybrid functionals. The Journal of Chemical Physics 2019, 151
(6)
https://doi.org/10.1063/1.5107479
Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.
Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.
The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.