Performance of Coupled-Cluster Singles and Doubles on Modern Stream Processing Architectures

Fales, B. Scott; Curtis, Ethan R.; Johnson, Kate; Lahana, Dean; Seritan, Stefan; Wang, Yuanheng; Weir, Hayley; Martı́nez, Todd J.; Hohenstein, Edward G.

doi:10.1021/acs.jctc.0c00336

Cited by 22 publications

(22 citation statements)

References 72 publications

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“…The SOS‐MP2 method 86 neglects exchange‐like terms to arrive at a formal scaling of O (N 4 ), and THC‐SOS‐MP2 further reduces this scaling to O (N 3 ). Recently, a GPU‐accelerated coupled‐cluster code has also been implemented in TeraChem, enabling coupled‐cluster singles and doubles (CCSD) as well as any method that can be written as a subset of CCSD diagrams 87 …”

Section: Single Reference Post‐scf Methodsmentioning

confidence: 99%

TeraChem: A graphical processing unit‐accelerated electronic structure package for large‐scale ab initio molecular dynamics

Seritan

Bannwarth

Fales

et al. 2020

WIREs Comput Mol Sci

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212

171

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TeraChem was born in 2008 with the goal of providing fast on‐the‐fly electronic structure calculations to facilitate ab initio molecular dynamics studies of large biochemical systems such as photoswitchable proteins and multichromophoric antenna complexes. Originally developed for videogaming applications, graphics processing units (GPUs) offered a low‐cost parallel computer architecture that became more accessible for general‐purpose GPU computing with the release of CUDA in 2007. The evaluation of the electron repulsion integrals (ERIs) is a major bottleneck in electronic structure codes and provides an attractive target for acceleration on GPUs. Thus, highly efficient routines for evaluation of and contractions between the ERIs and density matrices were implemented in TeraChem. Electronic structure methods were developed and implemented to leverage these integral contraction routines, resulting in the first quantum chemistry package designed from the ground up for GPUs. This GPU acceleration makes TeraChem capable of performing large‐scale ground and excited state calculations in the gas and condensed phase. Today, TeraChem's speed forms the basis for a suite of quantum chemistry applications, including optimization and dynamics of proteins, automated and interactive chemical discovery tools, and large‐scale nonadiabatic dynamics simulations. This article is categorized under: Electronic Structure Theory > Ab Initio Electronic Structure Methods Software > Quantum Chemistry Structure and Mechanism > Computational Biochemistry and Biophysics

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Section: Single Reference Post‐scf Methodsmentioning

confidence: 99%

TeraChem: A graphical processing unit‐accelerated electronic structure package for large‐scale ab initio molecular dynamics

Seritan

Bannwarth

Fales

et al. 2020

WIREs Comput Mol Sci

Self Cite

212

171

View full text Add to dashboard Cite

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“…Dr. Hohenstein then discussed an implementation of CCSD and EOM-CCSD algorithms on graphics cards, which makes the calculation of 100 atom systems computationally feasible. The CCSD calculations on eight graphics cards matched the performance of sixty-four 16-core CPU-based nodes …”

Section: Introductionmentioning

confidence: 99%

Viewpoints on the 2020 Virtual Conference on Theoretical Chemistry

DiRisio

Jones

et al. 2020

J. Phys. Chem. A

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“…14,15 They have, for instance, demonstrated that NCIs are strongly attenuated in a solvated environment. 16 Despite the intense efforts associated with developing a posteriori dispersion corrections [17][18][19][20][21][22][23][24][25][26][27][28][29][30][31][32][33][34] or with reducing the cost of wavefunction-based methods, [35][36][37][38][39][40][41] the finite-temperature description of competing NCIs remains coarse if the solvent is represented as a continuum. In particular, interaction energies estimated by dispersion-corrected computations in implicitly modeled solvent can be one magnitude larger than experimental energies in solutions.…”

Section: Introductionmentioning

confidence: 99%

Assessing the persistence of chalcogen bonds in solution with neural network potentials

Juraskova,

Celerse,

Laplaza

et al. 2022

Preprint

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Non-covalent bonding patterns are commonly harvested as a design principle in the field of catalysis, supramolecular chemistry and functional materials to name a few. Yet, their computational description generally neglects finite temperature and environment effects, which promote competing interactions and alter their static gas-phase properties. Recently, neural network potentials (NNPs) trained on Density Functional Theory (DFT) data have become increasingly popular to simulate molecular phenomena in condensed phase with an accuracy comparable to ab initio methods. To date, most applications have centered on solid-state materials or fairly simple molecules made of a limited number of elements. Herein, we focus on the persistence and strength of chalcogen bonds involving a benzotelluradiazole in condensed phase. While the tellurium-containing heteroaromatic molecules are known to exhibit pronounced interactions with anions and lone pairs of different atoms, the relevance of competing intermolecular interactions, notably with the solvent, are complicated to monitor experimentally but also challenging to model at an accurate electronic structure level. Here, we train a direct and baselined NNPs to reproduce hybrid DFT energies and forces in order to identify what are the most prevalent non-covalent interactions occurring in a solute-Cl --THF mixture. The simulations in explicit solvent highlight the clear competition with chalcogen bonds formed with the solvent and the short-range directionality of the interaction with direct consequences for the molecular properties in the solution. The comparison with other potentials (e.g., AMOEBA, direct NNP and continuum solvent model) also demonstrates that baselined NNPs offer a reliable picture of the non-covalent interaction interplay occurring in solution.

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Performance of Coupled-Cluster Singles and Doubles on Modern Stream Processing Architectures

Cited by 22 publications

References 72 publications

TeraChem: A graphical processing unit‐accelerated electronic structure package for large‐scale ab initio molecular dynamics

TeraChem: A graphical processing unit‐accelerated electronic structure package for large‐scale ab initio molecular dynamics

Viewpoints on the 2020 Virtual Conference on Theoretical Chemistry

Assessing the persistence of chalcogen bonds in solution with neural network potentials

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