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Title: Intensive Atomization Energy: Re-Thinking a Metric for Electronic Structure Theory Methods

Abstract

Abstract The errors in atomization energies (

Authors:
; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for the Computational Design of Functional Layered Materials (CCDM)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1371107
DOE Contract Number:
SC0012575
Resource Type:
Journal Article
Resource Relation:
Journal Name: Zeitschrift fuer Physikalische Chemie; Journal Volume: 230; Journal Issue: 5-7; Related Information: CCDM partners with Temple University (lead); Brookhaven National Laboratory; Drexel University; Duke University; North Carolina State University; Northeastern University; Princeton University; Rice University; University of Pennsylvania
Country of Publication:
United States
Language:
English
Subject:
catalysis (heterogeneous), solar (photovoltaic), energy storage (including batteries and capacitors), hydrogen and fuel cells, defects, mechanical behavior, materials and chemistry by design, synthesis (novel materials)

Citation Formats

Perdew, John P., Sun, Jianwei, Garza, Alejandro J., and Scuseria, Gustavo E. Intensive Atomization Energy: Re-Thinking a Metric for Electronic Structure Theory Methods. United States: N. p., 2016. Web. doi:10.1515/zpch-2015-0713.
Perdew, John P., Sun, Jianwei, Garza, Alejandro J., & Scuseria, Gustavo E. Intensive Atomization Energy: Re-Thinking a Metric for Electronic Structure Theory Methods. United States. doi:10.1515/zpch-2015-0713.
Perdew, John P., Sun, Jianwei, Garza, Alejandro J., and Scuseria, Gustavo E. 2016. "Intensive Atomization Energy: Re-Thinking a Metric for Electronic Structure Theory Methods". United States. doi:10.1515/zpch-2015-0713.
@article{osti_1371107,
title = {Intensive Atomization Energy: Re-Thinking a Metric for Electronic Structure Theory Methods},
author = {Perdew, John P. and Sun, Jianwei and Garza, Alejandro J. and Scuseria, Gustavo E.},
abstractNote = {Abstract The errors in atomization energies (},
doi = {10.1515/zpch-2015-0713},
journal = {Zeitschrift fuer Physikalische Chemie},
number = 5-7,
volume = 230,
place = {United States},
year = 2016,
month = 1
}
  • Abstract The errors in atomization energies (
  • No abstract prepared.
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  • Domain based local pair natural orbital coupled cluster theory with single-, double-, and perturbative triple excitations (DLPNO-CCSD(T)) is a highly efficient local correlation method. It is known to be accurate and robust and can be used in a black box fashion in order to obtain coupled cluster quality total energies for large molecules with several hundred atoms. While previous implementations showed near linear scaling up to a few hundred atoms, several nonlinear scaling steps limited the applicability of the method for very large systems. In this work, these limitations are overcome and a linear scaling DLPNO-CCSD(T) method for closed shellmore » systems is reported. The new implementation is based on the concept of sparse maps that was introduced in Part I of this series [P. Pinski, C. Riplinger, E. F. Valeev, and F. Neese, J. Chem. Phys. 143, 034108 (2015)]. Using the sparse map infrastructure, all essential computational steps (integral transformation and storage, initial guess, pair natural orbital construction, amplitude iterations, triples correction) are achieved in a linear scaling fashion. In addition, a number of additional algorithmic improvements are reported that lead to significant speedups of the method. The new, linear-scaling DLPNO-CCSD(T) implementation typically is 7 times faster than the previous implementation and consumes 4 times less disk space for large three-dimensional systems. For linear systems, the performance gains and memory savings are substantially larger. Calculations with more than 20 000 basis functions and 1000 atoms are reported in this work. In all cases, the time required for the coupled cluster step is comparable to or lower than for the preceding Hartree-Fock calculation, even if this is carried out with the efficient resolution-of-the-identity and chain-of-spheres approximations. The new implementation even reduces the error in absolute correlation energies by about a factor of two, compared to the already accurate previous implementation.« less