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Wilhelm, Jan ; Seewald, Patrick ; Golze, Dorothea

Low-Scaling GW with Benchmark Accuracy and Application to Phosphorene Nanosheets

Wilhelm, Jan , Seewald, Patrick and Golze, Dorothea (2021) Low-Scaling GW with Benchmark Accuracy and Application to Phosphorene Nanosheets. Journal of Chemical Theory and Computation 17 (3), pp. 1662-1667.

Date of publication of this fulltext: 21 May 2021 04:49
Article
DOI to cite this document: 10.5283/epub.45833


Abstract

GW is an accurate method for computing electron addition and removal energies of molecules and solids. In a conventional GW implementation, however, its computational cost is O(N-4) in the system size N, which prohibits its application to many systems of interest. We present a low-scaling GW algorithm with notably improved accuracy compared to our previous algorithm [J. Phys. Chem. Lett. 2018, 9, ...

GW is an accurate method for computing electron addition and removal energies of molecules and solids. In a conventional GW implementation, however, its computational cost is O(N-4) in the system size N, which prohibits its application to many systems of interest. We present a low-scaling GW algorithm with notably improved accuracy compared to our previous algorithm [J. Phys. Chem. Lett. 2018, 9, 306-312]. This is demonstrated for frontier orbitals using the GW100 benchmark set, for which our algorithm yields a mean absolute deviation of only 6 meV with respect to canonical implementations. We show that also excitations of deep valence, semicore, and unbound states match conventional schemes within 0.1 eV. The high accuracy is achieved by using minimax grids with 30 grid points and the resolution of the identity with the truncated Coulomb metric. We apply the low-scaling GW algorithm with improved accuracy to phosphorene nanosheets of increasing size. We find that their fundamental gap is strongly size-dependent varying from 4.0 eV (1.8 nm x 1.3 nm, 88 atoms) to 2.4 eV (6.9 nm x 4.8 nm, 990 atoms) at the evGW(0)@PBE level.



Involved Institutions


Details

Item typeArticle
Journal or Publication TitleJournal of Chemical Theory and Computation
Publisher:AMER CHEMICAL SOC
Open Access Type:Hybrid Open Acces
Place of Publication:WASHINGTON
Volume:17
Number of Issue or Book Chapter:3
Page Range:pp. 1662-1667
Date23 February 2021
InstitutionsPhysics > Institute of Theroretical Physics
Physics > Institute of Theroretical Physics > Chair Ferdinand Evers
Identification Number
ValueType
10.1021/acs.jctc.0c01282DOI
KeywordsGAUSSIAN-BASIS SETS; CORRELATED MOLECULAR CALCULATIONS; RANDOM-PHASE-APPROXIMATION; AUXILIARY BASIS EXPANSIONS; SPACE-TIME METHOD; ELECTRONIC-STRUCTURE; CORRELATION ENERGIES; GREENS-FUNCTION; ATOMS; RESOLUTION
Dewey Decimal Classification500 Science > 530 Physics
StatusPublished
RefereedYes, this version has been refereed
Created at the University of RegensburgYes
URN of the UB Regensburgurn:nbn:de:bvb:355-epub-458336
Item ID45833

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