Published September 23, 2024 | Version v1
Journal article

Solving multipole challenges in the GW100 benchmark enables precise low-scaling GW calculations

  • 1. Institute of Theoretical Physics and Regensburg Center for Ultrafast Nanoscopy (RUN), University of Regensburg, 93053 Regensburg, Germany
  • 2. Faculty for Chemistry and Food Chemistry, Technische Universität Dresden, 01062 Dresden, Germany

Description

The GW approximation is a widely used method for computing electron addition and removal energies of molecules and solids. The computational effort of conventional GW algorithms increases as O(N4) with the system size N, hindering the application of GW to large and complex systems. Low-scaling GW algorithms are currently very actively developed. Benchmark studies at the single-shot G0W0 level indicate excellent numerical precision for frontier quasiparticle energies, with mean absolute deviations <10 meV between low-scaling and standard implementations for the widely used GW100 test set. A notable challenge for low-scaling GW algorithms remains in achieving high precision for five molecules within the GW100 test set, namely O3, BeO, MgO, BN, and CuCN, for which the deviations are in the range of several hundred meV at the G0W0 level. This is because of a spurious transfer of spectral weight from the quasiparticle to the satellite spectrum in G0W0 calculations, resulting in multipole features in the self-energy and spectral function, which low-scaling algorithms fail to describe. We show in this paper that including eigenvalue self-consistency in the Green's function (evGW0) achieves a proper separation between satellite and quasiparticle peak, leading to a single solution of the quasiparticle equation with spectral weight close to one. evGW0 quasiparticles energies from low-scaling GW closely align with reference calculations; the mean absolute error is only 12 meV for the five molecules. We thus demonstrate that low-scaling GW with self-consistency in G is well suited for computing frontier quasiparticle energies.

Additional details

Identifiers

DOI
10.1103/PhysRevB.110.125146;
arXiv
arXiv:2405.20473;
Crossref Funder ID
10.13039/100018693; 10.13039/501100001659;

Publishing Information

Journal Title
Physical Review B
Journal Volume
110
Journal Issue
12
Journal Page Range
19 pgs.
ISSN
1550-235X

INIS

Country of Publication
United States
Country of Input or Organization
International Atomic Energy Agency (IAEA)

Optional Information

Copyright
©2024 American Physical Society
Contract/Grant/Project number
453275048; 503985532
Notes
Contact Email: Contact author: jan.wilhelm@physik.uni-regensburg.de; Record automatically processed
Funding organization
HORIZON EUROPE Framework Programme; Deutsche Forschungsgemeinschaft