Solving multipole challenges in the benchmark enables precise low-scaling calculations
Creators
- 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 approximation is a widely used method for computing electron addition and removal energies of molecules and solids. The computational effort of conventional algorithms increases as with the system size , hindering the application of to large and complex systems. Low-scaling algorithms are currently very actively developed. Benchmark studies at the single-shot level indicate excellent numerical precision for frontier quasiparticle energies, with mean absolute deviations meV between low-scaling and standard implementations for the widely used test set. A notable challenge for low-scaling algorithms remains in achieving high precision for five molecules within the test set, namely , and , for which the deviations are in the range of several hundred meV at the level. This is because of a spurious transfer of spectral weight from the quasiparticle to the satellite spectrum in 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 () achieves a proper separation between satellite and quasiparticle peak, leading to a single solution of the quasiparticle equation with spectral weight close to one. quasiparticles energies from low-scaling closely align with reference calculations; the mean absolute error is only 12 meV for the five molecules. We thus demonstrate that low-scaling with self-consistency in 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