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Vlček V, Rabani E, Neuhauser D, et al. Stochastic GW Calculations for Molecules. J Chem Theory Comput. 2017;13(10):4997-5003doi: 10.1021/acs.jctc.7b00770.
Vlček, V., Rabani, E., Neuhauser, D., & Baer, R. (2017). Stochastic GW Calculations for Molecules. Journal of chemical theory and computation, 13(10), 4997-5003. https://doi.org/10.1021/acs.jctc.7b00770
Vlček, Vojtěch, et al. "Stochastic GW Calculations for Molecules." Journal of chemical theory and computation vol. 13,10 (2017): 4997-5003. doi: https://doi.org/10.1021/acs.jctc.7b00770
Vlček V, Rabani E, Neuhauser D, Baer R. Stochastic GW Calculations for Molecules. J Chem Theory Comput. 2017 Oct 10;13(10):4997-5003. doi: 10.1021/acs.jctc.7b00770. Epub 2017 Oct 02. PMID: 28876912.
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J Chem Theory Comput. 2017 Oct 10;13(10):4997-5003. doi: 10.1021/acs.jctc.7b00770. Epub 2017 Oct 02.

Stochastic GW Calculations for Molecules.

Journal of chemical theory and computation

Vojtěch Vlček, Eran Rabani, Daniel Neuhauser, Roi Baer

Affiliations

  1. Department of Chemistry and Biochemistry, University of California , Los Angeles, California 90095, United States.
  2. Fritz Haber Center for Molecular Dynamics, Institute of Chemistry, The Hebrew University of Jerusalem , Jerusalem 91904, Israel.
  3. Department of Chemistry, University of California and Materials Science Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
  4. The Raymond and Beverly Sackler Center for Computational Molecular and Materials Science, Tel Aviv University , Tel Aviv, Israel 69978.

PMID: 28876912 DOI: 10.1021/acs.jctc.7b00770

Abstract

Quasiparticle (QP) excitations are extremely important for understanding and predicting charge transfer and transport in molecules, nanostructures, and extended systems. Since density functional theory (DFT) within the Kohn-Sham (KS) formulation does not provide reliable QP energies, many-body perturbation techniques such as the GW approximation are essential. The main practical drawback of GW implementations is the high computational scaling with system size, prohibiting its use in extended, open boundary systems with many dozens of electrons or more. Recently, a stochastic formulation of GW (sGW) was presented (Phys. Rev. Lett. 2014, 113, 076402) with a near-linear-scaling complexity, illustrated for a series of silicon nanocrystals reaching systems of more than 3000 electrons. This advance provides a route for many-body calculations on very large systems that were impossible with previous approaches. While earlier we have shown the gentle scaling of sGW, its accuracy was not extensively demonstrated. Therefore, we show that this new sGW approach is very accurate by calculating the ionization energies of a group of sufficiently small molecules where a comparison to other GW codes is still possible. Using a set of 10 such molecules, we demonstrate that sGW provides reliable vertical ionization energies in close agreement with benchmark deterministic GW results (J. Chem. Theory Comput, 2015, 11, 5665), with mean (absolute) deviation of 0.05 and 0.09 eV. For completeness, we also provide a detailed review of the sGW theory and numerical implementation.

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