Core-Level Binding Energies from GW: An Efficient Full-Frequency Approach within a Localized Basis

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Core-Level Binding Energies from GW : An Efficient Full-Frequency Approach within a Localized Basis. / Golze, Dorothea; Wilhelm, Jan; Van Setten, Michiel J.; Rinke, Patrick.

In: Journal of Chemical Theory and Computation, Vol. 14, No. 9, 11.09.2018, p. 4856-4869.

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@article{ffdf2697ec2844468625a54e2285bb79,
title = "Core-Level Binding Energies from GW: An Efficient Full-Frequency Approach within a Localized Basis",
abstract = "The GW method is routinely used to predict charged valence excitations in molecules and solids. However, the numerical techniques employed in the most efficient GW algorithms break down when computing core excitations as measured by X-ray photoelectron spectroscopy (XPS). We present a full-frequency approach on the real axis using a localized basis to enable the treatment of core levels in GW. Our scheme is based on the contour deformation technique and allows for a precise and efficient calculation of the self-energy, which has a complicated pole structure for core states. The accuracy of our method is validated by comparing to a fully analytic GW algorithm. Furthermore, we report the obtained core-level binding energies and their deviations from experiment for a set of small molecules and large polycyclic hydrocarbons. The core-level excitations computed with our GW approach deviate by less than 0.5 eV from the experimental reference. For comparison, we also report core-level binding energies calculated by density functional theory (DFT)-based approaches such as the popular delta self-consistent field (ΔSCF) method. Our implementation is optimized for massively parallel execution, enabling the computation of systems up to 100 atoms.",
author = "Dorothea Golze and Jan Wilhelm and {Van Setten}, {Michiel J.} and Patrick Rinke",
year = "2018",
month = "9",
day = "11",
doi = "10.1021/acs.jctc.8b00458",
language = "English",
volume = "14",
pages = "4856--4869",
journal = "Journal of Chemical Theory and Computation",
issn = "1549-9618",
publisher = "AMERICAN CHEMICAL SOCIETY",
number = "9",

}

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TY - JOUR

T1 - Core-Level Binding Energies from GW

T2 - An Efficient Full-Frequency Approach within a Localized Basis

AU - Golze, Dorothea

AU - Wilhelm, Jan

AU - Van Setten, Michiel J.

AU - Rinke, Patrick

PY - 2018/9/11

Y1 - 2018/9/11

N2 - The GW method is routinely used to predict charged valence excitations in molecules and solids. However, the numerical techniques employed in the most efficient GW algorithms break down when computing core excitations as measured by X-ray photoelectron spectroscopy (XPS). We present a full-frequency approach on the real axis using a localized basis to enable the treatment of core levels in GW. Our scheme is based on the contour deformation technique and allows for a precise and efficient calculation of the self-energy, which has a complicated pole structure for core states. The accuracy of our method is validated by comparing to a fully analytic GW algorithm. Furthermore, we report the obtained core-level binding energies and their deviations from experiment for a set of small molecules and large polycyclic hydrocarbons. The core-level excitations computed with our GW approach deviate by less than 0.5 eV from the experimental reference. For comparison, we also report core-level binding energies calculated by density functional theory (DFT)-based approaches such as the popular delta self-consistent field (ΔSCF) method. Our implementation is optimized for massively parallel execution, enabling the computation of systems up to 100 atoms.

AB - The GW method is routinely used to predict charged valence excitations in molecules and solids. However, the numerical techniques employed in the most efficient GW algorithms break down when computing core excitations as measured by X-ray photoelectron spectroscopy (XPS). We present a full-frequency approach on the real axis using a localized basis to enable the treatment of core levels in GW. Our scheme is based on the contour deformation technique and allows for a precise and efficient calculation of the self-energy, which has a complicated pole structure for core states. The accuracy of our method is validated by comparing to a fully analytic GW algorithm. Furthermore, we report the obtained core-level binding energies and their deviations from experiment for a set of small molecules and large polycyclic hydrocarbons. The core-level excitations computed with our GW approach deviate by less than 0.5 eV from the experimental reference. For comparison, we also report core-level binding energies calculated by density functional theory (DFT)-based approaches such as the popular delta self-consistent field (ΔSCF) method. Our implementation is optimized for massively parallel execution, enabling the computation of systems up to 100 atoms.

UR - http://www.scopus.com/inward/record.url?scp=85052364899&partnerID=8YFLogxK

U2 - 10.1021/acs.jctc.8b00458

DO - 10.1021/acs.jctc.8b00458

M3 - Article

VL - 14

SP - 4856

EP - 4869

JO - Journal of Chemical Theory and Computation

JF - Journal of Chemical Theory and Computation

SN - 1549-9618

IS - 9

ER -

ID: 29222141