Accurate Absolute and Relative Core-Level Binding Energies from GW

Golze D, Keller L, Rinke P (2020)

Publication Type: Journal article

Publication year: 2020

Journal

Journal of Physical Chemistry Letters American Chemical Society

Book Volume: 11

Pages Range: 1840-1847

Journal Issue: 5

DOI: 10.1021/acs.jpclett.9b03423

Abstract

We present an accurate approach to compute X-ray photoelectron spectra based on the GW Green's function method that overcomes the shortcomings of common density functional theory approaches. GW has become a popular tool to compute valence excitations for a wide range of materials. However, core-level spectroscopy is thus far almost uncharted in GW. We show that single-shot perturbation calculations in the G0W0 approximation, which are routinely used for valence states, cannot be applied for core levels and suffer from an extreme, erroneous transfer of spectral weight to the satellite spectrum. The correct behavior can be restored by partial self-consistent GW schemes or by using hybrid functionals with almost 50% of exact exchange as a starting point for G0W0. We also include relativistic corrections and present a benchmark study for 65 molecular 1s excitations. Our absolute and relative GW core-level binding energies agree within 0.3 and 0.2 eV with experiment, respectively.

Involved external institutions

Aalto University Espoo

Finland (FI)

How to cite

APA:

Golze, D., Keller, L., & Rinke, P. (2020). Accurate Absolute and Relative Core-Level Binding Energies from GW. Journal of Physical Chemistry Letters, 11(5), 1840-1847. https://doi.org/10.1021/acs.jpclett.9b03423

MLA:

Golze, Dorothea, Levi Keller, and Patrick Rinke. "Accurate Absolute and Relative Core-Level Binding Energies from GW." Journal of Physical Chemistry Letters 11.5 (2020): 1840-1847.

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