Equation-of-Motion Coupled-Cluster Cumulant Green’s Function for Excited States and X-ray Spectra
Abstract
Green’s function methods within many-body perturbation theory provide a general framework for treating electronic correlations in excited states and spectra. Conventional methods using the Dyson equation or the cumulant expansion are typically based on the GW self-energy approximation. In order to extend this approximation in molecular systems, a non-perturbative real-time coupled-cluster cumulant Green’s function approach has been introduced, where the cumulant is obtained as the solution to a set of coupled first order, non-linear differential equations. This approach naturally includes non-linear corrections to conventional cumulant Green’s function techniques where the cumulant is linear in the GW self-energy. The method yields the spectral function associated with the core Green’s function, which is directly related to the x-ray photoemission spectra (XPS) of molecular systems. The approach also yields very good results for binding energies and satellite excitations. The x-ray absorption spectrum (XAS) is then obtained as a convolution of the core spectral function and an effective one-body absorption spectrum. Here this approach is extended to include the full coupled-cluster-singles (CCS) core Green’s function by including the complete form of the non-linear contributions to the cumulant as well as all single, double, and triple cluster excitations in the CC amplitude equations. This approachmore »
- Authors:
-
- Univ. of Washington, Seattle, WA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1829677
- Report Number(s):
- PNNL-SA-163615
Journal ID: ISSN 2296-2646
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Frontiers in Chemistry
- Additional Journal Information:
- Journal Volume: 9; Journal ID: ISSN 2296-2646
- Publisher:
- Frontiers Research Foundation
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; coupled cluster; electronic structure; electronic structure calculations; Ab initio calculation; excited electronic states; computational chemistry
Citation Formats
Vila, Fernando D., Kas, Joshua J., Rehr, John J., Kowalski, Karol, and Peng, Bo. Equation-of-Motion Coupled-Cluster Cumulant Green’s Function for Excited States and X-ray Spectra. United States: N. p., 2021.
Web. doi:10.3389/fchem.2021.734945.
Vila, Fernando D., Kas, Joshua J., Rehr, John J., Kowalski, Karol, & Peng, Bo. Equation-of-Motion Coupled-Cluster Cumulant Green’s Function for Excited States and X-ray Spectra. United States. https://doi.org/10.3389/fchem.2021.734945
Vila, Fernando D., Kas, Joshua J., Rehr, John J., Kowalski, Karol, and Peng, Bo. Wed .
"Equation-of-Motion Coupled-Cluster Cumulant Green’s Function for Excited States and X-ray Spectra". United States. https://doi.org/10.3389/fchem.2021.734945. https://www.osti.gov/servlets/purl/1829677.
@article{osti_1829677,
title = {Equation-of-Motion Coupled-Cluster Cumulant Green’s Function for Excited States and X-ray Spectra},
author = {Vila, Fernando D. and Kas, Joshua J. and Rehr, John J. and Kowalski, Karol and Peng, Bo},
abstractNote = {Green’s function methods within many-body perturbation theory provide a general framework for treating electronic correlations in excited states and spectra. Conventional methods using the Dyson equation or the cumulant expansion are typically based on the GW self-energy approximation. In order to extend this approximation in molecular systems, a non-perturbative real-time coupled-cluster cumulant Green’s function approach has been introduced, where the cumulant is obtained as the solution to a set of coupled first order, non-linear differential equations. This approach naturally includes non-linear corrections to conventional cumulant Green’s function techniques where the cumulant is linear in the GW self-energy. The method yields the spectral function associated with the core Green’s function, which is directly related to the x-ray photoemission spectra (XPS) of molecular systems. The approach also yields very good results for binding energies and satellite excitations. The x-ray absorption spectrum (XAS) is then obtained as a convolution of the core spectral function and an effective one-body absorption spectrum. Here this approach is extended to include the full coupled-cluster-singles (CCS) core Green’s function by including the complete form of the non-linear contributions to the cumulant as well as all single, double, and triple cluster excitations in the CC amplitude equations. This approach naturally builds in orthogonality and shake-up effects analogous to those in the Mahan-Noizeres-de Dominicis edge singularity corrections that enhance the XAS near the edge. Themethod is illustrated for the XPS and XAS of NH3.},
doi = {10.3389/fchem.2021.734945},
journal = {Frontiers in Chemistry},
number = ,
volume = 9,
place = {United States},
year = {Wed Sep 22 00:00:00 EDT 2021},
month = {Wed Sep 22 00:00:00 EDT 2021}
}
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