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An efficient all-electron G$^0$W$^0$ method and a quasiparticle selfconsistent GW (QSGW) method for molecules are proposed in the molecular orbital space with the full random phase approximation. The convergence with basis set is examined.…

Mesoscale and Nanoscale Physics · Physics 2015-03-17 San-Huang Ke

Core-electron x-ray photoelectron spectroscopy is a powerful technique for studying the electronic structure and chemical composition of molecules, solids and surfaces. However, the interpretation of measured spectra and the assignment of…

Materials Science · Physics 2019-10-23 J. Matthias Kahk , Johannes Lischner

We apply the renormalized singles with correlation (RSc) Green's function in the $GW$ approximation to calculate accurate quasiparticle (QP) energies and orbitals. The RSc Green's function includes all orders of singles contributions from…

Chemical Physics · Physics 2022-10-19 Jiachen Li , Weitao Yang

Two self-consistent schemes involving Hedin's $GW$ approximation are studied for a set of sixteen different atoms and small molecules. We compare results from the fully self-consistent $GW$ approximation (SC$GW$) and the quasi-particle…

Materials Science · Physics 2015-06-19 Peter Koval , Dietrich Foerster , Daniel Sánchez-Portal

This paper describes an all-electron implementation of the self-consistent GW (sc-GW) approach -- i.e. based on the solution of the Dyson equation -- in an all-electron numeric atom-centered orbital (NAO) basis set. We cast Hedin's…

Materials Science · Physics 2013-08-12 Fabio Caruso , Patrick Rinke , Xinguo Ren , Angel Rubio , Matthias Scheffler

The GW approximation is widely used for reliable and accurate modeling of single-particle excitations. It also serves as a starting point for many theoretical methods, such as its use in the Bethe-Salpeter equation (BSE) and dynamical…

Computational Physics · Physics 2024-03-25 Weiwei Gao , Zhao Tang , Jijun Zhao , James R. Chelikowsky

Ab initio many-body perturbation theory within the $GW$ approximation is a Green's function formalism widely used in the calculation of quasiparticle excitation energies of solids. In what has become an increasingly standard approach,…

We present theoretical calculations of quasiparticle energies in closed-shell molecules using the GW method. We compare three different approaches: a full-frequency $G_0W_0$ (FF-$G_0W_0$) method with density functional theory (DFT-PBE) used…

Materials Science · Physics 2015-06-22 Johannes Lischner , Sahar Sharifzadeh , Jack Deslippe , Jeffrey B. Neaton , Steven G. Louie

Although the GW approximation is recognized as one of the most accurate theories for predicting materials excited states properties, scaling up conventional GW calculations for large systems remains a major challenge. We present a powerful…

Computational Physics · Physics 2018-03-28 Weiwei Gao , Weiyi Xia , Xiang Gao , Peihong Zhang

We combine the renormalized singles (RS) Green's function with the T-Matrix approximation for the single-particle Green's function to compute quasiparticle energies for valence and core states of molecular systems. The $G_{\text{RS}}T_0$…

Chemical Physics · Physics 2021-08-05 Jiachen Li , Zehua Chen , Weitao Yang

We introduce an alternative route to quasiparticle self-consistent $GW$ calculations ($\mathrm{qs}GW$) on the basis of a Joint Approximate Diagonalization of the one-body $GW$ Green's functions $G(\varepsilon_n^{QP})$ taken at the input…

Materials Science · Physics 2024-12-05 Ivan Duchemin , Xavier Blase

We present a tight-binding based GW approach for the calculation of quasiparticle energy levels in confined systems such as molecules. Key quantities in the GW formalism like the microscopic dielectric function or the screened Coulomb…

Materials Science · Physics 2009-11-10 T. A. Niehaus , M. Rohlfing , F. Della Sala , A. Di Carlo , Th. Frauenheim

In recent years, Green's function methods have garnered considerable interest due to their ability to target both charged and neutral excitations. Among them, the well-established $GW$ approximation provides accurate ionization potentials…

Chemical Physics · Physics 2023-08-31 Enzo Monino , Pierre-François Loos

X-ray photoelectron spectroscopy (XPS) measures electron removal energies, providing direct access to core and valence electron binding energies, hence probing the electronic structure. In this work, we benchmark for the first time the ab…

Other Condensed Matter · Physics 2023-10-11 Iskander Mukatayev , Benoît Sklénard , Valerio Olevano , Jing Li

GW calculations with fully self-consistent G and W -- based on the iterative solution of the Dyson equation -- provide an approach for consistently describing ground and excited states on the same quantum mechanical level. We show that for…

Materials Science · Physics 2012-09-27 Fabio Caruso , Patrick Rinke , Xinguo Ren , Matthias Scheffler , Angel Rubio

We report an all-electron, atomic orbital (AO) based, two-component (2C) implementation of the $GW$ approximation (GWA) for closed-shell molecules. Our algorithm is based on the space-time formulation of the GWA and uses analytical…

Chemical Physics · Physics 2023-09-11 Arno Förster , Erik van Lenthe , Edoardo Spadetto , Lucas Visscher

We report quasiparticle-energy calculations of the electronic bandstructure as measured by valence-band photoemission for selected II-VI compounds and group-III-nitrides. By applying GW as perturbation to the ground state of the fictitious,…

Materials Science · Physics 2009-11-11 Patrick Rinke , Abdallah Qteish , Joerg Neugebauer , Christoph Freysoldt , Matthias Scheffler

The many-body $GW$ formalism, for the calculation of ionization potentials or electronic affinities, relies on the frequency-dependent dielectric function built from the electronic degrees of freedom. Considering the case of water as a…

Materials Science · Physics 2024-09-04 Ivan Duchemin , David Amblard , Xavier Blase

While highly successful, density functional theory is known to have limitations owing to its neglect of many-body electron-electron interactions. This neglect leads to errors in the single-particle energies, leading to underestimated band…

Materials Science · Physics 2026-04-16 John Vinson , Terrence Jach , Rainer Unterumsberger , Michael A. Woodcox , Burkhard Beckhoff

Photoelectron spectra of early $3d-$transition metal dioxide anions, ScO$_{2}^-$, TiO$_{2}^-$, VO$_{2}^-$, CrO$_{2}^-$, MnO$_{2}^-$, are calculated using semilocal and hybrid density functional theory (DFT) and many-body perturbation theory…

Materials Science · Physics 2021-03-17 Meisam Rezaei , Serdar Öğüt