Ionized, electron-attached, and excited states of molecular systems with spin–orbit coupling: Two-component GW and Bethe–Salpeter implementations

Holzer, Christof; Klopper, Wim

doi:10.1063/1.5094244

Cited by 70 publications

(112 citation statements)

References 100 publications

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“…The total tensor space was 423151, for which the standard GW using the full spectral function was not applicable. Therefore, the calculations were performed with RI‐ GW (resolution‐of‐the‐identity GW ) employing analytic continuation for HOMO and LUMO only . The resulting orbitals about the Fermi level are presented in Figure .…”

Section: Resultsmentioning

confidence: 99%

Photoinitiated Charge Transfer in a Triangular Silver(I) Hydride Complex and Its Oxophilicity

Kruppa

Groß

Gui

et al. 2019

Chemistry A European J

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What prompted you to investigate this system?In our collaborative research center "3MET"w ea re fascinated by metal-metal interactions, which determine the photo-physical/ chemical properties of molecular transition metal complexes and are hitherto not fully understood. Inspired by previous studies on multinuclear silver hydrides and our work on bimetallic phosphinestabilized compounds, we extended the nuclearity by designing a trimetallic system that allows for direct optical excitation of a metal-centered chromophore. What was the inspiration for this cover design?In order to emphasize the UV-induced electron transfer within the [Ag 3 H] scaffold, we chose acomic style illustration which highlights the resulting enforcement of argentophilic interaction within the metal core. Having in mind the explorative spirit of the scientific field of metal complexes and its search for new frontiers, we imagined the vast expanses of the universe. Finally,i na nh omage to the 1980s film "Tron", we attempted to illustrate the abstract inner workings of aC PU running complex quantum chemical algorithms. Does the research open other avenues that you would like to investigate?One aspect of the study which surprised us is the seemingly high reactivity of odd-electron silver hydride molecular ions towards dioxygen. Consequently,w ea re very curious about their molecular/ electronic structure, envisioning their gas phase spectroscopic and theoretical characterization. We plan to probe how different ligands and other metal centers control optical properties and photoreactivity of metal hydrides also gearing towards their luminescence and ultrafast electronic dynamics in both gas phase and solution.Invited for the cover of this issue aret he research groups of Rolf Diller,G ereon Niedner-Schatteburg, Christoph Riehn and Werner R. Thiel from the TU Kaiserslautern (TUK) and the group of Wim Klopper of the KarlsruheI nstitute of Technology (KIT) collaborating within the research center "3MET" (SFB/TRR 88). The image depicts the photoinitiated charge transfer within aphosphine-stabilized triangular silver hydride complex. Read the full text of the article at

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Section: Resultsmentioning

confidence: 99%

Photoinitiated Charge Transfer in a Triangular Silver(I) Hydride Complex and Its Oxophilicity

Kruppa

Groß

Gui

et al. 2019

Chemistry A European J

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“…Single-shot G 0 W 0 , eigenvalue-only self-consistent GW (evGW) and quasiparticle self-consistent (qsGW) calculations, as implemented by Holzer, van Setten, Klopper and co-workers in Turbomole, [50][51][52] were performed on the DFT optimised structures, starting from B3LYP orbitals. These calculations used either the def2-SVP or def2-TZVPP basis-set (and in selected cases the def2-QZVPP and aug-cc-pVTZ basis-sets) and one of two GW implementations that differ in how the self-energy is obtained; in terms of a spectral representation (SR) or by analytical continuation (AC).…”

Section: Methodsmentioning

confidence: 99%

The Effect of Particle Size on the Optical and Electronic Properties of MgO Nanoparticles

Zwijnenburg

2021

Preprint

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evGW-BSE is used to predict the (band) edge states, fundamental gap, optical gap, exciton binding energy and UV-Vis absorption spectra for a series of cuboidal MgO rocksalt nanoparticles, the largest of with has 216 atoms and edges of 1 nm. The evolution of the electronic and optical properties with particle size was studied, where it was found that while the edge states and fundamental gap change with particle size, the optical gap remains essentially fixed for cuboid nanoparticles containing 48 atoms or more. The explanation for that observation is that while the optical gap is associated with an exciton that is well localised on the magnesium corner atoms and the oxygen atoms directly surrounding it, the edge states, while primarily localised on the magnesium corner atoms (electron) and oxygen corner atoms (hole), show significant delocalisation along the edges away from the corner atoms. The BSE/evGW optical gap for the smallest particles, the (MgO)4 cube, matches with that obtained independently from coupled cluster theory, while for the (MgO)32, a cube with edges of 0.6 nm, the BSE/evGW predicted excitation spectrum agrees well with the experimentally reported reflection spectra of MgO nanoparticles.

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“…Single-shot G 0 W 0 , eigenvalue-only self-consistent GW (evGW) and quasiparticle self-consistent (qsGW) calculations, as implemented by Holzer, van Setten, Klopper and co-workers in Turbomole, [50][51][52] were performed on the DFT optimised structures, starting from B3LYP orbitals and in selected case PBE 53 orbitals. These calculations used either the def2-SVP or def2-TZVPP basis-set (and in selected cases the def2-QZVPP and aug-cc-pVTZ basis-sets) and one of two GW implementations that differ in how the selfenergy is obtained; in terms of a spectral representation (SR) or by analytical continuation (AC).…”

Section: Methodsmentioning

confidence: 99%

The Effect of Particle Size on the Optical and Electronic Properties of MgO Nanoparticles

Zwijnenburg¹

2021

Preprint

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The (band) edge states, fundamental gaps, optical gaps, exciton binding energies and UV-Vis spectra for a series of cuboidal nanoparticles of the prototypical oxide magnesium oxide (MgO), the largest of with has 216 atoms and edges of 1 nm, were predicted using many-body perturbation theory (evGW-BSE). The evolution of the properties with particle size was explicitly studied. It was found that while the edge states and fundamental gap change with particle size, the optical gap remains essentially fixed for all but the smallest nanoparticles, in line with what was previously observed experimentally. The explanation for these observations is demonstrated to be that while the optical gap is associated with an exciton that is highly localised around the particle’s corner atoms, the edge states, while primarily localised on the magnesium corner atoms (electron) and oxygen corner atoms (hole), show significant delocalisation along the edges. The strong localisation of the exciton associated with the optical gap on the corner atoms is argued to also explain why the nanoparticles have a much smaller optical gaps and red-shifted spectra than bulk MgO. Finally, it is discussed how this non-quantum confinement behaviour, where the properties of the nanoparticles arise from surface defects rather than differences in localisation of edge or exciton states, appears typical of alkaline earth oxide nanoparticles, and that the true optical gap of bulk crystals of such materials is also probably the result of surface defects, even if unobservable experimentally.

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Ionized, electron-attached, and excited states of molecular systems with spin–orbit coupling: Two-component GW and Bethe–Salpeter implementations

Cited by 70 publications

References 100 publications

Photoinitiated Charge Transfer in a Triangular Silver(I) Hydride Complex and Its Oxophilicity

Photoinitiated Charge Transfer in a Triangular Silver(I) Hydride Complex and Its Oxophilicity

The Effect of Particle Size on the Optical and Electronic Properties of MgO Nanoparticles

The Effect of Particle Size on the Optical and Electronic Properties of MgO Nanoparticles

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