molgw 1: Many-body perturbation theory software for atoms, molecules, and clusters

Bruneval, Fabien; Rangel, Tonatiuh; Hamed, Samia M.; Shao, Meiyue; Yang, Chao; Neaton, Jeffrey B.

doi:10.1016/j.cpc.2016.06.019

Cited by 175 publications

(250 citation statements)

References 94 publications

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“…To better illustrate these points Fig. 20 shows the ionisation potential of 3d tran-sition metal atoms and the heat of formation of 3d-O dimers, computed by the molgw code [93]. We focus on these properties because it is known, e.g.…”

Section: Need For Self-consistencymentioning

confidence: 99%

Questaal: A package of electronic structure methods based on the linear muffin-tin orbital technique

Pashov

Acharya

Lambrecht

et al. 2020

Computer Physics Communications

115

113

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This paper summarises the theory and functionality behind Questaal, an open-source suite of codes for calculating the electronic structure and related properties of materials from first principles. The formalism of the linearised muffin-tin orbital (LMTO) method is revisited in detail and developed further by the introduction of short-ranged tight-binding basis functions for full-potential calculations. The LMTO method is presented in both Green's function and wave function formulations for bulk and layered systems. The suite's full-potential LMTO code uses a sophisticated basis and augmentation method that allows an efficient and precise solution to the band problem at different levels of theory, most importantly density functional theory, LDA+U , quasi-particle self-consistent GW and combinations of these with dynamical mean field theory. This paper details the technical and theoretical bases of these methods, their implementation in Questaal, and provides an overview of the code's design and capabilities. framework of an extension to the linear muffin-tin orbital (LMTO) technique including a highly precise and efficient full-potential implementation. An advanced fully-relativistic, non-collinear implementation based on the atomic sphere approximation is used for calculating transport and magnetic properties.

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Section: Need For Self-consistencymentioning

confidence: 99%

Questaal: A package of electronic structure methods based on the linear muffin-tin orbital technique

Pashov

Acharya

Lambrecht

et al. 2020

Computer Physics Communications

115

113

View full text Add to dashboard Cite

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“…The Greek letters represent the basis functions for the wavefunction, whereas the capitals P and Q run over an auxiliary basis set. In practice, we use an approach 73 in which the square root of the matrix (P | 1 r |Q) is calculated and thus the evaluation of Eq. (6) is further accelerated.…”

mentioning

confidence: 99%

Evaluating theGWApproximation with CCSD(T) for Charged Excitations Across the Oligoacenes

Rangel

Hamed

Bruneval

et al. 2016

J. Chem. Theory Comput.

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101

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Charged excitations of the oligoacene family of molecules, relevant for astrophysics and technological applications, are widely studied and therefore provide an excellent system for benchmarking theoretical methods. In this work, we evaluate the performance of many-body perturbation theory (MPBT) within the GW approximation, relative to new high-quality CCSD(T) reference data, for charged excitations of the acenes. We compare GW calculations with a number of hybrid density functional theory starting points and with eigenvalue selfconsistency. Special focus is given to elucidating the trend of GW -predicted excitations with molecule length, from benzene to hexacene. We find that GW calculations with starting points based on an optimally-tuned range separated hybrid (OTRSH) density functional and eigenvalue self-consistency can yield quantitative ionization potentials for the acenes. However, for the larger acenes, the predicted electron affinities can deviate considerably from reference values. Our work paves the way for predictive and cost-effective GW calculations of chargedexcitations of molecules and identifies certain limitations of current GW methods used in practice for larger molecules.

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“…The basis set convergence of GW and BSE calculations has been studied and reported extensively in Refs. 29,36,42,51,52 We first analyzed the basis set convergence of both G 0 W 0 and BSE calculations, on a small set of eight organic molecules that constitute the cyclometalated complexes under study, using the B3LYP functional. The molecules are reported in Fig.…”

Section: Basis Set Convergencementioning

confidence: 99%

Ab Initio Many-Body Perturbation Theory Calculations of the Electronic and Optical Properties of Cyclometalated Ir(III) Complexes

Cazzaniga¹,

Cargnoni²,

Penconi³

et al. 2019

J. Chem. Theory Comput.

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Cyclometalled Ir(III) compounds are the preferred choice as organic emitters in Organic Light Emitting Diodes. In practice, the presence of the transition metals surrounded by carefully designed ligands allows the fine tuning of the emission frequency as well as a good efficiency of the device. To support the development of new compounds the experimental measurements are generally compared with ab-initio calculation of the absorption and emission spectra. The standard approach for these calculations is TDDFT with hybrid exchange and correlation functional like the B3LYP. Due to the size of these compounds the application of more complex quantum chemistry approaches can be challenging. In this work we used Many Body Perturbation Theory approaches (in particular the GW approximation with the Bethe-Salpeter equation) 1 arXiv:2001.01959v1 [cond-mat.mtrl-sci] 7 Jan 2020 implemented in gaussian basis sets, to calculate the quasiparticle properties and the adsorption spectra of six cyclometalled Ir(III) complexes going behind TDDFT. In the presented results we compared standard TDDFT simulation with BSE calculations performed on top on perturbative G 0 W 0 and accounting for eigenvalue self consistency.Moreover, in order to investigate in detail the effect of the DFT starting point, we concentrate on Ir(ppy) 3 performing GW-BSE simulations starting from different DFT exchange and correlation potentials.

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molgw 1: Many-body perturbation theory software for atoms, molecules, and clusters

Cited by 175 publications

References 94 publications

Questaal: A package of electronic structure methods based on the linear muffin-tin orbital technique

Questaal: A package of electronic structure methods based on the linear muffin-tin orbital technique

Evaluating theGWApproximation with CCSD(T) for Charged Excitations Across the Oligoacenes

Ab Initio Many-Body Perturbation Theory Calculations of the Electronic and Optical Properties of Cyclometalated Ir(III) Complexes

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