Renormalized Singles Green’s Function for Quasi-Particle Calculations beyond the G0W0 Approximation

Jin, Ye; Su, Neil Qiang; Yang, Weitao

doi:10.1021/acs.jpclett.8b03337

Cited by 28 publications

(114 citation statements)

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“…This beckons for a judicious choice of the starting point in G 0 W 0 calculations or an elimination of the starting point dependence. The dependence on the preceding mean-field calculation can be eliminated or reduced by employing some form of self-consistency as discussed in section 5 or, as proposed only very recently, by replacing G 0 by a renormalized singles Green's function (Jin et al, 2019). In this section we focus on the optimal choice of the starting point.…”

Section: The G0w0 Approach: Concept and Implementationmentioning

confidence: 99%

The GW Compendium: A Practical Guide to Theoretical Photoemission Spectroscopy

2019

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The GW approximation in electronic structure theory has become a widespread tool for predicting electronic excitations in chemical compounds and materials. In the realm of theoretical spectroscopy, the GW method provides access to charged excitations as measured in direct or inverse photoemission spectroscopy. The number of GW calculations in the past two decades has exploded with increased computing power and modern codes. The success of GW can be attributed to many factors: favorable scaling with respect to system size, a formal interpretation for charged excitation energies, the importance of dynamical screening in real systems, and its practical combination with other theories. In this review, we provide an overview of these formal and practical considerations. We expand, in detail, on the choices presented to the scientist performing GW calculations for the first time. We also give an introduction to the many-body theory behind GW , a review of modern applications like molecules and surfaces, and a perspective on methods which go beyond conventional GW calculations. This review addresses chemists, physicists and material scientists with an interest in theoretical spectroscopy. It is intended for newcomers to GW calculations but can also serve as an alternative perspective for experts and an up-to-date source of computational techniques.

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Section: The G0w0 Approach: Concept and Implementationmentioning

confidence: 99%

The GW Compendium: A Practical Guide to Theoretical Photoemission Spectroscopy

2019

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“…Several studies have focused on the possibility of addressing this issue (see, among the others, Ref. [207]), trying to eliminate the dependence [208] which may lead to large discrepancies between calculated and experimental values, in terms of bandgap/band edge (and relative deeper states) values. An alternative procedure to the one-shot G 0 W 0 is the eigenvalues update in the Green's function G only, keeping the screening Coulomb part as obtained from DFT (GW 0 approximation) or the full update, i.e.…”

Section: Beyond the Single-particle Hamiltonian: Including Many-body And Excitonic Effectsmentioning

confidence: 99%

Modeling of plasmonic properties of nanostructures for next generation solar cells and beyond

Manzhos

Giorgi

Lüder

et al. 2021

Advances in Physics: X

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Plasmonic particles and nanostructures are widely used in photovoltaic and photonics. Surface plasmons were found to enhance different types of solar cells including plasmonic DSSCs, plasmonic solid semiconductor solar cells, plasmonic organic solar cells, and plasmonic perovskite solar cell. Size, composition, and shape of plasmonic nanoparticles as well as nanometer-distance control between particles are key design factors of plasmonic nanostructures. Modeling is rapidly gaining in importance for mechanistic understanding and rational design of plasmonic nanostructures. We review the modeling approaches used to model plasmon resonance features of nanostructures, from classical approaches that can routinely handle most particle sizes used in solar cells to approaches beyond classical electrodynamics such as ab initio approaches based on time-dependent density functional theory (TD-DFT). We highlight recently emerging approaches which have the potential to significantly enhance modeling capabilities in the coming years, in particular, by allowing atomistic (ab initio) modeling at realistic length scales, i.e. of particle sizes beyond 10 nm which are of most interest to plasmonic solar cells but remain problematic with traditional DFT-based techniques, such as density functional tight binding (DFTB) based approaches, time-dependent orbital-free DFT, and machine learning-based approaches, as well as many-body perturbation theory which is expected to gain usage with advances in computing power.

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“…The RS Green's function constructed with RS eigenvalues is shown to predict accurate quasiparticle energies for valence states in the GW method as well as valence and core states in the T-matrix methods. 41,44 The RS Green's function shares a similar thinking as the renormalized single-excitation (rSE) correction in the random phase approximation (RPA) calculations for the correlation energy. 13,45 The accuracy of RPA with rSE calculations for predicting binding energies of rare-gas dimers is significantly improved.…”

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confidence: 99%

“…In the present work, to overcome the first challenge, we applied renormalized singles (RS) in the multireference DFT. RS was developed to provide a good starting point in the GW calculations, 41 which is the RS Green's function. The motivation of the RS Green's function is to use the form of the Hartree-Fock 42,43 (HF) self-energy to include all singles contributions.…”

mentioning

confidence: 99%

“…However, the HF Green's function itself is not a good starting point for GW calculations. 41 Therefore, the HF Hamiltonian is constructed with KS orbitals and diagonalized separately in the occupied and virtual subspaces of the DFA used. This renormalization procedure absorbs all singles contributions into the self-energy to eliminate the dependence on the choice of the DFA.…”

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confidence: 99%

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Multireference Density Functional Theory for Describing Ground and Excited States with Renormalized Singles

Li,

Chen,

Yang

2021

Preprint

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We applied renormalized singles (RS) in the multireference density functional theory (DFT) approach to calculate accurate electronic energies of ground states and excited states for molecular systems. The multireference DFT approach, developed recently, determines the total energy of the N -electron system as the sum of the (N − 2)electron energy from a density functional approximation (DFA) and the two-electron addition excitation energies from the particle-particle Tamm-Dancoff approximation (ppTDA) linear response approach. The ppTDA@RS-DFA approach first constructs the RS Hamiltonian to capture all singles contributions of the (N −2)-electron auxiliary system described by a chosen DFA. Then the RS Hamiltonian is used in ppTDA to calculate two-electron addition excitation energies. The total energy is optimized with the optimized effective potential (OEP) method. The multireference description of both the ground and excited states of the N -electron systems comes naturally through the linear response theory. We show that the ppTDA@RS-DFA approach provides considerable improvement over the ppTDA@DFA, the original approach without using RS, and describes both ground state and excited state properties accurately, with electron densities preserving the proper symmetry for systems having strong (static) correlation. For ground states, ppTDA@RS-DFA properly describes dissociation energies, equilibrium bond lengths and the dissociation curves of all tested molecules, and the double bond rotation of ethylene. For excited states, ppTDA@RS-DFA provides accurate excitation energies of molecular systems and largely eliminates the dependence on the choice of the DFA. ppTDA@RS-DFA thus provides a promising and very efficient multireference approach to systems with static correlation.

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Renormalized Singles Green’s Function for Quasi-Particle Calculations beyond the G₀W₀ Approximation

Cited by 28 publications

References 40 publications

The GW Compendium: A Practical Guide to Theoretical Photoemission Spectroscopy

The GW Compendium: A Practical Guide to Theoretical Photoemission Spectroscopy

Modeling of plasmonic properties of nanostructures for next generation solar cells and beyond

Multireference Density Functional Theory for Describing Ground and Excited States with Renormalized Singles

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