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arXiv:2312.04154 · Journal of Chemical Theory and Computation

Total Energy beyond GW: Exact Results and Guidelines for Approximations

Abdallah El-Sahili, Francesco Sottile, Lucia Reining

Published Feb 7, 2024• 5 citations
arXivHTMLPDF

Abstract

The total energy and electron addition and removal spectra can, in principle, be obtained exactly from the one-body Green's function (GF). In practice, the GF is obtained from an approximate self-energy. In the framework of many-body perturbation theory, we derive different expressions that are based on an approximate self-energy, but that yield nevertheless, in principle, the exact exchange-correlation contribution to the total energy for any interaction strength. Response functions play a crucial role, which explains why, for example, ingredients from time-dependent density functional theory can be used to build these approximate self-energies. We show that the key requirement for obtaining exact results is the consistent combination of ingredients. Also when further approximations are made, as it is necessary in practice, this consistency remains the key to obtain good results. All findings are illustrated using the exactly solvable symmetric Hubbard dimer.

DOI
10.1021/acs.jctc.3c01200

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The total energy and electron addition and removal spectra can, in principle, be obtained exactly from the one-body Green's function (GF). In practice, the GF is obtained from an approximate self-energy. In the framework of many-body perturbation theory, we derive different expressions that are based on an approximate self-energy, but that yield nevertheless, in principle, the exact exchange-correlation contribution to the total energy for any interaction strength. Response functions play a crucial role, which explains why, for example, ingredients from time-dependent density functional theory can be used to build these approximate self-energies. We show that the key requirement for obtaining exact results is the consistent combination of ingredients. Also when further approximations are made, as it is necessary in practice, this consistency remains the key to obtain good results. All findings are illustrated using the exactly solvable symmetric Hubbard dimer.
In this lecture we present many-body perturbation theory as a method to determine quasiparticle excitations in solids, especially electronic band structures, accurately from first principles.The main ingredient is the electronic self-energy that, in principle, contains all many-body exchange and correlation effects beyond the Hartree potential.As its exact mathematical expression is unknown, approximations must be used in practical calculations.The approximation is obtained using a systematic algebraic approach on the basis of Green function techniques.It constitutes an expansion of the self-energy up to linear order in the screened Coulomb potential, which describes the interaction between the quasiparticles and includes dynamic screening through the creation of exchange-correlation holes around the bare particles.The implementation of the approximation relies on a perturbative treatment starting from density functional theory.Besides a detailed mathematical discussion we focus on the underlying physical concepts and show some illustrative applications.
In many-body perturbation theory (MBPT) the self-energy $\ensuremath{\Sigma}=iGW\ensuremath{\Gamma}$ plays a key role since it contains all the many-body effects of the system. The exact self-energy is not known; as a first approximation one can set the vertex function $\ensuremath{\Gamma}$ to unity which leads to the GW approximation. The latter properly describes the high-density regime, where screening is important; in the low-density regime, instead, other approximations are proposed, such as the TTT matrix, which describes multiple scattering between two particles. Here we combine the two approaches. Starting from the fundamental equations of MBPT, we show how one can derive the TTT-matrix approximation to the self-energy in a common framework with GWGWGW. This allows us to elucidate several aspects of this formulation, including the origin of, and link between, the electron-hole and the particle-particle TTT matrix, the derivation of a screened TTT matrix, and the conversion of the TTT matrix into a vertex correction. The exactly solvable Hubbard molecule is used for illustration.
It is commonly accepted that the GW approximation for the electron self-energy is successful for the description of the band structure of weakly to moderately correlated systems, whereas it will fail for strongly correlated materials. In the present work, we discuss two important aspects of this approximation: first, the "self-screening error," which is due to an incorrect treatment of induced exchange, and second, the atomic limit, in which, instead, correlation is directly responsible for the observed problem. Using the example of the removal of a particle from a box, we show that the self-screening error stems from the use of test charge-test charge screening and that it can be corrected by a two-point vertex contribution to the self-energy derived from time-dependent density functional theory (TDDFT). We explain why the addition of a particle, instead, requires the use of a different approximate vertex. This illustrates why the general vertex function, valid both for valence and conduction states, must be a three-point function. Moreover, we show that also the bad performance of GW in the atomic limit is due to the neglect of the vertex in the self-energy; in that case, the TDDFT-derived vertex correction is not sufficient in order to remove the error even qualitatively. We discuss the effects of the self-screening error as well as the atomic limit using GW for the exactly solvable two-site Hubbard model.
Several widely used methods for the calculation of band structures and photo emission spectra, such as the GW approximation, rely on many-body perturbation theory. They can be obtained by iterating a set of functional differential equations (DEs) relating the one-particle Green's function (GF) to its functional derivative with respect to an external perturbing potential. In this work, we apply a linear response expansion in order to obtain insights into various approximations for GF calculations. The expansion leads to an effective screening while keeping the effects of the interaction to all orders. In order to study various aspects of the resulting equations, we discretize them and retain only one point in space, spin and time for all variables. Within this one-point model we obtain an explicit solution for the GF, which allows us to explore the structure of the general family of solutions and to determine the specific solution that corresponds to the physical one. Moreover, we analyze the performances of established approaches like GW over the whole range of interaction strength, and we explore alternative approximations. Finally, we link certain approximations for the exact solution to the corresponding manipulations of the DE which produces them. This link is crucial in view of a generalization of our findings to the real (multidimensional functional) case where only the DE is known.
The well-known and well-used Density Functional Theory (DFT) is a variational theory for the ground-state. There are no guarantees that it delivers good results for excited state properties such as quasiparticle energies or wave function. All that is guaranteed is that the total energy is exact, the chemical potential is correct, and that the eective electronic states (Kohn-Sham states) generate the right electron density at the variational minimum. Luttinger-Ward approaches to electronic structure are attractive as beyond-DFT schemes since, in principle, they oer a variational functional of the one-electron Green’s function that yields both the correct total energy and all one-particle properties at the variational extremum. However, compared to DFT, these methods face a number of additional challenges beyond the familiar problem of choosing an exchange-correlation functional: (a) they have a much greater computational cost compared to DFT, (b) one must choose some set of trial Green’s functions, and (c) one must locate an extremum (not necessarily a minimum). This talk aims both to be pedagogical and to provide a summary of our most recent work in this area. We focus mainly on the random-phase approximation (RPA) for the correlation functional which yields the GW self-energy for the Green’s function. We will describe ecient approaches for computing the RPA correlation energy; how various types of approximations to the correlation energy create a ladder of approximate self-energy operators and what type of physics is included in these approximations (exchange, screening, Hubbard U, etc.); and how the extremization is in fact highly problematic. We will end with some ideas for making practical progress with the extremization and their relation to the successful Quasiparticle Self-consistent GW (QSGW) scheme [1].
Many-body perturbation theory is a powerful framework to calculate spectroscopic quantities, as well as the total energy. However, the field suffers from the fact that different flavors of approximations lead to a wide range of results. We present several in principle exact expansions and discuss how to use them consistently. We concentrate on the first two orders in the respective screened Coulomb interaction. Of special interest is a consistent expansion around the Kohn-Sham system. We illustrate the performance of the various choices using the symmetric Hubbard dimer over a wide range of correlation strength. In particular, the expansion based on exact Kohn-Sham ingredients stands out as a promising route towards good energies and good spectra.