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Selfconsistent random phase approximation methods
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DOI：10.1063/5.0056565.png)
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Abstract
En 中文
This Perspective reviews recent efforts toward selfconsistent calculations of ground-state energies within the random phase approximation (RPA) in the (generalized) Kohn-Sham (KS) density functional theory context. Since the RPA correlation energy explicitly depends on the non-interacting KS potential, an additional condition to determine the energy as a functional of the density is necessary. This observation leads to the concept of functional selfconsistency (FSC), which requires that the KS density equals the interacting density defined as the functional derivative of the ground-state energy with respect to the external potential. While all existing selfconsistent RPA schemes violate FSC, the recent generalized KS semicanonical projected RPA (GKS-spRPA) method takes a step toward satisfying it. This leads to systematic improvements in densities, binding energy curves, reference state stability, and molecular properties compared to non-selfconsistent RPA as well as optimized effective potential RPA. GKS-spRPA orbital energies accurately approximate valence and core ionization potentials, and even electron affinities of non-valence bound anions. The computational cost and performance of GKS-spRPA are compared to those of related selfconsistent schemes, including GW and orbital optimization methods, and limitations are discussed. Large differences between KS and interacting densities observed in the absence of FSC and the well-rounded performance of GKS-spRPA suggest that the KS potential as a density functional should be defined via the FSC condition for explicitly potential-dependent density functionals.
Keywords:
DENSITY-FUNCTIONAL THEORY
CORRELATED MOLECULAR CALCULATIONS
CONSISTENT BASIS-SETS
GAUSSIAN-BASIS SETS
EXCHANGE-CORRELATION ENERGY
CONVERGENT BASIS-SETS
ELECTRON-GAS
HARTREE-FOCK
POTENTIALS
EQUATIONS
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