Beyond the random phase approximation: Improved description of short range correlation by a renormalized adiabatic local density approximation

Abstract

We assess the performance of a recently proposed renormalized adiabatic local density approximation (rALDA) for \textit{ab initio} calculations of electronic correlation energies in solids and molecules. The method is an extension of the random phase approximation (RPA) derived from time-dependent density functional theory and the adiabatic connection fluctuation-dissipation theorem and contains no fitted parameters. The new kernel is shown to preserve the accurate description of dispersive interactions from RPA while significantly improving the description of short range correlation in molecules, insulators, and metals. For molecular atomization energies the rALDA is a factor of 7(4) better than RPA(PBE) when compared to experiments, and a factor of 3(1.5) better than RPA(PBE) for cohesive energies of solids. For transition metals the inclusion of full shell semi-core states is found to be crucial for both RPA and rALDA calculations and can improve the cohesive energies by up to 0.4 eV. Finally we discuss straightforward generalizations of the method, which might improve results even further.

arXiv commentNew version with changed results for transition metals. The new results were obtained with semi-core states included and are much closer to experimental values than previous results

References in corpus (11)

• Van der Waals Density Functional for General Geometries
• A real-space grid implementation of the Projector Augmented Wave method
• W4 theory for computational thermochemistry: in pursuit of confident sub-kJ/mol predictions
• Random-phase approximation and its applications in computational chemistry and materials science
• Dispersive and Covalent Interactions Between Graphene and Metal Surfaces from the Random Phase Approximation
• First-Principle Description of Correlation Effects in Layered Materials
• Linear density response function in the projector-augmented wave method: Applications to solids, surfaces, and interfaces
• The random phase approximation applied to solids, molecules, and graphene-metal interfaces: From weak to strong binding regimes
• Correlation energy functional and potential from time-dependent exact-exchange theory
• Extending the random-phase approximation for electronic correlation energies: The renormalized adiabatic local density approximation
• Beyond the RPA on the cheap: improved correlation energies with the efficient "Radial Exchange Hole" kernel

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