Long-range correlation energy calculated from coupled atomic response functions.

By A. Ambrosetti, Anthony Reilly, Robert A. Distasio Jr., Alexandre Tkatchenko. Journal of Chemical Physics, 2013

595 citations recorded by the source corpus.

An accurate determination of the electron correlation energy is an essential prerequisite for describing the structure, stability, and function in a wide variety of systems. Therefore, the development of efficient approaches for the calculation of the correlation energy (and hence the dispersion energy as well) is essential and such methods can be coupled with many density-functional approximations, local methods for the electron correlation energy, and even interatomic force fields. In this work, we build upon the previously developed many-body dispersion (MBD) framework, which is intimately linked to the random-phase approximation for the correlation energy. We separate the correlation energy into short-range contributions that are modeled by semi-local functionals and long-range contributions that are calculated by mapping the complex all-electron problem onto a set of atomic response functions coupled in the dipole approximation. We propose an effective range-separation of the coupling between the atomic response functions that extends the already broad applicability of the MBD method to non-metallic materials with highly anisotropic responses, such as layered nanostructures. Application to a variety of high-quality benchmark datasets illustrates the accuracy and applicability of the improved MBD approach, which offers the prospect of first-principles modeling of large structurally complex systems with an accurate description of the long-range correlation energy.

Subfields: Atomic and Molecular Physics, and Optics, Materials Chemistry, Structural Biology

View Paper: https://www.semanticscholar.org/paper/7b7dc3dc18655935b3c668dd551e4587f607aa49

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In Atomic and Molecular Physics, and Optics

In Materials Chemistry

Citations in the corpus

Materials perspective on Casimir and van der Waals interactions (2015, methodology): “For example, for polarizable supramolecular systems, such as the “buckyball catcher” complex, pairwise dispersion corrections overestimate the binding energy by 0.4–0.6 eV (Tkatchenko et al., 2012a) compared to reference DQMC values.”