Accurate and efficient method for many-body van der Waals interactions.
By Alexandre Tkatchenko, Robert A. Distasio Jr., Roberto Car, Matthias Scheffler. 2012
1,053 citations recorded by the source corpus.
An efficient method is developed for the microscopic description of the frequency-dependent polarizability of finite-gap molecules and solids. This is achieved by combining the Tkatchenko-Scheffler van der Waals (vdW) method [Phys. Rev. Lett. 102, 073005 (2009)] with the self-consistent screening equation of classical electrodynamics. This leads to a seamless description of polarization and depolarization for the polarizability tensor of molecules and solids. The screened long-range many-body vdW energy is obtained from the solution of the Schrödinger equation for a system of coupled oscillators. We show that the screening and the many-body vdW energy play a significant role even for rather small molecules, becoming crucial for an accurate treatment of conformational energies for biomolecules and binding of molecular crystals. The computational cost of the developed theory is negligible compared to the underlying electronic structure calculation.
Subfields: Atomic and Molecular Physics, and Optics
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In Atomic and Molecular Physics, and Optics
- Alexandre Tkatchenko
- Grgoire Montavon
- O. A. von Lilienfeld
- Matthias Rupp
- T. Bereau
- O. V. Lilienfeld
- Klaus‐Robert Müller
- T. Thonhauser
Citations in the corpus
- Machine learning of molecular electronic properties in chemical compound space (2013, methodology): “Polarizabilities, calculated using PBE0, or with the more approximate self-consistent screening (SCS) model29, are strongly correlated.”
- van der Waals forces in density functional theory: a review of the vdW-DF method (2014, methodology): “The expansion (54) implies that the popular vdW-DF versions, unlike RPA and unlike the vdW-DF framework [109], cannot account for many-body dispersion effects [51, 149, 190, 203, 204] at every length scale.”
- Collective many-body van der Waals interactions in molecular systems (2012, methodology): “Therefore, the adjustment of a single physically motivated rangeseparation parameter allows the vdW-MB method to be coupled to a wide array of theoretical methods, ranging from classical force fields to higher level quantum chemical calculations (26).”
- Materials perspective on Casimir and van der Waals interactions (2015, background): “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.”