DiStasio, Robert A. and von Lilienfeld, O. Anatole and Tkatchenko, Alexandre. (2012) Collective many-body van der Waals interactions in molecular systems. Proceedings of the National Academy of Sciences of the United States of America, 109 (37). pp. 14791-14795.
Full text not available from this repository.
Official URL: http://edoc.unibas.ch/43359/
Downloads: Statistics Overview
Abstract
Van der Waals (vdW) interactions are ubiquitous in molecules and condensed matter, and play a crucial role in determining the structure, stability, and function for a wide variety of systems. The accurate prediction of these interactions from first principles is a substantial challenge because they are inherently quantum mechanical phenomena that arise from correlations between many electrons within a given molecular system. We introduce an efficient method that accurately describes the nonadditive many-body vdW energy contributions arising from interactions that cannot be modeled by an effective pairwise approach, and demonstrate that such contributions can significantly exceed the energy of thermal fluctuations--a critical accuracy threshold highly coveted during molecular simulations--in the prediction of several relevant properties. Cases studied include the binding affinity of ellipticine, a DNA-intercalating anticancer agent, the relative energetics between the A- and B-conformations of DNA, and the thermodynamic stability among competing paracetamol molecular crystal polymorphs. Our findings suggest that inclusion of the many-body vdW energy is essential for achieving chemical accuracy and therefore must be accounted for in molecular simulations.
Faculties and Departments: | 05 Faculty of Science > Departement Chemie > Former Organization Units Chemistry > Physikalische Chemie (Lilienfeld) |
---|---|
UniBasel Contributors: | von Lilienfeld, Anatole |
Item Type: | Article, refereed |
Article Subtype: | Research Article |
Publisher: | National Academy of Sciences |
ISSN: | 0027-8424 |
e-ISSN: | 1091-6490 |
Note: | Publication type according to Uni Basel Research Database: Journal article |
Identification Number: |
|
Last Modified: | 14 Oct 2016 14:38 |
Deposited On: | 20 Jun 2016 09:50 |
Repository Staff Only: item control page