Reference : Understanding Molecular Crystals with Dispersion-Inclusive Density Functional Theory:...
Scientific journals : Article
Physical, chemical, mathematical & earth Sciences : Chemistry
http://hdl.handle.net/10993/25674
Understanding Molecular Crystals with Dispersion-Inclusive Density Functional Theory: Pairwise Corrections and Beyond
-
Kronik, Leeor [Department of Materials and Interfaces, Weizmann Institute of Science, Rehovoth 76100, Israel]
Tkatchenko, Alexandre mailto [Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany]
2014
ACCOUNTS OF CHEMICAL RESEARCH
AMER CHEMICAL SOC
47
11, SI
3208-3216
Yes (verified by ORBilu)
International
0001-4842
1155 16TH ST, NW, WASHINGTON, DC 20036 USA
[en] Molecular crystals are ubiquitous in many areas of science and engineering, including biology and medicine. Until recently, our ability to understand and predict their structure and properties using density functional theory was severely limited by the lack of approximate exchangecorrelation functionals able to achieve sufficient accuracy. Here we show that there are many cases where the simple, minimally empirical pairwise correction scheme of Tkatchenko and Scheffler provides a useful prediction of the structure and properties of molecular crystals. After a brief introduction of the approach, we demonstrate its strength through some examples taken from our recent work. First, we show the accuracy of the approach using benchmark data sets of molecular complexes. Then we show its efficacy for structural determination using the hemozoin crystal, a challenging system possessing a wide range of strong and weak binding scenarios. Next, we show that it is equally useful for response properties by considering the elastic constants exhibited by the supramolecular diphenylalanine peptide solid and the infrared signature of water libration movements in brushite. Throughout, we emphasize lessons learned not only for the methodology but also for the chemistry and physics of the crystals in question. We further show that in many other scenarios where the simple pairwise correction scheme is not sufficiently accurate, one can go beyond it by employing a computationally inexpensive many-body dispersive approach that results in useful, quantitative accuracy, even in the presence of significant screening and/or multibody contributions to the dispersive energy. We explain the principles of the many-body approach and demonstrate its accuracy for benchmark data sets of small and large molecular complexes and molecular solids.
http://hdl.handle.net/10993/25674
10.1021/ar500144s
Review

File(s) associated to this reference

Fulltext file(s):

FileCommentaryVersionSizeAccess
Limited access
Understanding Molecular Crystals with Dispersion-Inclusive Density-Functional Theory: Pairwise Corrections and Beyond.pdfPublisher postprint3.34 MBRequest a copy

Bookmark and Share SFX Query

All documents in ORBilu are protected by a user license.