Article (Scientific journals)
Understanding non-covalent interactions in larger molecular complexes from first principles
Al-Hamdani, Yasmine; Tkatchenko, Alexandre
2019In Journal of Chemical Physics, 150, p. 010901
Peer Reviewed verified by ORBi
 

Files


Full Text
140-perspective-on-noncovalent-interactions-in-large-molecules-JCP-2019.pdf
Publisher postprint (2.2 MB)
Download

All documents in ORBilu are protected by a user license.

Send to



Details



Abstract :
[en] Non-covalent interactions pervade all matter and play a fundamental role in layered materials, biological systems, and large molecular complexes. Despite this, our accumulated understanding of non-covalent interactions to date has been mainly developed in the tens-of-atoms molecular regime. This falls considerably short of the scales at which we would like to understand energy trends, structural properties, and temperature dependencies in materials where non-covalent interactions have an appreciable role. However, as more reference information is obtained beyond moderately sized molecular systems, our understanding is improving and we stand to gain pertinent insights by tackling more complex systems, such as supramolecular complexes, molecular crystals, and other soft materials. In addition, accurate reference information is needed to provide the drive for extending the predictive power of more efficient workhorse methods, such as density functional approximations that also approximate van der Waals dispersion interactions. In this perspective, we discuss the first-principles approaches that have been used to obtain reference interaction energies for beyond modestly sized molecular complexes. The methods include quantum Monte Carlo, symmetry-adapted perturbation theory, non-canonical coupled cluster theory, and approaches based on the random-phase approximation. By considering the approximations that underpin each method, the most accurate theoretical references for supramolecular complexes and molecular crystals to date are ascertained. With these, we also assess a handful of widely used exchange-correlation functionals in density functional theory. The discussion culminates in a framework for putting into perspective the accuracy of high-level wavefunction-based methods and identifying future challenges.
Disciplines :
Physics
Author, co-author :
Al-Hamdani, Yasmine
Tkatchenko, Alexandre ;  University of Luxembourg > Faculty of Science, Technology and Communication (FSTC) > Physics and Materials Science Research Unit
External co-authors :
no
Language :
English
Title :
Understanding non-covalent interactions in larger molecular complexes from first principles
Publication date :
01 January 2019
Journal title :
Journal of Chemical Physics
ISSN :
1089-7690
Publisher :
American Institute of Physics, New York, United States - New York
Volume :
150
Pages :
010901
Peer reviewed :
Peer Reviewed verified by ORBi
Focus Area :
Physics and Materials Science
Computational Sciences
Available on ORBilu :
since 31 October 2019

Statistics


Number of views
216 (6 by Unilu)
Number of downloads
204 (4 by Unilu)

Scopus citations®
 
62
Scopus citations®
without self-citations
59
OpenCitations
 
41
WoS citations
 
62

Bibliography


Similar publications



Contact ORBilu