Frontier orbitals and quasiparticle energy levels in ionic liquids
File(s)
Published version
Author(s)
Kahk, Juhan
Lovelock, Kevin
Kuusik, Ivar
Kisand, Vambola
Lischner, Johannes
Type
Journal Article
Abstract
Room temperature ionic liquids play an important role in many technological applications and a detailed understanding of their frontier molecular orbitals is required to optimize interfacial barriers,reactivity and stability with respect to electron injection and removal. In this work, we calculate quasiparticle energy levels of ionic liquids using first-principles many-body perturbation theory within the GW approximation and compare our results to various mean-field approaches, including semilocal and hybrid density-functional theory and Hartree-Fock. We find that the mean-field results depend qualitatively and quantitatively on the treatment of exchange-correlation effects, while GW calculations produce results that are in excellent agreement with experimental photoelectron spectra of gas phase ion pairs and ionic liquids. These results establish the GW approach as a valuable tool for understanding the electronic structures of ionic liquids.
Date Issued
2020-10-07
Date Acceptance
2020-08-25
Citation
npj Computational Materials, 2020, 6 (148), pp.1-7
ISSN
2057-3960
Publisher
Nature Research
Start Page
1
End Page
7
Journal / Book Title
npj Computational Materials
Volume
6
Issue
148
Copyright Statement
© The Author(s) 2020. This article is licensed under a Creative Commons
Attribution 4.0 International License, which permits use, sharing,
adaptation, distribution and reproduction in any medium or format, as long as you give
appropriate credit to the original author(s) and the source, provide a link to the Creative
Commons license, and indicate if changes were made. The images or other third party
material in this article are included in the article’s Creative Commons license, unless
indicated otherwise in a credit line to the material. If material is not included in the
article’s Creative Commons license and your intended use is not permitted by statutory
regulation or exceeds the permitted use, you will need to obtain permission directly
from the copyright holder. To view a copy of this license, visit http://creativecommons.
org/licenses/by/4.0/.
Attribution 4.0 International License, which permits use, sharing,
adaptation, distribution and reproduction in any medium or format, as long as you give
appropriate credit to the original author(s) and the source, provide a link to the Creative
Commons license, and indicate if changes were made. The images or other third party
material in this article are included in the article’s Creative Commons license, unless
indicated otherwise in a credit line to the material. If material is not included in the
article’s Creative Commons license and your intended use is not permitted by statutory
regulation or exceeds the permitted use, you will need to obtain permission directly
from the copyright holder. To view a copy of this license, visit http://creativecommons.
org/licenses/by/4.0/.
Sponsor
Engineering & Physical Science Research Council (EPSRC)
The Royal Society
Identifier
https://www.nature.com/articles/s41524-020-00413-4
Grant Number
EP/R002010/1
URF\R\191004
Publication Status
Published
Date Publish Online
2020-10-07