Frontier orbitals and quasiparticle energy levels in ionic liquids

Kahk, J. M., Kuusik, I., Kisand, V., Lovelock, K. R.J. ORCID: https://orcid.org/0000-0003-1431-269X and Lischner, J. (2020) Frontier orbitals and quasiparticle energy levels in ionic liquids. npj Computational Materials, 6 (1). 148. ISSN 2057-3960 doi: 10.1038/s41524-020-00413-4

Abstract/Summary

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.

Item Type	Article
URI	https://reading-clone.eprints-hosting.org/id/eprint/93445
Item Type	Article
Refereed	Yes
Divisions	Life Sciences > School of Chemistry, Food and Pharmacy > Department of Chemistry
Publisher	Nature Research
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