Frontier orbitals and quasiparticle energy levels in ionic liquids
| Autor: | Kevin R. J. Lovelock, I. Kuusik, Johannes Lischner, Juhan Matthias Kahk, Vambola Kisand |
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| Přispěvatelé: | Engineering & Physical Science Research Council (EPSRC), The Royal Society |
| Rok vydání: | 2020 |
| Předmět: |
GW approximation
Work (thermodynamics) Materials science FOS: Physical sciences 02 engineering and technology 010402 general chemistry 01 natural sciences Spectral line chemistry.chemical_compound Atomic orbital lcsh:TA401-492 General Materials Science Molecular orbital Perturbation theory lcsh:Computer software Condensed Matter - Materials Science Materials Science (cond-mat.mtrl-sci) Computational Physics (physics.comp-ph) 021001 nanoscience & nanotechnology 0104 chemical sciences Computer Science Applications lcsh:QA76.75-76.765 chemistry Mechanics of Materials Chemical physics Modeling and Simulation Ionic liquid Quasiparticle lcsh:Materials of engineering and construction. Mechanics of materials 0210 nano-technology Physics - Computational Physics |
| Zdroj: | npj Computational Materials, Vol 6, Iss 1, Pp 1-7 (2020) |
| ISSN: | 2057-3960 |
| DOI: | 10.1038/s41524-020-00413-4 |
| Popis: | 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. |
| Databáze: | OpenAIRE |
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