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Electronic structure of aqueous solutions: Bridging the gap between theory and experiments
Predicting the electronic properties of aqueous liquids has been a long-standing challenge for quantum mechanical methods. However, it is a crucial step in understanding and predicting the key role played by aqueous solutions and electrolytes in a wide variety of emerging energy and environmental te...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
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American Association for the Advancement of Science
2017
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5482551/ https://www.ncbi.nlm.nih.gov/pubmed/28691091 http://dx.doi.org/10.1126/sciadv.1603210 |
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author | Pham, Tuan Anh Govoni, Marco Seidel, Robert Bradforth, Stephen E. Schwegler, Eric Galli, Giulia |
author_facet | Pham, Tuan Anh Govoni, Marco Seidel, Robert Bradforth, Stephen E. Schwegler, Eric Galli, Giulia |
author_sort | Pham, Tuan Anh |
collection | PubMed |
description | Predicting the electronic properties of aqueous liquids has been a long-standing challenge for quantum mechanical methods. However, it is a crucial step in understanding and predicting the key role played by aqueous solutions and electrolytes in a wide variety of emerging energy and environmental technologies, including battery and photoelectrochemical cell design. We propose an efficient and accurate approach to predict the electronic properties of aqueous solutions, on the basis of the combination of first-principles methods and experimental validation using state-of-the-art spectroscopic measurements. We present results of the photoelectron spectra of a broad range of solvated ions, showing that first-principles molecular dynamics simulations and electronic structure calculations using dielectric hybrid functionals provide a quantitative description of the electronic properties of the solvent and solutes, including excitation energies. The proposed computational framework is general and applicable to other liquids, thereby offering great promise in understanding and engineering solutions and liquid electrolytes for a variety of important energy technologies. |
format | Online Article Text |
id | pubmed-5482551 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2017 |
publisher | American Association for the Advancement of Science |
record_format | MEDLINE/PubMed |
spelling | pubmed-54825512017-07-07 Electronic structure of aqueous solutions: Bridging the gap between theory and experiments Pham, Tuan Anh Govoni, Marco Seidel, Robert Bradforth, Stephen E. Schwegler, Eric Galli, Giulia Sci Adv Research Articles Predicting the electronic properties of aqueous liquids has been a long-standing challenge for quantum mechanical methods. However, it is a crucial step in understanding and predicting the key role played by aqueous solutions and electrolytes in a wide variety of emerging energy and environmental technologies, including battery and photoelectrochemical cell design. We propose an efficient and accurate approach to predict the electronic properties of aqueous solutions, on the basis of the combination of first-principles methods and experimental validation using state-of-the-art spectroscopic measurements. We present results of the photoelectron spectra of a broad range of solvated ions, showing that first-principles molecular dynamics simulations and electronic structure calculations using dielectric hybrid functionals provide a quantitative description of the electronic properties of the solvent and solutes, including excitation energies. The proposed computational framework is general and applicable to other liquids, thereby offering great promise in understanding and engineering solutions and liquid electrolytes for a variety of important energy technologies. American Association for the Advancement of Science 2017-06-23 /pmc/articles/PMC5482551/ /pubmed/28691091 http://dx.doi.org/10.1126/sciadv.1603210 Text en Copyright © 2017 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). http://creativecommons.org/licenses/by-nc/4.0/ This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license (http://creativecommons.org/licenses/by-nc/4.0/) , which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited. |
spellingShingle | Research Articles Pham, Tuan Anh Govoni, Marco Seidel, Robert Bradforth, Stephen E. Schwegler, Eric Galli, Giulia Electronic structure of aqueous solutions: Bridging the gap between theory and experiments |
title | Electronic structure of aqueous solutions: Bridging the gap between theory and experiments |
title_full | Electronic structure of aqueous solutions: Bridging the gap between theory and experiments |
title_fullStr | Electronic structure of aqueous solutions: Bridging the gap between theory and experiments |
title_full_unstemmed | Electronic structure of aqueous solutions: Bridging the gap between theory and experiments |
title_short | Electronic structure of aqueous solutions: Bridging the gap between theory and experiments |
title_sort | electronic structure of aqueous solutions: bridging the gap between theory and experiments |
topic | Research Articles |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5482551/ https://www.ncbi.nlm.nih.gov/pubmed/28691091 http://dx.doi.org/10.1126/sciadv.1603210 |
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