: 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.

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. - In: SCIENCE ADVANCES. - ISSN 2375-2548. - 3:6(2017), pp. e1603210-e1603210. [10.1126/sciadv.1603210]

Electronic structure of aqueous solutions: Bridging the gap between theory and experiments

Govoni, Marco;
2017

Abstract

: 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.
2017
3
6
e1603210
e1603210
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. - In: SCIENCE ADVANCES. - ISSN 2375-2548. - 3:6(2017), pp. e1603210-e1603210. [10.1126/sciadv.1603210]
Pham, Tuan Anh; Govoni, Marco; Seidel, Robert; Bradforth, Stephen E; Schwegler, Eric; Galli, Giulia
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11380/1295256
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