Predicting the electronic properties of liquids has been a long-standing challenge for quantum-mechanical methods. Yet it is a crucial step in understanding and optimizing the properties of aqueous solutions and electrolytes, which play a key role in a wide variety of emerging energy and environmental technologies, including battery and photoelectrochemical cell design. To address this challenge, we propose an efficient and accurate approach to predict the electronic properties of aqueous solutions, based on the combination of first-principles methods and experimental validation using state-of-the-art spectroscopic measurements. We present results for the photoelectron spectra of a broad range of aqueous solutions, showing that first-principles molecular dynamics simulations and electronic structure calculations using dielectric hybrid functionals provide a quantitative description of their electronic properties, including excitation energies, of the solvent and solutes. 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.

Predictive description of electronic properties in aqueous solutions

253rd National Meeting (2017)

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