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- W3147223869 abstract "The absolute-scale electronic energetics of liquid water and aqueous solutions, both in the bulk and at associated interfaces, are the central determiners of water-based chemistry. However, such information is generally experimentally inaccessible. We demonstrate that a refined implementation of the liquid microjet photoelectron spectroscopy (PES) technique can be adopted to address this. Implementing concepts from condensed matter physics, we establish novel all-liquid-phase vacuum and equilibrated solution-metal-electrode Fermi level referencing procedures. This enables the precise and accurate quantification of previously elusive solute-induced perturbations of water's electronic energetics and vertical ionization energy (VIE) definition on an absolute and universal chemical potential scale. Applying these procedures over a broad range of ionization energies, we accurately and respectively determine the VIE and oxidative stability of liquid water as 11.33 $pm$ 0.02 eV and 6.60 $pm$ 0.08 eV with respect to its liquid-vacuum-interface potential and Fermi level. Combining our referencing schemes, we determine the work function of liquid water as 4.73 $pm$ 0.09 eV. Further, applying our novel approach to a pair of exemplary aqueous solutions, we extract absolute VIEs of aqueous iodide anions, reaffirm the robustness of water's electronic structure to high bulk salt concentrations, and quantify reference-level dependent reductions of water's VIE and a 0.48 $pm$ 0.13 eV contraction of the solution's work function upon partial hydration of a known surfactant. Our combined experimental accomplishments mark a major advance in our ability to quantify electronic-structure interactions and chemical reactivity in water, which now explicitly extends to the measurement of absolute-scale bulk and interfacial solution energetics, including those of relevance to aqueous electrochemical processes." @default.
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- W3147223869 date "2021-04-04" @default.
- W3147223869 modified "2023-09-27" @default.
- W3147223869 title "Accurate Vertical Ionization Energy and Work Function Determinations of Liquid Water and Aqueous Solutions" @default.
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