Journal
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 67
Volume 67, Issue -, Pages 283-305Publisher
ANNUAL REVIEWS
DOI: 10.1146/annurev-physchem-040513-103715
Keywords
hydration; ionization; photodetachment; electron binding energies; liquid jet
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Funding
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1301465] Funding Source: National Science Foundation
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The valence orbital electron binding energies of water and of embedded solutes are crucial quantities for understanding chemical reactions taking place in aqueous solution, including oxidation/reduction, transition-metal coordination, and radiation chemistry. Their experimental determination based on liquid-photoelectron spectroscopy using soft X-rays is described, and we provide an overview of valence photoelectron spectroscopy studies reported to date. We discuss principal experimental aspects and several theoretical approaches to compute the measured binding energies of the least tightly bound molecular orbitals. Solutes studied are presented chronologically, from simple electrolytes, via transition-metal ion solutions and several organic and inorganic molecules, to biologically relevant molecules, including aqueous nucleotides and their components. In addition to the lowest vertical ionization energies, the measured valence photoelectron spectra also provide information on adiabatic ionization energies and reorganization energies for the oxidation (ionization) half-reaction. For solutes with low solubility, resonantly enhanced ionization provides a promising alternative pathway.
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