Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 9, Issue 16, Pages 4753-4757Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.8b01966
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- Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy (DOE) through the Chemical Sciences Division of the Lawrence Berkeley National Laboratory (LBNL) [DE-AC02-05CH11231]
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Measurement of interfacial electronic spectra is a powerful tool for characterizing the properties of ions in physical, biological, environmental, and industrial systems. Here, we describe measurement of the complete charge-transfer-to-solvent (CTTS) spectrum of thiocyanate at the air/water interface using our recently developed femtosecond broadband deep ultraviolet electronic sum frequency generation technique. We find that the lower energy CTTS band characterized in bulk thiocyanate spectra is not observed in the vertical bar chi((2))vertical bar(2) power spectrum of the air/water interface, likely reflecting the different solvation environments, altering of the charge distribution of the ion, and possible ion-ion effects, and that sodium and potassium salts yield identical spectra. Additional experiments and comparison with theoretical calculations are necessary to extract the interesting chemical details responsible for these salient spectral differences.
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