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Charge-Transfer-to-Solvent Spectrum of Thiocyanate at the Air/Water Interface Measured by Broadband Deep Ultraviolet Electronic Sum Frequency Generation Spectroscopy
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 |<i>χ</i><sup>(2)</sup>|<sup>2</sup>-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
Media 1: High-speed multispectral videography with a periscope array in a spectral shaper
Originally published in Optics Letters on 15 December 2014 (ol-39-24-6942