The infrared signatures of nitric acid HNO3 and its conjugate anion NO3- at the surface of an aqueous layer are derived from electronic structure calculations at the HF/SBK+* level of theory on the HNO3 center dot(H2O)(3) -> NO3-center dot H3O+center dot(H2O)(2) model reaction system embedded in clusters comprising 33, 40, 45, and 50 classical, polarizable waters, mimicking various degrees of solvation [Bianco, R.; Wang, S.; Hynes, J. T. J. Phys. Chem. A 2007, 111, 11033]. The molecular level character of the various bands is discussed, and the solvation patterns are described in terms of hydrogen bonding and resulting polarization of the species' intramolecular bonds. Connection is made with assorted experimental results, including surface-sensitive Sum Frequency Generation spectroscopy of aqueous nitric acid solutions, infrared spectroscopy of amorphous thin films of nitric acid monohydrate (NAM) and dihydrate (NAD), and infrared and Raman spectroscopic results for bulk aqueous solutions of nitric acid and nitrate salts.