X-ray reflectivity and vibrational sum frequency spectroscopy are used to probe the structure of the ethylammonium nitrate (EAN)-air interface. X-ray reflectivity reveals that the EAN-air interface is structured and consists of alternating nonpolar and charged layers that extend 31 A into the bulk. Vibrational sum frequency spectroscopy reveals interfacial cations have their ethyl moieties oriented toward air, with the CH(3) C(3) axis positioned approximately 36.5 degrees from interface normal. This structure is invariant between 15 and 51 degrees C. On account of its molecular symmetry, the orientation of the nitrate anion cannot be determined with certainty.
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