The reaction of sea salt aerosol with NO2 under ambient conditions was explored using particles that were generated by atomizing an aqueous solution of synthetic sea salt. The aerosol at 9-30% relative humidity, was mixed with 1-3 mbar of NO2 and then passed through an optical cell where reactants and products were monitored by infrared spectroscopy. The duration times of the reaction, partial pressure of NO2, and relative humidity were systematically varied in order to explore the aerosol heterogeneous chemistry. Infrared spectra of the aerosol revealed that a substantial fraction of the particulate Cl- was replaced by NO3- and that there was a significant production of ClNO, consistent with the stoichiometery 2 NO2 + Cl- --> NO3- + ClNO. The rate of the reaction was found to increase both with NO2 pressure and relative humidity. The infrared spectra also revealed that, even under arid conditions, the sea salt aerosol particles contain more water than can be explained by the various hydrates in sea salt, suggesting that the particles possess a complex structure. This complex structure involves microcrystalline and amorphous regions with pockets for water inclusions.