Despite years of effort, the composition of polar stratospheric clouds (PSCs) is still uncertain. Future studies may be able to use FTIR extinction measurements to determine PSC composition. These studies require accurate optical constants for PSC materials. It has been suggested that accurate infrared (IR) optical constants for aerosols can only be derived from aerosol spectra. We have examined the IR spectra of nitric acid trihydrate (NAT) and nitric acid dihydrate (NAD) films and aerosols formed using a variety of experimental conditions. We conclude that several spectroscopically different types of NAD and NAT may exist. Alternatively, NAT could be birefringent and its spectra depend strongly on crystallographic orientation. The important causes for the different types or orientations seem to be the formation conditions and temperature, rather than whether the material is a film or aerosol. ¿ 1999 American Geophysical Union