During August and September of 2002, a relative humidity (RH) scanning tandem differential mobility analyzer system was used to measure the deliquescence/crystallization properties of ambient aerosol populations in southeast Texas. During August, sampling was conducted at a rural site on the Texas A&M campus in College Station, and in September, sampling was conducted at an urban site near the Houston ship channel. Measurements from both sites indicate that there are cyclical changes in the composition of the soluble fraction of the aerosol, which are not strongly linked to the local aerosol source. The observations show that as temperature increases and RH decreases, the hysteresis loop describing the RH dependence of aerosol hygroscopic growth collapses. On the basis of results from other studies that have shown the dominant ions present in aerosols in this region to be ammonium and sulfate, it is proposed that this collapse is due to a decrease in the ammonium to sulfate ratio in the aerosol particles, which coincides with increasing temperature and decreasing RH. This cyclical change in aerosol acidity may influence secondary organic aerosol production and may exaggerate the impact of the aerosol on human health. The compositional changes also result in a daily cycle in crystallization RH that is in phase with that of the ambient RH, which reduces the probability that hygroscopic particles will crystallize in the afternoon when the ambient RH is a minimum.