During the Nitrogen, Aerosol Composition, and Halogens on a Tall Tower campaign at the National Oceanic and Atmospheric Administration Boulder Atmospheric Observatory tower, Erie, CO, USA, in winter 2011, soluble trace gases, the ionic composition of size-resolved aerosols, and the associated meteorological conditions were measured. Median gas-phase mixing ratios of HCl, HNO3, and NH3 were 0.072, 0.202, and 5.79 nmol mol−1, respectively. Most aerosol Cl− was associated with supermicrometer size fractions whereas NO3− and NH4+ were associated primarily with submicrometer size fractions. Aerosol pHs inferred from the measured phase partitioning and thermodynamic properties of HNO3 and NH3 were similar both in terms of absolute values and variability as a function of size. Aerosols were acidic across all size fractions and throughout the duration of the campaign (mostly in the pH range of 2 to 3). The pHs inferred from the HCl/Cl− couple were consistently higher by about 1 to 2 pH units, suggesting possible bias in the associated thermodynamic evaluation of HCl. Specifically, relative to those for HNO3 and NH3, the Henry's law constant for HCl is associated with much greater uncertainty. Condensation of HCl replaced Cl− consumed in the production of ClNO2. Additionally, total Cl (HCl + Cl−) was greater than ClNO2 in sampled air parcels, suggesting that Cl availability was not the limiting factor in ClNO2 production. Median ClNO2 yields from N2O5 reaction with particulate Cl− associated with all size fractions were greater than 0.9.