Atmospheric aerosol particles influence climate through their direct and indirect effects. These impacts depend in part on the morphology of the particles, which is determined by their composition. The effect of pH on morphology was investigated using particles composed of 3-methylglutaric acid and ammonium sulfate by manipulating the starting pH of the bulk solution through the addition of aqueous sodium hydroxide. Efflorescence, deliquescence, phase separation, and mixing transitions were observed with optical microscopy. Due to changes in its protonation states, the solubility of the organic component increases with increasing pH, which shifts the location of the separation relative humidity (SRH) from 78.7% for the fully protonated acid to 63.9% for the fully deprotonated acid. Surprisingly, this shift in the SRH leads to hysteresis between the SRH and the mixing relative humidity (MRH). Particle pH has the greatest effect on phase transitions that require nucleus formation, that is, efflorescence and SRH.

Aerosol particle morphology influences the effect of particles on climate. Recent studies have documented the high acidity found in many ambient aerosol particles. The effect of this acidity on the phase transitions of mixed organic/inorganic aerosol particles has not been addressed. To investigate this effect, six organic compounds and ammonium sulfate were investigated individually with varying amounts of sulfuric acid to determine the role of low pH in the separation, efflorescence, and deliquescence transitions. All phase transitions were affected by the addition of sulfuric acid. This effect was attributed primarily to the change in the identity of the inorganic component as the ammonium/sulfate ratio (ASR) was changed from 2 to 1.5 to 1. The separation relative humidity (SRH) decreased with increasing amounts of sulfuric acid for each system studied, with the largest effect seen in compounds that have a lower SRH when mixed with ammonium sulfate. Control studies without an inorganic salt revealed that for some systems, phase separation occurs for mixtures of sulfuric acid and an organic acid. Overall, it was found that for aerosol particles at low pH (≤0.35) composed of organic acids and inorganic salts, phase separation can be impeded in some cases.

Heterogeneous ice nucleation is an important mechanism for cloud formation in the upper troposphere. Recently, pores on atmospheric particles have been proposed to play a significant role in ice nucleation. To understand how ice nucleation occurs in idealized pores, we characterized the immersion freezing activity of various sizes of carbon nanotubes. Carbon nanotubes are used both as a model for pores and proxy for soot particles. We determined that carbon nanotubes with inner diameters between 2 and 3 nm exhibit the highest ice nucleation activity. Implications for the freezing behavior of porous materials and nucleation on soot particles will be discussed.

The ice nucleation activity of fly ash, a byproduct of coal combustion, depends on its composition.