Contribution of pollen to atmospheric ice nuclei concentrations

Primary biological aerosol particles (PBAP) contribute to the concentrations of ice nuclei (IN) in the atmosphere. Laboratory studies have shown that pollen grains, a subset of PBAP, can serve as immersion mode ice nuclei at temperatures ranging from -9 to -25 deg C. At the peak of the pollen season pollen concentrations can reach surface-level concentrations exceeding 1 per liter of air. Furthermore, previous studies have suggested that the ice nucleating ability of some types of pollen is derived from non-proteinaceous macromolecules, which may become dispersed by the rupturing of the pollen sac during wetting and drying cycles. If true, this mechanism is expected to produce highly elevated IN concentrations at temperatures warmer than -25 deg C. Here we test this hypothesis by measuring ambient IN concentrations from the beginning to the end of the 2013 pollen season in Raleigh, North Carolina. Raleigh is surrounded by a dense mixed hardwood forest composed primarily of oak, hickory, and pine species. Air samples were collected using a swirling aerosol collector twice per week and the solution was analyzed for ice nuclei activity using a droplet freezing assay setup. Rainwater samples were collected during rain events at the peak of the pollen season and analyzed with the drop freezing assay to compare the potentially enhanced IN concentrations measured near the ground with IN concentrations found aloft. Raw freezing spectra were used to probe the freezing activity of both abundant and rare IN contained in sample liquids by analysis of drops that had varying degrees of preconcentration and size (~50 to ~650 μm). Extreme value statistics is used to collapse the raw freezing data into a single ice nuclei spectrum, defined as number of ice nuclei per volume of air as a function of temperature, that spans ~6 orders of magnitude in IN concentration. For a selected number of samples, concentrations of biological and non-biological ambient aerosol and particles are measured by the use of a UV fluorescence Wideband Integrated Bioaerosol Sensor (WIBS-4A) and used to infer the fraction of fluorescent particles that are able to serve as IN. Results show that IN concentrations for nuclei that require minimal supercooling were enhanced for one sample during the pollen season. However, no general trend was observed between ambient pollen counts and observed IN concentrations, suggesting that ice nuclei multiplication via pollen sac rupturing and subsequent release of macromolecules was not prevalent for the pollen types and meteorological conditions typically encountered in the Southeastern U.S.