PNNL

Abstract

Although it has been shown that size of atmospheric particles has a direct correlation with their ability to act as cloud droplet and ice nuclei, the influence of composition of freshly emitted and aged particles in nucleation processes is poorly understood. In this work we combine data from field measurements of ice nucleation with chemical imaging of the sampled particles to link aerosol composition with ice nucleation ability. Field measurements and sampling were conducted during the Indirect and Semidirect Aerosols Campaign (ISDAC) over Barrow, Alaska, in the springtime of 2008. In-situ ice nucleation measurements were conducted using a Continuous Flow Diffusion Chamber (CFDC). Measured number concentrations of ice nuclei (IN) varied from frequent values of 0.01 per liter to more than 10 per liter. Residuals of airborne droplets and ice crystals were collected through a counterflow virtual impactor (CVI). The compositions of individual atmospheric particles and the residuals were studied using Computer Controlled Scanning Electron Microscopy with Energy Dispersive X-ray analysis (CCSEM/EDX) and Scanning Transmission X-ray Microscopy coupled with Near Edge X-ray Absorption Fine Structure spectroscopy (STXM/NEXAFS). Chemical analysis of cloud particle residuals collected during an episode of high ice nucleation suggests that both size and composition may influence aerosol's ability to act as IN. The STXM/NEXAFS chemical composition maps of individual residuals have characteristic structures of either inorganic or black carbon cores coated by organic materials. In a separate flight, particle samples from a biomass burning plume were collected. Although it has previously been suggested that episodes of biomass burning contribute to increased numbers of highly effective ice nuclei, in this episode we observed that only a small fraction were effective ice nuclei. Most of the particles from the biomass plume episode were smaller in size and were composed of homogeneous organic material without identifiable cores.