Case study evaluation of size-resolved molecular composition and phase state of carbonaceous particles in wildfire influenced smoke from the Pacific Northwest

Abstract

Wildfires are significant sources of carbonaceous particles in the atmosphere. Given the dependence of atmospheric processes on particle physical and molecular properties, the interplay between particle size, phase state and chemical composition is investigated here for aerosol influenced by a 2021 Pacific Northwest wildfire event. Both micro-spectroscopy and high resolution mass spectrometry analyses highlight a similarity in particle compositions independent of both particle size (0.1–0.32 μm particle diameters) and day/night cycle influences. Microscopy techniques revealed similar phase states for periods of both day and night, with increases in liquid-like character for smaller particles. Finally, we apply an evaporation kinetics model on estimated volatility distributions from assigned molecular formulae, similarly revealing a slight increase in liquid-like character for smaller particles with no significant day/night dependency. While the observations here are limited to a case study, the lack of influence from the day/night cycle on chemical composition and phase state of particles in a wildfire influenced plume is of particular note given that dependences are otherwise commonly observed for different environments/sources. This observation, combined with the lack of compositional dependencies for size-resolved wildfire-influenced particles, may have substantial implications for wildfire particle optical properties, transport, and atmospheric models.