Determining contributions of biomass burning and other sources to fine particle contemporary carbon in the western United States

Abstract

Six-day integrated fine particle samples were collected at urban and rural sampling sites using Hi-Volume samplers during winter and summer 2004–2005 as part of the IMPROVE (Interagency Monitoring of PROtected Visual Environments) Radiocarbon Study. Filter samples from six sites (Grand Canyon, Mount Rainier, Phoenix, Puget Sound, Rocky Mountain National Park, and Tonto National Monument) were analyzed for levoglucosan, a tracer for biomass combustion, and other species by High-Performance Anion-Exchange Chromatography with Pulsed Amperometric Detection (HPAEC-PAD). Contemporary carbon concentrations were available from previous carbon isotope measurements at Lawrence Livermore National Laboratory. Primary contributions of biomass burning to measured fine particle contemporary carbon were estimated for residential wood burning (winter) and wild/prescribed fires (summer). Calculated contributions ranged from below detection limit to more than 100% and were typically higher at rural sites and during winter. Mannitol, a sugar alcohol emitted by fungal spores, was analyzed and used to determine contributions of fungal spores to fine particle contemporary carbon. Contributions reached up to 13% in summer samples, with higher contributions at rural sites. Concentrations of methyltetrols, oxidation products of isoprene, were also measured by HPAEC-PAD. Secondary organic aerosol (SOA) from isoprene oxidation was estimated to contribute up to 22% of measured contemporary carbon. For each sampling site, a substantial portion of the contemporary carbon was unexplained by primary biomass combustion, fungal spores, or SOA from isoprene oxidation. This unexplained fraction likely contains contributions from other SOA sources, including oxidation products of primary smoke emissions and plant emissions other than isoprene, as well as other primary particle emissions from meat cooking, plant debris, other biological aerosol particles, bio-diesel combustion, and other sources. Loss of levoglucosan during atmospheric aging of biomass burning emissions likely also results in an underestimate of apportioned primary smoke contributions.