Measurement report: Seasonal Secondary and Biomass-Burning Aerosol Sources and Enhancements of Cloud Condensation Nuclei at a Central US Background Site
Abstract. Long-term measurements of aerosol chemistry are essential for understanding seasonal source variability and aerosol–climate interactions in continental environments. We present a multi-year (2021–2023) analysis of submicron aerosol composition at the U.S. Department of Energy Southern Great Plains (SGP) site using co-located Aerosol Chemical Speciation Monitor (ACSM), Interagency Monitoring of Protected Visual Environments (IMPROVE) network filter measurements, and supporting optical, size-distribution, and cloud condensation nuclei (CCN) observations. Organic aerosol (OA), nitrate (NO3), ammonium (NH4), sulfate (SO4), and mineral dust exhibited pronounced seasonal cycles. NO3 and NH4 dominated winter aerosol mass, consistent with thermodynamic partitioning of ammonium nitrate (NH4NO3), while OA and SO4 peaked in spring and summer, reflecting enhanced photochemistry and biogenic precursor emissions.
Positive Matrix Factorization with a rolling-window ME-2 framework resolved biomass-burning OA (BBOA), semi-volatile oxygenated OA (SVOOA), and low-volatility oxygenated OA (LVOOA). SVOOA and LVOOA together dominated annual OA mass, with strong summer maxima, while BBOA contributed episodically during fire events. We identified 168 biomass- burning episodes using BBOA spikes detected using rolling-median residual spike detection. Fire plumes increased aerosol absorption coefficient modestly but enhanced CCN number concentrations by up to a factor of four. HYSPLIT and satellite fire products indicate dominant contributions from Great Plains grassland and cropland burns, with additional forest and distant sources. These results provide a comprehensive characterization of aerosol seasonal behavior and biomass-burning impacts in the central United States, demonstrating the value of long-term, high-time-resolution mass-spectrometric observations.