Changing Nature of Organic Carbon over the United States.

Abstract

Total organic carbon (TOC) mass concentrations are decreasing across the contiguous United States (CONUS). We investigate decadal trends in organic carbon (OC) thermal fractions [OC1 (volatilizes at 140 °C), OC2 (280 °C), OC3 (480 °C), OC4 (580 °C)] and pyrolyzed carbon (PC), reported at 121 locations in the Interagency Monitoring of Protected Visual Environments (IMPROVE) network from 2005 to 2015 for 23 regions across the CONUS. Reductions in PC and OC2 drive decreases in TOC (TOC = OC1 + OC2 + OC3 + OC4 + PC) mass concentrations. OC2 decreases by 40% from 2005 to 2015, and PC decreases by 34%. The largest absolute mass decreases occur in the eastern United States, and relative changes normalized to local concentrations are more uniform across the CONUS. OC is converted to organic mass (OM) using region- and season-specific OM:OC ratios. Simulations with GEOS-Chem reproduce OM trends and suggest that decreases across the CONUS are due to aerosol liquid water (ALW) chemistry. Individual model species, notably aerosol derived from isoprene oxidation products and formed in ALW, correlate significantly (p < 0.05) with OM2, even in arid regions. These findings contribute to literature that suggests air quality rules aimed at SO2 and NOx emissions induce the cobenefit of reducing organic particle mass through ALW chemistry, and these benefits extend beyond the eastern United States.