Evaluation of assumptions for estimating chemical light extinction at U.S. national parks

Abstract

Studies were conducted at Great Smoky Mountains National Park (NP) (GRSM), Tennessee, Mount Rainier NP (MORA), Washington, and Acadia NP (ACAD), Maine, to evaluate assumptions used to estimate aerosol light extinction from chemical composition. The revised IMPROVE equation calculates light scattering from concentrations of PM2.5 sulfates, nitrates, organic carbon mass (OM), and soil. Organics are assumed to be nonhygroscopic. Organic carbon (OC) is converted to OM with a multiplier of 1.8. Experiments were conducted to evaluate assumptions on aerosol hydration state, the OM/OC ratio, OM hygroscopicity, and mass scattering efficiencies. Sulfates were neutralized by ammonium during winter at GRSM (W, winter) and at MORA during summer but were acidic at ACAD and GRSM (S, summer) during summer. Hygroscopic growth was mostly smooth and continuous, rarely exhibiting hysteresis. Deliquescence was not observed except infrequently during winter at GRSM (W). Water-soluble organic carbon (WSOC) was separated from bulk OC with solid-phase absorbents. The average OM/OC ratios were 2.0, 2.7, 2.1, and 2.2 at GRSM (S), GRSM (W), MORA, and ACAD, respectively. Hygroscopic growth factors (GF) at relative humidity (RH) 90% for aerosols generated from WSOC extracts averaged 1.19, 1.06, 1.13, and 1.16 at GRSM (S), GRSM (W), MORA, and ACAD, respectively. Thus, the assumption that OM is not hygroscopic may lead to underestimation of its contribution to light scattering.Implications: Studies at IMPROVE sites conducted in U.S. national parks showed that aerosol organics comprise more PM2.5 mass and absorb more water as a function of relative humidity than is currently assumed by the IMPROVE equation for calculating chemical light extinction. Future strategies for reducing regional haze may therefore need to focus more heavily on understanding the origins and control of anthropogenic sources of organic aerosols.