Comparison of ozone formation attribution techniques in the northeastern United States

Abstract

The Integrated Source Apportionment Method (ISAM) has been revised in the Community Multiscale Air Quality (CMAQ) model. This work updates ISAM to maximize its flexibility, particularly for ozone (O3) modeling, by providing multiple attribution options, including products inheriting attribution fully from nitrogen oxide reactants, fully from volatile organic compound (VOC) reactants, equally from all reactants, or dynamically from NOx or VOC reactants based on the indicator gross production ratio of hydrogen peroxide (H2O2) to nitric acid (HNO3). The updated ISAM has been incorporated into the most recent publicly accessible versions of CMAQ (v5.3.2 and beyond). This study's primary objective is to document these ISAM updates and demonstrate their impacts on source apportionment results for O3 and its precursors. Additionally, the ISAM results are compared with the Ozone Source Apportionment Technology (OSAT) in the Comprehensive Air-quality Model with Extensions (CAMx) and the brute-force method (BF). All comparisons are performed for a 4 km horizontal grid resolution application over the northeastern US for a selected 2 d summer case study (9 and 10 August 2018). General similarities among ISAM, OSAT, and BF results add credibility to the new ISAM algorithms. However, some discrepancies in magnitude or relative proportions among tracked sources illustrate the distinct features of each approach, while others may be related to differences in model formulation of chemical and physical processes. Despite these differences, OSAT and ISAM still provide useful apportionment data by identifying the geographical and temporal contributions of O3 and its precursors. Both OSAT and ISAM attribute the majority of O3 and NOx contributions to boundary, mobile, and biogenic sources, whereas the top three contributors to VOCs are found to be biogenic, boundary, and area sources.