Applications of Adjoint Modelling in Chemical Composition: Studies of Tropospheric Ozone at Middle and High Northern Latitudes

• Main Author: Walker, Thomas
• Other Authors: Jones, Dylan, Physics
• Format: Thesis
• Language: English
• Subjects: atmospheric science; chemical composition; adjoint model; data assimilation; 0608; Arctic; Nunavut
• Online Access: http://hdl.handle.net/1807/65764

Ozone is integral to tropospheric chemistry, and understanding the processes controlling its distribution is important in climate and air pollution contexts. The GEOS-Chem global chemical transport model and its adjoint are used to interpret the impacts of midlatitude precursor emissions and atmospheric transport on the tropospheric ozone distribution at middle and high northern latitudes. In the Arctic, the model reproduces seasonal cycles of peroxyacetyl nitrate (PAN) and ozone measured at the surface, and observed ozone abundances in the summer free troposphere. Source attribution analysis suggests that local photochemical production, ≤ 0.25 ppbv/day, driven by PAN decomposition accounts for more than 50% of ozone in the summertime Arctic boundary layer. In the mid-troposphere, photochemical production accounts for 30-40% of ozone, while ozone transported from midlatitudes contributes 25-35%. Adjoint sensitivity studies link summertime ozone production to anthropogenic, biomass burning, soil, and lightning emissions between 50N-70N. Over Alert, Nunavut, the sensitivity of mid-tropospheric ozone to lightning emissions sometimes exceeds that to anthropogenic emissions. Over the eastern U.S., numerous models overestimate ozone in the summertime boundary layer. An inversion analysis, using the GEOS-Chem four-dimensional variational data assimilation system, optimizes emissions of NOx and isoprene. Inversion results suggest the model bias cannot be explained by discrepancies in these precursor emissions. A separate inversion optimizes rates of key chemical reactions including ozone deposition rates, which are parameterized and particularly uncertain. The inversion suggests a factor of 2-3 increase in deposition rates in the northeastern U.S., decreasing the ozone bias from 17.5 ppbv to 6.0 ppbv. This analysis, however, is sensitive to the model boundary layer mixing scheme. Several inversion analyses are conducted to estimate lightning NOx emissions over North America in August 2006, using ozonesonde data. The high-resolution nested version of GEOS-Chem is used to better capture variability in the ozonesonde data. The analyses suggest North American lightning NOx totals between 0.076-0.204 Tg N. A major challenge is that the vertical distribution of the lightning source is not optimized, but the results suggest a bias in the vertical distribution. Reliably optimizing the three-dimensional distribution of lightning NOx emissions requires more information than the ozonesonde dataset contains. PhD