Abstract.Here we present the online meteorology and chemistry adjoint and tangent linear model, WRFPLUSChem (Weather Research and Forecasting plus chemistry), which incorporates modules to treat boundary layer mixing, emission, aging, dry deposition, and advection of black carbon aerosol. We also develop land surface and surface layer adjoints to account for coupling between radiation and vertical mixing. Model performance is verified against finite difference derivative approximations. A second-order checkpointing scheme is created to reduce computational costs and enable simulations longer than 6 h. The adjoint is coupled to WRFDA-Chem, in order to conduct a sensitivity study of anthropogenic and biomass burning sources throughout California during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaign. A cost-function weighting scheme was devised to reduce the impact of statistically insignificant residual errors in future inverse modeling studies. Results of the sensitivity study show that, for this domain and time period, anthropogenic emissions are overpredicted, while wildfire emission error signs vary spatially. We consider the diurnal variation in emission sensitivities to determine at what time sources should be scaled up or down. Also, adjoint sensitivities for two choices of land surface model (LSM) indicate that emission inversion results would be sensitive to forward model configuration. The tools described here are the first step in conducting four-dimensional variational data assimilation in a coupled meteorology-chemistry model, which will potentially provide new constraints on aerosol precursor emissions and their distributions. Such analyses will be invaluable to assessments of particulate matter health and climate impacts.

Quantifying methane (CH4) emissions from the oil and natural gas (O/NG) production sector is an important regulatory challenge in the United States. In this study, we conduct a set of inversion calculations using different methods to quantify lognormal distributed CH4 surface fluxes in the Haynesville‐Bossier O/NG production basin in Texas and Louisiana, combining three statistical cost functions, four meteorological configurations, and two days of aircraft measurements from a 2013 field campaign. We aggregate our posterior flux estimates to derive our best estimate of the basin‐wide CH4 emissions, 76 metric tons/hr, with a 95% highest density interval of 51–104 metric tons/hr, in agreement with previous estimates using mass balance and eddy covariance approaches with the same aircraft measurements. Our inversion estimate of basin‐wide CH4 emissions is 133% (89%–182%, 95% highest density interval) of a gridded Environmental Protection Agency's inventory for 2012, and the largest discrepancies between our study and this inventory are located in the northeastern quadrant of the basin containing active unconventional O/NG wells. Our inversion approach provides a new spatiotemporal characterization of CH4 emissions in this O/NG production region and shows the usefulness of inverse modeling for improving O/NG CH4 emission estimates.

Abstract. Biomass burning emissions of atmospheric aerosols, including black carbon, are growing due to increased global drought, and comprise a large source of uncertainty in regional climate and air quality studies. We develop and apply new incremental four-dimensional variational (4D-Var) capabilities in WRFDA-Chem to find optimal spatially and temporally distributed biomass burning (BB) and anthropogenic black carbon (BC) aerosol emissions. The constraints are provided by aircraft BC concentrations from the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites in collaboration with the California Air Resources Board (ARCTAS-CARB) field campaign and surface BC concentrations from the Interagency Monitoring of PROtected Visual Environment (IMPROVE) network on 22, 23, and 24 June 2008. We consider three BB inventories, including Fire INventory from NCAR (FINN) v1.0 and v1.5 and Quick Fire Emissions Database (QFED) v2.4r8. On 22 June, aircraft observations are able to reduce the spread between a customized QFED inventory and FINNv1.0 from a factor of 3.5 (×3.5) to only ×2.1. On 23 and 24 June, the spread is reduced from ×3.4 to ×1.4. The posterior corrections to emissions are heterogeneous in time and space, and exhibit similar spatial patterns of sign for both inventories. The posterior diurnal BB patterns indicate that multiple daily emission peaks might be warranted in specific regions of California. The US EPA's 2005 National Emissions Inventory (NEI05) is used as the anthropogenic prior. On 23 and 24 June, the coastal California posterior is reduced by ×2, where highway sources dominate, while inland sources are increased near Barstow by ×5. Relative BB emission variances are reduced from the prior by up to 35 % in grid cells close to aircraft flight paths and by up to 60 % for fires near surface measurements. Anthropogenic variance reduction is as high as 40 % and is similarly limited to sources close to observations. We find that the 22 June aircraft observations are able to constrain approximately 14 degrees of freedom of signal (DOF), while surface and aircraft observations together on 23/24 June constrain 23 DOF. Improving hourly-to daily-scale concentration predictions of BC and other aerosols during BB events will require more comprehensive and/or targeted measurements and a more complete accounting of sources of error besides the emissions.