United States (US) background ozone (O3) is the counterfactual O3 that would exist with zero US anthropogenic emissions. Estimates of US background O3 typically come from chemical transport models (CTMs), but different models vary in their estimates of both background and total O3. Here, a measurement-model data fusion approach is used to estimate CTM biases in US anthropogenic O3 and multiple US background O3 sources, including natural emissions, long-range international emissions, short-range international emissions from Canada and Mexico, and stratospheric O3. Spatially and temporally varying bias correction factors adjust each simulated O3 component so that the sum of the adjusted components evaluates better against observations compared to unadjusted estimates. The estimated correction factors suggest a seasonally consistent positive bias in US anthropogenic O3 in the eastern US, with the bias becoming higher with coarser model resolution and with higher simulated total O3, though the bias does not increase much with higher observed O3. Summer average US anthropogenic O3 in the eastern US was estimated to be biased high by 2, 7, and 11 ppb (11%, 32%, and 49%) for one set of simulations at 12, 36, and 108 km resolutions and 1 and 6 ppb (10% and 37%) for another set of simulations at 12 and 108 km resolutions. Correlation among different US background O3 components can increase the uncertainty in the estimation of the source-specific adjustment factors. Despite this, results indicate a negative bias in modeled estimates of the impact of stratospheric O3 at the surface, with a western US spring average bias of -3.5 ppb (-25%) estimated based on a stratospheric O3 tracer. This type of data fusion approach can be extended to include data from multiple models to leverage the strengths of different data sources while reducing uncertainty in the US background ozone estimates.
The Community Multiscale Air Quality (CMAQ) model has been used for regulatory purposes at the U.S. EPA and in the research community for decades. In 2012, we released the Weather Research and Forecasting (WRF)-CMAQ coupled model that enables aerosol information from CMAQ to affect meteorological processes through direct effects on shortwave radiation. Both CMAQ and WRF-CMAQ are considered limited-area models. Recently, we have extended domain coverage to the global scale by linking the meteorological Model for Prediction Across Scales - Atmosphere (MPAS-A, hereafter referred simply to as MPAS) with CMAQ to form the MPAS-CMAQ global coupled model. To configure these three different models, i.e., CMAQ (offline), WRF-CMAQ, and MPAS-CMAQ, we have developed the Advanced Air Quality Modeling System (AAQMS) for constructing each of them effortlessly. We evaluate this newly built MPAS-CMAQ coupled model using two global configurations: a 120 km uniform mesh and a 92-25 km variable mesh with the finer area over North America. Preliminary computational tests show good scalability and model evaluation, when using a 3-year simulation (2014-2016) for the uniform mesh case and a monthly simulation of January and July 2016 for the variable mesh case, on ozone and PM2.5 and show reasonable performance with respect to observations. The 92-25 km configuration has a high bias in winter-time surface ozone across the United States, and this bias is consistent with the 120 km result. Summertime surface ozone in the 92-25 km configuration is less biased than the 120 km case. The MPAS-CMAQ system reasonably reproduces the daily variability of daily average PM from the Air Quality System (AQS) network.
The Community Multiscale Air Quality Model (CMAQ) is a local- to hemispheric-scale numerical air quality modeling system developed by the U.S. Environmental Protection Agency (USEPA) and supported by the Community Modeling and Analysis System (CMAS) center. CMAQ is used for regulatory purposes by the USEPA program offices and state and local air agencies and is also widely used by the broader global research community to simulate and understand complex air quality processes and for computational environmental fate and transport and climate and health impact studies. Leveraging state-of-the-science cloud computing resources for high-performance computing (HPC) applications, CMAQ is now available as a fully tested, publicly available technology stack (HPC cluster and software stack) for two major cloud service providers (CSPs). Specifically, CMAQ configurations and supporting materials have been developed for use on their HPC clusters, including extensive online documentation, tutorials and guidelines to scale and optimize air quality simulations using their services. These resources allow modelers to rapidly bring together CMAQ, cloud-hosted datasets, and visualization and evaluation tools on ephemeral clusters that can be deployed quickly and reliably worldwide. Described here are considerations in CMAQ version 5.3.3 cloud use and the supported resources for each CSP, presented through a benchmark application suite that was developed as an example of a typical simulation for testing and verifying components of the modeling system. The outcomes of this effort are to provide findings from performing CMAQ simulations on the cloud using popular vendor-provided resources, to enable the user community to adapt this for their own needs, and to identify specific areas of potential optimization with respect to storage and compute architectures.
We updated the chemical mechanism of the GEOS-Chem global 3-D model of atmospheric chemistry to include new recommendations from the NASA Jet Propulsion Laboratory (JPL) chemical kinetics Data Evaluation 19-5 and from the International Union of Pure and Applied Chemistry (IUPAC) and to balance carbon and nitrogen. We examined the impact of these updates on the GEOS-Chem version 14.0.1 simulation. Notable changes include 11 updates to reactions of reactive nitrogen species, resulting in a 7% net increase in the stratospheric NOx (NO + NO2) burden; an updated CO + OH rate formula leading to a 2.7% reduction in total tropospheric CO; adjustments to the rate coefficient and branching ratios of propane + OH, leading to reduced tropospheric propane (-17%) and increased acetone (+3.5%) burdens; a 41% increase in the tropospheric burden of peroxyacetic acid due to a decrease in the rate coefficient for its reaction with OH, further contributing to reductions in peroxyacetyl nitrate (PAN; -3.8%) and acetic acid (-3.4%); and a number of minor adjustments to halogen radical cycling. Changes to the global tropospheric burdens of other species include -0.7% for ozone, +0.3% for OH (-0.4% for methane lifetime against oxidation by tropospheric OH), +0.8% for formaldehyde, and -1.7% for NOx. The updated mechanism reflects the current state of the science, including complex chemical dependencies of key atmospheric species on temperature, pressure, and concentrations of other compounds. The improved conservation of carbon and nitrogen will facilitate future studies of their overall atmospheric budgets.

