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Accurate meteorological fields are imperative for correct chemical transport modeling. Observation nudging, along with objective analysis, is generally considered a low-cost and effective technique to improve meteorological simulations. However, the meteorological impact of observation nudging on chemistry has not been well characterized. This study involved two simulations to analyze the impact of observation nudging on simulated meteorology and ozone concentrations during the 2013 Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) Texas campaign period, using the Weather Research and Forecasting (WRF) and Community Multiscale Air Quality (CMAQ) models. The results showed improved correlations between observed and simulated parameters. For example, the index of agreement (IOA) improved by about 9 % for surface temperature and 6–11 % for surface zonal (U-WIND) and meridional (V-WIND) winds when observation nudging was employed. Analysis of a cold front event indicated that nudging improved the timing of wind transition during the front passage. Observation nudging also reduced the model biases for the planetary boundary layer height predictions. Additionally, the IOA for CMAQ simulated surface ozone improved by 6 % during the simulation period. The high-ozone episode on 25 September was a post-front ozone event in Houston. The small-scale morning wind shifts near the Houston Ship Channel combined with higher aloft ozone early morning likely caused the day's ozone exceedance. While observation nudging did not recreate the wind shifts on that day and failed to reproduce the observed high ozone, analyses of surface and aircraft data found that observation nudging helped the model yield improved ozone predictions. In a 2 h period during the event, substantially better winds in the sensitivity case noticeably improved the ozone. The average IOA for ozone in the period increased from just over 0.4 to near 0.7. Further work on improving the capability of nudging to reproduce local meteorological events such as stagnations and wind reversals could enhance a chemical transport model's skill for predicting high-ozone events.

We derive free-tropospheric NO2 volume mixing ratios (VMRs) by applying a cloud-slicing technique to data from the Ozone Monitoring Instrument (OMI) on the Aura satellite. In the cloud-slicing approach, the slope of the above-cloud NO2 column versus the cloud scene pressure is proportional to the NO2 VMR. In this work, we use a sample of nearby OMI pixel data from a single orbit for the linear fit. The OMI data include cloud scene pressures from the rotational-Raman algorithm and above-cloud NO2 vertical column density (VCD) (defined as the NO2 column from the cloud scene pressure to the top of the atmosphere) from a differential optical absorption spectroscopy (DOAS) algorithm. We compare OMI-derived NO2 VMRs with in situ aircraft profiles measured during the NASA Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in 2006. The agreement is generally within the estimated uncertainties when appropriate data screening is applied. We then derive a global seasonal climatology of free-tropospheric NO2 VMR in cloudy conditions. Enhanced NO2 in the free troposphere commonly appears near polluted urban locations where NO2 produced in the boundary layer may be transported vertically out of the boundary layer and then horizontally away from the source. Signatures of lightning NO2 are also shown throughout low and middle latitude regions in summer months. A profile analysis of our cloud-slicing data indicates signatures of lightning-generated NO2 in the upper troposphere. Comparison of the climatology with simulations from the global modeling initiative (GMI) for cloudy conditions (cloud optical depth > 10) shows similarities in the spatial patterns of continental pollution outflow. However, there are also some differences in the seasonal variation of free-tropospheric NO2 VMRs near highly populated regions and in areas affected by lightning-generated NOx.

Global-scale chemical transport model simulations indicate lightning NOx dominates upper tropospheric O3 production above Eastern North America during summertime but vary in their estimates. To improve our understanding, a regional-scale model (REAM) with higher resolution is applied. To examine the uncertainties in modeling the impact of convective transport and lightning NOx production on upper tropospheric chemical tracer distributions, REAM simulations of chemical tracers are driven by two meteorological models, WRF and MM5, with different cumulus convective parameterizations. The model simulations are evaluated using INTEX-A aircraft measurements and satellite measurements of NO2 columns and cloud top pressure, and we find that mid and upper tropospheric trace gas concentrations are affected strongly by convection and lightning NOx production. WRF with the KF-eta convection scheme simulates larger convective updraft mass fluxes below 150 hPa than MM5 with the Grell scheme. The inclusion of the entrainment and detrainment processes leads to more outflow in the mid troposphere in WRF than MM5. The ratio of C2H6/C3H8 is found to be a sensitive parameter to convective outflow; the simulation by WRF-REAM is in closer agreement with INTEX-A measurements than MM5-REAM, implying that convective mass fluxes by WRF are more realistic. WRF also simulates lower cloud top heights (10–12 km) than MM5 (up to 16 km), and hence smaller amounts of estimated (intra-cloud) lightning NOx and lower emission altitudes. WRF simulated cloud top heights are in better agreement with GOES satellite measurements than MM5. Simulated lightning NOx production difference (due primarily to cloud top height difference) is mostly above 12 km. At 8–12 km, the models simulate a contribution of 60–75% of NOx and up to 20 ppbv of O3 from lightning, although the decrease of lightning NOx effect from the Southeast to Northeast and eastern Canada is overestimated. The model differences and biases found in this study reflect some major uncertainties of upper tropospheric NOx and O3 simulations driven by those in meteorological simulations and lightning parameterizations.

Lightning NOx emissions calculated using the US National Lightning Detection Network data were found to account for 30% of the total NOx emissions for July–August 2004, a period chosen both for having higher lightning NOx production and high ozone levels, thus maximizing the likelihood that such emissions could impact peak ozone levels. Including such emissions led to modest, but sometimes significant increases in simulated surface ozone when using the Community Multi-scale Air Quality Model (CMAQ). Three model simulations were performed, two with the addition of lightning NOx emissions, and one without. Domain-wide daily maximum 8-h ozone changes due to lightning NOx were less than 2 ppbv in 71% of the cases with a maximum of 10 ppbv; whereas the difference in 1-h ozone was less than 2 ppbv in 77% of the cases with a maximum of 6 ppbv. Daily maximum 1-h and 8-h ozone for grids containing O3 monitoring stations changed slightly, with more than 43% of the cases differing less than 2 ppbv. The greatest differences were 42 ppbv for both 1-h and 8-h O3, though these tended to be on days of lower ozone. Lightning impacts on the season-wide maximum 1-h and 8-h averaged ozone decreased starting from the 1st to 4th highest values (an average of 4th highest, 8-h values is used for attainment demonstration in the US). Background ozone values from the y-intercept of O3 versus NOz curve were 42.2 and 43.9 ppbv for simulations without and with lightning emissions, respectively. Results from both simulations with lightning NOx suggest that while North American lightning production of NOx can lead to significant local impacts on a few occasions, they will have a relatively small impact on typical maximum levels and determination of Policy Relevant Background levels.