Estimating lightning NOx production over South Africa

Research Brief

Impact of Lightning NOx Emissions on Atmospheric Composition and Meteorology in Africa and Europe

NOx emissions from lightning have been added to the CHIMERE v2020r1 model using a parameterization based on convective clouds. In order to estimate the impact of these emissions on pollutant concentrations, two simulations, using the online coupled WRF-CHIMERE models with and without NOx emissions from lightning, have been carried out over the months of July and August 2013 and over a large area covering Europe and the northern part of Africa. The results show that these emissions modify the pollutant concentrations as well as the meteorology. The changes are most significant where the strongest emissions are located. Adding these emissions improves Aerosol Optical Depth in Africa but has a limited impact on the surface concentrations of pollutants in Europe. For the two-month average we find that the maximum changes are localized and may reach ±0.5 K for 2 m temperature, ±0.5 m s−1 for 10 m wind speed, 10 W m−2 for short wave radiation surface flux, and 50 and 2 μg m−3 for dust and sea salt surface concentrations, respectively. This leads to maximum changes of 1 μg m−3 for surface concentrations of PM2.5.

Simulating Lightning NO_X Production in CMAQv5.2: Evolution of Scientific Updates

This work describes the lightning NOX (LNOX) production schemes in the Community Multiscale Air Quality (CMAQ) model. We first document the existing LNOX production scheme and associated LNOX vertical distribution algorithm. We then describe updates that were made to the scheme originally based on monthly National Lightning Detection Network (mNLDN) observations. The updated scheme uses hourly NLDN (hNLDN) observations. These NLDN-based schemes are good for retrospective model applications when historical lightning data are available. For applications when observed data are not available (i.e., air quality forecasts, future climate studies, and simulations focused outside the NLDN), we have developed a scheme that is based on linear and log-linear parameters derived from regression of multiyear historical NLDN (pNLDN) observations and meteorological model simulations. Preliminary assessment for total column LNOX production reveals that the mNLDN scheme overestimates LNOX by over 40 % during summer months compared with the updated hNLDN scheme that reflects the observed lightning activity more faithfully in time and space. The pNLDN performance varies with year, but it generally produced LNOX columns that are comparable to hNLDN and mNLDN, and in most cases, it outperformed mNLDN. Nevertheless, when no observed lightning data are available, pNLDN can provide reasonable estimates of LNOX emissions over time and space for this important natural NOX source that influences air quality regulations.

Nitrogen oxides in the global upper troposphere: interpreting cloud-sliced NO₂ observations from the OMI satellite instrument

Nitrogen oxides (NOx≡NO+NO2) in the upper troposphere (UT) have a large impact on global tropospheric ozone and OH (the main atmospheric oxidant). New cloud-sliced observations of UT NO2 at 450–280 hPa (∼6–9 km) from the Ozone Monitoring Instrument (OMI) produced by NASA and the Royal Netherlands Meteorological Institute (KNMI) provide global coverage to test our understanding of the factors controlling UT NOx. We find that these products offer useful information when averaged over coarse scales (20∘×32∘, seasonal), and that the NASA product is more consistent with aircraft observations of UT NO2. Correlation with Lightning Imaging Sensor (LIS) and Optical Transient Detector (OTD) satellite observations of lightning flash frequencies suggests that lightning is the dominant source of NOx to the upper troposphere except for extratropical latitudes in winter. The NO2 background in the absence of lightning is 10–20 pptv. We infer a global mean NOx yield of 280±80 moles per lightning flash, with no significant difference between the tropics and midlatitudes, and a global lightning NOx source of 5.9±1.7 Tg N a−1. There is indication that the NOx yield per flash increases with lightning flash footprint and with flash energy.

Nitrogen oxides in the global upper troposphere: interpreting cloud-sliced NO₂ observations from the OMI satellite instrument

Nitrogen oxides (NOx ≡ NO + NO2) in the upper troposphere (UT) have a large impact on global tropospheric ozone and OH (the main atmospheric oxidant). New cloud-sliced observations of UT NO2 at 450–280 hPa (~ 6–9 km) from the OMI satellite instrument produced by NASA and KNMI provide global coverage to test our understanding of the factors controlling UT NOx. We find that these products offer useful information when averaged over coarse scales (20° × 32°, seasonal), and that the NASA product is more consistent with aircraft observations of UT NO2. Correlation with LIS/OTD satellite observations of lightning flash frequencies shows that lightning is the dominant source of NOx to the upper troposphere except for extratropical latitudes in winter. We infer a global mean NOx yield of 280 moles per lightning flash, with no significant difference between the tropics and mid-latitudes, and a global lightning NOx source of 5.6 Tg N a−1. There is indication that the NOx yield per flash increases with lightning flash footprint and with flash energy.

The chemistry–climate model ECHAM6.3-HAM2.3-MOZ1.0

The chemistry–climate model ECHAM-HAMMOZ contains a detailed representation of tropospheric and stratospheric reactive chemistry and state-of-the-art parameterizations of aerosols using either a modal scheme (M7) or a bin scheme (SALSA). This article describes and evaluates the model version ECHAM6.3-HAM2.3-MOZ1.0 with a focus on the tropospheric gas-phase chemistry. A 10-year model simulation was performed to test the stability of the model and provide data for its evaluation. The comparison to observations concentrates on the year 2008 and includes total column observations of ozone and CO from IASI and OMI, Aura MLS observations of temperature, HNO3, ClO, and O3 for the evaluation of polar stratospheric processes, an ozonesonde climatology, surface ozone observations from the TOAR database, and surface CO data from the Global Atmosphere Watch network. Global budgets of ozone, OH, NOx, aerosols, clouds, and radiation are analyzed and compared to the literature. ECHAM-HAMMOZ performs well in many aspects. However, in the base simulation, lightning NOx emissions are very low, and the impact of the heterogeneous reaction of HNO3 on dust and sea salt aerosol is too strong. Sensitivity simulations with increased lightning NOx or modified heterogeneous chemistry deteriorate the comparison with observations and yield excessively large ozone budget terms and too much OH. We hypothesize that this is an impact of potential issues with tropical convection in the ECHAM model.

Characteristics of intercontinental transport of tropospheric ozone from Africa to Asia

In this study, we characterize the transport of ozone from Africa to Asia through the analysis of the simulations of a global chemical transport model, GEOS-Chem, from 1987 to 2006. The receptor region Asia is defined within 5–60∘ N and 60–145∘ E, while the source region Africa is within 35∘ S–15∘ N and 20∘ W–55∘ E and within 15–35∘ N and 20∘ W–30∘ E. The ozone generated in the African troposphere from both natural and anthropogenic sources is tracked through tagged ozone simulation. Combining this with analysis of trajectory simulations using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model, we find that the upper branch of the Hadley cell connects with the subtropical westerlies in the Northern Hemisphere (NH) to form a primary transport pathway from Africa to Asia in the middle and upper troposphere throughout the year. The Somali jet that runs from eastern Africa near the equator to the Indian subcontinent in the lower troposphere is the second pathway that appears only in NH summer. The influence of African ozone mainly appears over Asia south of 40∘ N. The influence shows strong seasonality, varying with latitude, longitude, and altitude. In the Asian upper troposphere, imported African ozone is largest from March to May around 30∘ N (12–16 ppbv) and lowest during July–October around 10∘ N (∼ 2 ppbv). In the Asian middle and lower troposphere, imported African ozone peaks in NH winter between 20 and 25∘ N. Over 5–40∘ N, the mean fractional contribution of imported African ozone to the overall ozone concentrations in Asia is largest during NH winter in the middle troposphere (∼ 18 %) and lowest in NH summer throughout the tropospheric column (∼ 6 %). This seasonality mainly results from the collective effects of the ozone precursor emissions in Africa and meteorology and chemistry in Africa, in Asia and along the transport pathways. The seasonal swing of the Hadley circulation and subtropical westerlies along the primary transport pathway plays a dominant role in modulating the seasonality. There is more imported African ozone in the Asian upper troposphere in NH spring than in winter. This is likely due to more ozone in the NH African upper troposphere generated from biogenic and lightning NOx emissions in NH spring. The influence of African ozone on Asia appears larger in NH spring than in autumn. This can be attributed to both higher altitudes of the elevated ozone in Africa and stronger subtropical westerlies in NH spring. In NH summer, African ozone hardly reaches Asia because of the blocking by the Saharan High, Arabian High, and Tibetan High on the transport pathway in the middle and upper troposphere, in addition to the northward swing of the subtropical westerlies. The seasonal swings of the intertropical convergence zone (ITCZ) in Africa, coinciding with the geographic variations of the ozone precursor emissions, can further modulate the seasonality of the transport of African ozone, owing to the functions of the ITCZ in enhancing lightning NOx generation and uplifting ozone and ozone precursors to upper layers. The strength of the ITCZ in Africa is also found to be positively correlated with the interannual variation of the transport of African ozone to Asia in NH winter. Ozone from NH Africa makes up over 80 % of the total imported African ozone over Asia in most altitudes and seasons. The interhemispheric transport of ozone from southern hemispheric Africa (SHAF) is most evident in NH winter over the Asian upper troposphere and in NH summer over the Asian lower troposphere. The former case is associated with the primary transport pathway in NH winter, while the latter case is associated with the second transport pathway. The intensities of the ITCZ in Africa and the Somali jet can each explain ∼ 30 % of the interannual variations in the transport of ozone from SHAF to Asia in the two cases.