Lightning NOx Production and Its Consequences for Tropospheric Chemistry

Cloud-resolving case-study simulations of convective transport and lightning NO production have yielded results which are directly applicable to the design of lightning parameterizations for global chemical transport models. In this work we have used cloud-resolving models (the Goddard Cumulus Ensemble Model (GCE) and MMS) to drive an off-line cloud-scale chemical transport model (CSCTM). The CSCTM, in conjunction with aircraft measurements of NO x in thunderstorms and ground-l;>ased lightning observations, has been used to constrain the amount of NO produced per flash. Cloud and chemistry simulations for several case studies of storms in different environments will be presented. Observed lightning flash rates have been incorporated into the CSCTM, and several scenarios of NO production per intracloud (IC) and per cloud-to-ground (CG) flash have been tested for each storm. The resulting NOx mixing ratios are compared with aircraft measurements taken within the storm (typically the anvil region) to determine the most likely NO production scenario. The range of values of NO production per flash (or per meter of lightning channel length) that have been deduced from the model will be shown and compared with values of production in the literature that have been deduced from observed NO spikes and from anvil flux calculations. Results show that on a per flash basis, IC flashes are nearly as productive of NO as CG flashes. This result simplifies the lightning parameterization for global models (ie., an algorithm for estimating the IC/CG ratio is not necessary). Vertical profiles of lightning NOx mass at the end of the 3-D storm simulations have been summarized to yield suggested profiles for use in global models. Estimates of mean NO production per flash vary by a factor of three from one simulated storm to another. When combined with the global flash rate of 44 flashes per second from NASA's Optical Transient Detector (OTD) measurements, these estimates and the results from other techniques yield global NO production rates of2-9 TgN/year. Simulations of the photochemistry over the 24 hours following a storm has been performed to determine the additional ozone production which can be attributed to lightning NO. Convective transport of HOx precursors leads to the generation of a HOx plume which substantially aids the downstream ozone production

Tropospheric Ozone as a Short-lived Chemical Climate Forcer

Tropospheric ozone is the third most important greenhouse gas according to the most recent IPCC assessment. However, tropospheric ozone is highly variable in both space and time. Ozone that is located in the vicinity of the tropopause has the greatest effect on climate forcing. Nitrogen oxides (NOx) are the most important precursors for ozone In most of the troposphere. Therefore, pollution that is lofted upward in thunderstorm updrafts or NOx produced by lightning leads to efficient ozone production in the upper troposphere, where ozone is most important climatically. Global and regional model estimates of the impact of North American pollution and lightning on ozone radiative forcing will be presented. It will be shown that in the Northern Hemisphere summer, the lightning effect on ozone radiative forcing can dominate over that of pollution, and that the radiative forcing signal from North America extends well into Europe and North Africa. An algorithm for predicting lightning flash rates and estimating lightning NOx emissions is being incorporated into the NASA GEOS-5 Chemistry and Climate Model. Changes in flash rates and emissions over an ENSO cycle and in future climates will be assessed, along with the resulting changes in upper tropospheric ozone. Other research on the production of NOx per lightning flash and its distribution in the vertical based on cloud-resolving modeling and satellite observations will be presented. Distributions of NO2 and O3 over the Middle East from the OMI instrument on NASA's Aura satellite will also be shown

An estimate of the stratospheric contribution to springtime tropospheric ozone maxima using TOPSE measurements and beryllium-7 simulations

Measurements of tropospheric ozone (O3) between 30°N and 70°N show springtime maxima at remote locations. The contribution of seasonal changes in stratosphere–troposphere exchange (STE) to these maxima was investigated using measurements from the Tropospheric Ozone Production about the Spring Equinox Experiment (TOPSE) campaign and the beryllium-7 (7Be) distribution from a calculation driven by fields from the Goddard Earth Observing System Data Assimilation System (GEOS DAS). Comparison with TOPSE measurements revealed that upper tropospheric model-calculated 7Be mixing ratios were reasonable (a change from previous calculations) but that lower tropospheric mixing ratios were too low most likely due to an overestimation of scavenging. Temporal fluctuations were well captured although their amplitudes were often underestimated. Analysis of O3measurements indicated that O3 mixing ratios increased by 5–10% month−1 for θ \u3c 300 K (the underworld) and by 10–15% month−1 for θ \u3e 300 K (the tropospheric middleworld). 7Be mixing ratios decreased with time for θ \u3c 290 K and increased with time for θ \u3e 300 K. Model-calculated middleworld increases of 7Be were a factor of 2 less than measured increases. 7Be with a stratospheric source (strat-7Be) increased by 4.6–8.8% month−1 along TOPSE flight paths within the tropospheric middleworld. Increases in strat-7Be were not seen along TOPSE flight paths in the underworld. Assuming changes in tropospheric O3 with a stratospheric source are the same as changes in strat-7Be and that 50% of O3 in the region of interest is produced in the stratosphere, changes in STE explain 20–60% of O3 increases in the tropospheric middleworld and less than 33% of O3 increases in the underworld

A TROPOMI- and GLM-Based Estimate of NOx Production by Lightning over the U.S.

Lightning produces NO because the extreme temperatures (>20000 K) in lightning channels dissociate molecular O2 and molecular N2, which then combine to form NOx which quickly reacts with O3 to form NO2. Lightning is responsible for 10-15% of NOx emissions globally. This is 2 8 Tg N a-1 [Schumann and Huntrieser, 2007] or 100 to 400 mol per flash. Much of the uncertainty stems from limited knowledge of lightning NOx production per flash (LNOx PE) or per unit flash length. Most LNOx is injected into mid- and upper-troposphere where away from deep convection its lifetime is longer relative to lower troposphere NOx. NOx in this region enhances the concentrations of upper tropospheric NOy, OH, and O3 and contributes to positive radiative forcing by O3 and negative forcing by CH4. We have previously used OMI NO2 to obtain estimates of LNOx production per flash over the Gulf of Mexico (Pickering et al., 2016, JGR), in convective events during NASAs TC4 field program (Bucsela et al., 2010, JGR), and over broad regions of the tropics (Allen et al., 2019, JGR) and midlatitudes (Bucsela et al., 2019, JGR). In the latter studies, we obtained PE values of 170 100 mol flash and 180 100 mol flash, respectively

A Three-Dimensional Total Odd Nitrogen (NO(y)) Simulation During SONEX using a Stretched-Grid Chemical Transport Model

The relative importance of various odd nitrogen (NOy) sources including lightning, aircraft, and surface emissions on upper tropospheric total odd nitrogen is illustrated as a first application of the three-dimensional Stretched-Grid University of Maryland/Goddard Chemical-Transport Model (SG-GCTM). The SG-GCTM has been developed to look at the effect of localized sources and/or small scale mixing processes on the large-scale or global chemical balance. For this simulation, the stretched-arid was chosen so that its maximum resolution is located over eastern North America and the North Atlantic; a region that includes most of the SONEX (the SASS (Subsonic Assessment) Ozone and Nitrogen Oxides Experiment) flight paths. The SONEX period (October-November 1997) is simulated by driving the SG-GCTM with assimilated data from the GEOS-STRAT DAS (Goddard Earth Observing System-STRAT Data Assimilation System). A new algorithm is used to parameterize the lightning, flash rates that are needed to calculate emissions of NOy by lightning. Model-calculated upper tropospheric NOy and NOy measurements from the NASA DC-8 aircraft are compared. Spatial variations in NOy were well captured especially with the stretched-grid run; however, model-calculated concentrations were often too high in the upper troposphere, particularly during the first several flights. The lightning algorithm does a reasonably good job; however, the use of emissions from observed lightning, flashes significantly improves the simulation on a few occasions, especially November 3, 1997, indicating that significant uncertainty remains in parameterizing lightning in CTMS. Aircraft emissions play a relatively minor role (about 12%) in the upper tropospheric NOY budget averaged along SONEX flight paths; however, the contribution of such emmissions is as large as about 30% during portions of some flights

The Effects of Lightning NO(x) Production during the July 21 EULINOX Storm studied with a 3-D Cloud-scale Chemical Transport Model

The July 21,1998 thunderstonn observed during the European Lightning Nitrogen Oxides Project (EULINOX) project was simulated using the three-dimensional Goddard Cumulus Ensemble (GCE) model. The simulation successfully reproduced a number of observed storm features including the splitting of the original cell into a southern cell which developed supercell characteristics, and a northern cell which became multicellular. Output from the GCE simulation was used to drive an offline cloud-scale chemical transport model which calculates tracer transport and includes a parameterization of lightning NO(x) production which uses observed flash rates as input. Estimates of lightning NO(x) production were deduced by assuming various values of production per intracloud and production per cloud-to-ground flash and comparing the results with in-cloud aircraft observations. The assumption that both types of flashes produce 360 moles of NO per flash on average compared most favorably with column mass and probability distribution functions calculated from observations. This assumed production per flash corresponds to a global annual lightning NOx source of 7 Tg N per yr. Chemical reactions were included in the model to evaluate the impact of lightning NO(x), on ozone. During the storm, the inclusion of lightning NOx in the model results in a small loss of ozone (on average less than 4 ppbv) at all model levels. Simulations of the chemical environment in the 24 hours following the storm show on average a small increase in the net production of ozone at most levels resulting from lightning NO(x), maximizing at approximately 5 ppbv per day at 5.5 km. Between 8 and 10.5 km, lightning NO(x) causes decreased net ozone production

Planning, implementation, and first results of the Tropical Composition, Cloud and Climate Coupling Experiment (TC4)

The Tropical Composition, Cloud and Climate Coupling Experiment (TC4), was based in Costa Rica and Panama during July and August 2007. The NASA ER-2, DC-8, and WB-57F aircraft flew 26 science flights during TC4. The ER-2 employed 11 instruments as a remote sampling platform and satellite surrogate. The WB-57F used 25 instruments for in situ chemical and microphysical sampling in the tropical tropopause layer (TTL). The DC-8 used 25 instruments to sample boundary layer properties, as well as the radiation, chemistry, and microphysics of the TTL. TC4 also had numerous sonde launches, two ground-based radars, and a ground-based chemical and microphysical sampling site. The major goal of TC4 was to better understand the role that the TTL plays in the Earth's climate and atmospheric chemistry by combining in situ and remotely sensed data from the ground, balloons, and aircraft with data from NASA satellites. Significant progress was made in understanding the microphysical and radiative properties of anvils and thin cirrus. Numerous measurements were made of the humidity and chemistry of the tropical atmosphere from the boundary layer to the lower stratosphere. Insight was also gained into convective transport between the ground and the TTL, and into transport mechanisms across the TTL. New methods were refined and extended to all the NASA aircraft for real-time location relative to meteorological features. The ability to change flight patterns in response to aircraft observations relayed to the ground allowed the three aircraft to target phenomena of interest in an efficient, well-coordinated manner

DISCOVER-AQ: An Overview and Initial Comparisons of NO2 with OMI Observations

The first deployment of the Earth Venture -1 DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project was conducted during July 2011 in the Baltimore-Washington region. Two aircraft (a P-3B for in-situ sampling and a King Air for remote sensing) were used along with an extensive array of surface-based in-situ and remote sensing instrumentation. Fourteen flight days were accomplished by both aircraft and over 250 profiles of trace gases and aerosols were performed by the P-3B over surface air quality monitoring stations, which were specially outfitted with sunphotometers and Pandora UV/Vis spectrometers. The King Air flew with the High Spectral Resolution Lidar for aerosols and the ACAM UV/Vis spectrometer for trace gases. This suite of observations allows linkage of surface air quality with the vertical distributions of gases and aerosols, with remotely-sensed column amounts observed from the surface and from the King Air, and with satellite observations from Aura (OMI and TES), GOME-2, MODIS and GOES. The DISCOVER-AQ data will allow determination of under what conditions satellite retrievals are indicative of surface air quality, and they will be useful in planning new satellites. In addition to an overview of the project, a preliminary comparison of tropospheric column NO2 densities from the integration of in-situ P-3B observations, from the Pandoras and ACAM, and from the new Goddard OMI NO2 algorithm will be presented

Impact of Lightning-NO Emissions on Summertime U.S. Photochemistry as Determined Using the CMAQ Model with NLDN-Constrained Flash Rates

Lightning-NO emissions are responsible for 15-30 ppbv enhancements in upper tropospheric ozone over the eastern United States during the summer time. Enhancements vary from year to year but were particularly large during the summer of 2006, a period during which meteorological conditions were particularly conducive to ozone formation. A lightning-NO parameterization has been developed that can be used with the CMAQ model. Lightning-NO emissions in this scheme are assumed to be proportional to convective precipitation rate and scaled so that monthly average flash rates in each grid box match National Lightning Detection Network (NLDN) observed flash rates after adjusting for climatological intracloud to cloud-to-ground (IC/CG) ratios. The contribution of lightning-NO emissions to eastern United States NOx and ozone distributions during the summer of 2006 will be evaluated by comparing results of 12- km CMAQ simulations with and without lightning-NO emissions to measurements from the IONS field campaign and to satellite retrievals from the Tropospheric Emission Spectrometer (TES) and the Ozone Monitoring Instrument (OMI) aboard the Aura satellite. Special attention will be paid to the impact of the assumed vertical distribution of emissions on upper tropospheric NOx and ozone amounts