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

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

The Sensitivity of U.S. Surface Ozone Formation to NOx, and VOCs as Viewed from Space

We investigated variations in the sensitivity of surface ozone formation in summer to precursor species concentrations of volatile organic compounds (VOCs) and nitrogen oxides (NO(x)) as inferred from the ratio of tropospheric columns of formaldehyde and nitrogen dioxide from the Aura Ozone Monitoring Instrument (OMI). The data indicate that ozone formation became: 1. more sensitive to NO(x) over most of the U.S, from 2005 to 2007 because of substantial decreases in NO(x) emissions primarily from stationary sources, and 2. more sensitive to NO(x) with increasing temperature, in part because emissions of highly reactive, biogenic isoprene increase with temperature, thus increasing the total VOC reactivity. Based on our interpretation of the data, current strategies implemented to reduce unhealthy levels of surface ozone should focus more on reducing NO(x) emissions, except in some downtown areas which have historically benefited from reductions in VOC emissions

Current Applications of OMI Tropospheric NO2 Data for Air Quality and a Look to the Future

Ozone Monitoring Instrument (OMI) Tropospheric NO2 products are being used to enhance the ability to monitor changes in NO2 air quality, update emission inventories, and evaluate regional air quality models. Trends in tropospheric column NO2 have been examined over the eastern United States in relation to emissions changes mandated by regulatory actions. Decreases of 20 to 40 percent over the period 2005 to 2008 were noted, largely in response to major emission reductions at power plants. The OMI data have been used to identify regions in which the opposite trend has been found. We have also used OMI NO2 in efforts to improve emission inventories for NOx emissions from soil. Lightning NOx emissions have been added to CMAQ, the US Environmental Protection Agency's regional air quality model. Evaluation of the resulting NO2 columns in the model is being conducted using the OMI NO2 observations. Community Multiscale Air Quality (CMAQ) together with the OMI NO2 data comprise a valuable tool for monitoring and predicting air quality. Looking to the future, we expect that the combination of Global Ozone Monitoring Experiment-2 (GOME-2) (morning) and OMI (afternoon) data sets obtained through use of the same retrieval algorithms will substantially increase the possibility of successful integration of satellite information into regional air quality forecast models. Farther down the road, we anticipate the Geostationary Coastal and Air Pollution Events (GEO-CAPE) platform to supply data possibly on an hourly basis, allowing much more comprehensive analysis of air quality from space

The Observed Response of Ozone Monitoring Instrument (OMI) NO2 Columns to NOx Emission Controls on Power Plants in the United States: 2005-2011

We show that Aura Ozone Monitoring Instrument (OMI) nitrogen dioxide (NO2) tropospheric column data may be used to assess changes of the emissions of nitrogen oxides (NOx) from power plants in the United States, though careful interpretation of the data is necessary. There is a clear response for OMI NO2 data to NOx emission reductions from power plants associated with the implementation of mandated emission control devices (ECDs) over the OMI record (2005e2011). This response is scalar for all intents and purposes, whether the reduction is rapid or incremental over several years. However, it is variable among the power plants, even for those with the greatest absolute decrease in emissions. We document the primary causes of this variability, presenting case examples for specific power plants

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

Application of OMI Observations to a Space-Based Indicator of NOx and VOC Controls on Surface Ozone Formation

We investigated variations in the relative sensitivity of surface ozone formation in summer to precursor species concentrations of volatile organic compounds (VOCs) and nitrogen oxides (NOx) as inferred from the ratio of the tropospheric columns of formaldehyde to nitrogen dioxide (the "Ratio") from the Aura Ozone Monitoring Instrument (OMI). Our modeling study suggests that ozone formation decreases with reductions in VOCs at Ratios less than 1 and NOx at Ratios greater than 2; both NOx and VOC reductions may decrease ozone formation for Ratios between 1 and 2. Using this criteria. the OMI data indicate that ozone formation became: 1. more sensitive to NOx over most of the United States from 2005 to 2007 because of the substantial decrease in NOx emissions, primarily from stationary sources, and the concomitant decrease in the tropospheric column of NO2. and 2. more sensitive to NOx with increasing temperature, in part because emissions of highly reactive, biogenic isoprene increase with temperature, thus increasing the total VOC reactivity. In cities with relatively low isoprene emissions (e.g .. Chicago). the data clearly indicate that ozone formation became more sensitive to NOx from 2005 to 2007. In cities with relatively high isoprene emissions (e.g ., Atlanta), we found that the increase in the Ratio due to decreasing NOx emissions was not obvious as this signal was convolved with variations in the Ratio associated with the temperature dependence of isoprene emissions and, consequently, the formaldehyde concentration

A trajectory modeling investigation of the biomass burning-tropical ozone relationship

The hypothesis that tropical total O3 maxima seen by the TOMS satellite derive from African biomass burning has been tested using isentropic trajectory analyses with global meteorological data fields. Two case studies from the 1989 biomass burning season demonstrate that a large fraction of the air arriving at the location of TOMS O3 maxima passed over regions of intense burning. Other trajectories initiated at a series of points over Africa and the Atlantic suggest flight strategies for field studies to be conducted in September 1992