The knowledge of the lightning-induced nitrogen oxides (LNOx) source is important for understanding and predicting the nitrogen oxides and ozone distributions in the troposphere and their trends, the ...oxidising capacity of the atmosphere, and the lifetime of trace gases destroyed by reactions with OH. This knowledge is further required for the assessment of other important NOx sources, in particular from aviation emissions, the stratosphere, and from surface sources, and for understanding the possible feedback between climate changes and lightning. This paper reviews more than 3 decades of research. The review includes laboratory studies as well as surface, airborne and satellite-based observations of lightning and of NOx and related species in the atmosphere. Relevant data available from measurements in regions with strong LNOx influence are identified, including recent observations at midlatitudes and over tropical continents where most lightning occurs. Various methods to model LNOx at cloud scales or globally are described. Previous estimates are re-evaluated using the global annual mean flash frequency of 44±5 s−1 reported from OTD satellite data. From the review, mainly of airborne measurements near thunderstorms and cloud-resolving models, we conclude that a "typical" thunderstorm flash produces 15 (2–40)×1025 NO molecules per flash, equivalent to 250 mol NOx or 3.5 kg of N mass per flash with uncertainty factor from 0.13 to 2.7. Mainly as a result of global model studies for various LNOx parameterisations tested with related observations, the best estimate of the annual global LNOx nitrogen mass source and its uncertainty range is (5±3) Tg a−1 in this study. In spite of a smaller global flash rate, the best estimate is essentially the same as in some earlier reviews, implying larger flash-specific NOx emissions. The paper estimates the LNOx accuracy required for various applications and lays out strategies for improving estimates in the future. An accuracy of about 1 Tg a−1 or 20%, as necessary in particular for understanding tropical tropospheric chemistry, is still a challenging goal.
Lightning is an important natural source of nitrogen oxide especially in the middle and upper troposphere. Hence, it is essential to represent lightning in chemistry transport and coupled ...chemistry-climate models. Using ERA-Interim meteorological reanalysis data we compare the lightning flash density distributions produced using several existing lightning parametrisations, as well as a new parametrisation developed on the basis of upward cloud ice flux at 440 hPa. The use of ice flux forms a link to the non-inductive charging mechanism of thunderstorms. Spatial and temporal distributions of lightning flash density are compared to tropical and subtropical observations for 2007-2011 from the Lightning Imaging Sensor (LIS) on the Tropical Rainfall Measuring Mission (TRMM) satellite. The well-used lightning flash parametrisation based on cloud-top height has large biases but the derived annual total flash density has a better spatial correlation with the LIS observations than other existing parametrisations. A comparison of flash density simulated by the different schemes shows that the cloud-top height parametrisation has many more instances of moderate flash densities and fewer low and high extremes compared to the other parametrisations. Other studies in the literature have shown that this feature of the cloud-top height parametrisation is in contrast to lightning observations over certain regions. Our new ice flux parametrisation shows a clear improvement over all the existing parametrisations with lower root mean square errors (RMSEs) and better spatial correlations with the observations for distributions of annual total, and seasonal and interannual variations. The greatest improvement with the new parametrisation is a more realistic representation of the zonal distribution with a better balance between tropical and subtropical lightning flash estimates. The new parametrisation is appropriate for testing in chemistry transport and chemistry-climate models that use a lightning parametrisation.
Lightning is an important source of NOx in the free troposphere, especially in the tropics, with strong impact on ozone production. However, estimates of lightning NOx (LNOx ) production efficiency ...(LNOx per flash) are still quite uncertain. In this study we present a systematic analysis of NO2 column densities from SCIAMACHY measurements over active thunderstorms, as detected by the World-Wide Lightning Location Network (WWLLN), where the WWLLN detection efficiency was estimated using the flash climatology of the satellite lightning sensors LIS/OTD. Only events with high lightning activity are considered, where corrected WWLLN flash rate densities inside the satellite pixel within the last hour are above 1 /km2 /h. For typical SCIAMACHY ground pixels of 30 × 60 km2 , this threshold corresponds to 1800 flashes over the last hour, which, for literature estimates of lightning NOx production, should result in clearly enhanced NO2 column densities. From 2004-2008, we find 287 coincidences of SCIAMACHY measurements and high WWLLN flash rate densities. For some of these events, a clear enhancement of column densities of NO2 could be observed, indeed. But overall, the measured column densities are below the expected values by more than one order of magnitude, and in most of the cases, no enhanced NO2 could be found at all. Our results are in contradiction to the currently accepted range of LNOx production per flash of 15 (2-40)×1025 molec/flash. This probably partly results from the specific conditions for the events under investigation, i.e. events of high lightning activity in the morning (local time) and mostly (for 162 out of 287 events) over ocean. Within the detected coincidences, the highest NO2 column densities were observed around the US Eastcoast. This might be partly due to interference with ground sources of NOx being uplifted by the convective systems. However, it could also indicate that flashes in this region are particularly productive. We conclude that current estimates of LNOx production might be biased high for two reasons. First, we observe a high variability of NO2 for coincident lightning events. This high variability can easily cause a publication bias, since studies reporting on high NOx production have likely been published, while studies finding no or low amounts of NOx might have been rejected as errorneous or not significant. Second, many estimates of LNOx production in literature have been performed over the US, which is probably not representative for global lightning.
Air quality transcends all scales with in the atmosphere from the local to the global with handovers and feedbacks at each scale interaction. Air quality has manifold effects on health, ecosystems, ...heritage and climate. In this review the state of scientific understanding in relation to global and regional air quality is outlined. The review discusses air quality, in terms of emissions, processing and transport of trace gases and aerosols. New insights into the characterization of both natural and anthropogenic emissions are reviewed looking at both natural (e.g. dust and lightning) as well as plant emissions. Trends in anthropogenic emissions both by region and globally are discussed as well as biomass burning emissions. In terms of chemical processing the major air quality elements of ozone, non-methane hydrocarbons, nitrogen oxides and aerosols are covered. A number of topics are presented as a way of integrating the process view into the atmospheric context; these include the atmospheric oxidation efficiency, halogen and HOx chemistry, nighttime chemistry, tropical chemistry, heat waves, megacities, biomass burning and the regional hot spot of the Mediterranean. New findings with respect to the transport of pollutants across the scales are discussed, in particular the move to quantify the impact of long-range transport on regional air quality. Gaps and research questions that remain intractable are identified. The review concludes with a focus of research and policy questions for the coming decade. In particular, the policy challenges for concerted air quality and climate change policy (co-benefit) are discussed.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
The eruption of the Eyjafjallajökull volcano, Iceland, in April and May 2010 caused unprecedented disruptions of European air traffic showing that timely monitoring of volcanic ash and SO2 dispersion ...as well as the corresponding plume heights are important for aviation safety. This paper describes the observations of SO2 and BrO columns in the eruption plume and the determination of the SO2 plume height using the GOME‐2 satellite instrument. During the eruptive period in May 2010, SO2 total columns of up to ∼20 DU and BrO columns of ∼7.7 × 1013 molec/cm2 were detected. The BrO/SO2 ratio estimated from the GOME‐2 observations of the Eyjafjallajökull eruption varies from 1.1 × 10−4 to 2.1 × 10−4. The SO2 plume heights estimated from the GOME‐2 observations on 5 May range from 8–13 km and mostly agree within 1–3 km with visual observations, radar data and modeling results. Furthermore, the GOME‐2 SO2 observations are compared with in situ measurements of the DLR Falcon aircraft on 17 and 18 May 2010 and with Brewer instruments at Valentia, Ireland and Hohenpeissenberg, Germany. The SO2 columns derived from the Falcon profile measurements range from 0.6–4.7 DU and the comparison with the GOME‐2 measurements shows a good agreement, mainly within 1 DU. The Brewer observations at Hohenpeissenberg also agree well with the GOME‐2 measurements with a daily average SO2 column of ∼1.3 DU during the overpass of the SO2 cloud on 18 May, whereas the Brewer instrument at Valentia shows up to 50% higher SO2 columns (∼8 DU) on 11 May.
Key Points
SO2 and BrO in the eruption plume of Eyjafjallajokull using GOME‐2
Direct retreival of the SO2 plume height from GOME‐2 measurements
Comparison of GOME‐2 data with model simulations, Falcon and Brewer observations
A case of long‐range transport of a biomass burning plume from Alaska to Europe is analyzed using a Lagrangian approach. This plume was sampled several times in the free troposphere over North ...America, the North Atlantic and Europe by three different aircraft during the IGAC Lagrangian 2K4 experiment which was part of the ICARTT/ITOP measurement intensive in summer 2004. Measurements in the plume showed enhanced values of CO, VOCs and NOy, mainly in form of PAN. Observed O3 levels increased by 17 ppbv over 5 days. A photochemical trajectory model, CiTTyCAT, was used to examine processes responsible for the chemical evolution of the plume. The model was initialized with upwind data and compared with downwind measurements. The influence of high aerosol loading on photolysis rates in the plume was investigated using in situ aerosol measurements in the plume and lidar retrievals of optical depth as input into a photolysis code (Fast‐J), run in the model. Significant impacts on photochemistry are found with a decrease of 18% in O3 production and 24% in O3 destruction over 5 days when including aerosols. The plume is found to be chemically active with large O3 increases attributed primarily to PAN decomposition during descent of the plume toward Europe. The predicted O3 changes are very dependent on temperature changes during transport and also on water vapor levels in the lower troposphere which can lead to O3 destruction. Simulation of mixing/dilution was necessary to reproduce observed pollutant levels in the plume. Mixing was simulated using background concentrations from measurements in air masses in close proximity to the plume, and mixing timescales (averaging 6.25 days) were derived from CO changes. Observed and simulated O3/CO correlations in the plume were also compared in order to evaluate the photochemistry in the model. Observed slopes change from negative to positive over 5 days. This change, which can be attributed largely to photochemistry, is well reproduced by multiple model runs even if slope values are slightly underestimated suggesting a small underestimation in modeled photochemical O3 production. The possible impact of this biomass burning plume on O3 levels in the European boundary layer was also examined by running the model for a further 5 days and comparing with data collected at surface sites, such as Jungfraujoch, which showed small O3 increases and elevated CO levels. The model predicts significant changes in O3 over the entire 10 day period due to photochemistry but the signal is largely lost because of the effects of dilution. However, measurements in several other BB plumes over Europe show that O3 impact of Alaskan fires can be potentially significant over Europe.
In this paper we present simulations with a Lagrangian particle dispersion model to study the intercontinental transport of pollution from North America during an aircraft measurement campaign over ...Europe. The model was used for both the flight planning and a detailed source analysis after the campaign, which is described here with examples from two episodes. Forward calculations of emission tracers from North America, Europe, and Asia were made in order to understand the transport processes. Both episodes were preceded by stagnant conditions over North America, leading to the accumulation of pollutants in the North American boundary layer. Both anthropogenic sources and, to a lesser extent, forest fire emissions contributed to this pollution, which was then exported by warm conveyor belts to the middle and upper troposphere, where it was transported rapidly to Europe. Concentrations of many trace gases (CO, NOy, CO2, acetone, and several volatile organic compounds; O3 in one case) and of ambient atmospheric ions measured aboard the research aircraft were clearly enhanced in the pollution plumes compared to the conditions outside the plumes. Backward simulations with the particle model were introduced as an indispensable tool for a more detailed analysis of the plume's source region. They make trajectory analyses (which, to date, were mainly used to interpret aircraft measurement data) obsolete. Using an emission inventory, we could decompose the tracer mixing ratios at the receptors (i.e., along the flight tracks) into contributions from every grid cell of the inventory. For both plumes we found that emission sources contributing to the tracer concentrations over Europe were distributed over large areas in North America. In one case, sources in California, Texas, and Florida contributed almost equally, and smaller contributions were also made by other sources located between the Yucatan Peninsula and Canada. In the other case, sources in eastern North America, including moderate contributions from forest fires, were most important. The plume's maximum was mainly caused by anthropogenic emissions from the New York area. To our knowledge, this is the first case reported where a pollution plume from a megacity was reliably detected over another continent.
We present simulations performed with six lightning parameterizations implemented in the Community Atmosphere Model (CAM5). The amount of lightning‐produced nitrogen oxides (LNOx) by the various ...schemes considered is estimated. We provide some insight on how the lightning NO injected in the atmosphere influences the global concentrations of key chemical species such as OH, HO2, H2O2, NOx, O3, SO2, CO, and HNO3. The vertical global averaged densities of HO2, H2O2, CO, and SO2 are depleted due to lightning while those of NO, NO2, O3, OH, and HNO3 increase. Our results indicate that the parameterizations based on the upward ice flux (ICEFLUX) exhibit the largest global and midlatitude spatial correlations (0.73 and 0.632 for ICEFLUX and 0.72 and 0.553 for cloud top height) with respect to satellite global flash rate observations. Five out of the six lightning schemes investigated exhibit larger LNOx per flash in the midlatitudes than in the tropics. In particular, it is found that the ICEFLUX midlatitude LNOx per flash exhibits the largest difference with respect to its predicted tropical LNOx per flash, in agreement with available observations. When using CAM5, the ICEFLUX lightning parameterization could be considered a reliable lightning scheme (within its intrinsic uncertainties) in terms of its geographical distribution. Both ICEFLUX and cloud top height results agree with the enhancements of NO2 and O3 produced by lightning over tropical Atlantic and Africa and the weaker lightning background over the tropical Pacific reported by Martin et al. (2007) in the periods and locations (upper troposphere) where lightning is expected to dominate the trace gas observations.
Key Points
Lightning schemes based on upward ice flux (ICEFLUX) and cloud top height (CTH) exhibit the largest spatial correlations with observation
Five out of six lightning schemes tested with CAM5 exhibit larger LNOx in midlatitudes than in tropics
ICEFLUX can be considered a reliable lightning scheme when tested in CAM5
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Unique in situ measurements of CO, O3, SO2, CH4, NO, NOx, NOy, VOC, CN, and rBC were carried out with the German Deutsches Zentrum für Luft‐ und Raumfahrt (DLR)‐Falcon aircraft in the central U.S. ...thunderstorms during the Deep Convective Clouds and Chemistry experiment in summer 2012. Fresh and aged anvil outflow (9–12 km) from supercells, mesoscale convective systems, mesoscale convective complexes, and squall lines were probed over Oklahoma, Texas, Colorado, and Kansas. For three case studies (30 May and 8 and 12 June) a combination of trace species, radar, lightning, and satellite information, as well as model results, were used to analyze and design schematics of major trace gas transport pathways within and in the vicinity of the probed thunderstorms. The impact of thunderstorms on the O3 composition in the upper troposphere/lower stratosphere (LS) region was analyzed. Overshooting cloud tops injected high amounts of biomass burning and lightning‐produced NOx emissions into the LS, in addition to low O3 mixing ratios from the lower troposphere. As a dynamical response, O3‐rich air from the LS was transported downward into the anvil and also surrounded the outflow. The ΔO3/ΔCO ratio was determined in the anvil outflow region. A pronounced in‐mixing of O3‐rich stratospheric air masses was observed in the outflow indicated by highly positive or even negative ΔO3/ΔCO ratios (+1.4 down to −3.9). Photochemical O3 production (ΔO3/ΔCO = +0.1) was found to be minor in the recently lofted pollution plumes. O3 mixing ratios within the aged anvil outflow were mainly enhanced due to dynamical processes.
Key Points
Overshooting of the central U.S. severe thunderstorms probed in situ by aircraft
ΔO3/ΔCO ratios were determined for fresh and aged (~12–24 h) anvil outflow
O3 enhanced (~20–50 nmol mol−1) in the aged anvil outflow mainly due to dynamical processes
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
During the Deep Convective Clouds and Chemistry (DC3) experiment in summer 2012, airborne measurements were performed in the anvil inflow/outflow of thunderstorms over the Central U.S. by three ...research aircraft. A general overview of Deutsches Zentrum für Luft‐ und Raumfahrt (DLR)‐Falcon in situ measurements (CO, O3, SO2, CH4, NO, NOx, and black carbon) is presented. In addition, a joint flight on 29 May 2012 in a convective line of isolated supercell storms over Oklahoma is described based on Falcon, National Science Foundation/National Center for Atmospheric Research Gulfstream‐V (NSF/NCAR‐GV), and NASA‐DC8 trace species in situ and lidar measurements. During DC3 some of the largest and most destructive wildfires in New Mexico and Colorado state's history were burning, which strongly influenced air quality in the DC3 thunderstorm inflow and outflow region. Lofted biomass burning (BB) plumes were frequently observed in the mid‐ and upper troposphere (UT) in the vicinity of deep convection. The impact of lightning‐produced NOx (LNOx) and BB emissions was analyzed on the basis of mean vertical profiles and tracer‐tracer correlations (CO‐NOx and O3‐NO). On a regular basis DC3 thunderstorms penetrated the tropopause and injected large amounts of LNOx into the lower stratosphere (LS). Inside convection, low O3 air (~80 nmol mol−1) from the lower troposphere was rapidly transported to the UT/LS region. Simultaneously, O3‐rich stratospheric air masses (~100–200 nmol mol−1) were present around and below the thunderstorm outflow and enhanced UT‐O3 mixing ratios significantly. A 10 year global climatology of H2O data from the Aura Microwave Limb Sounder confirmed that the Central U.S. is a preferred region for convective injection into the LS.
Key Points
Severe overshooting Central U.S. thunderstorms probed in situ by three aircraft
Highly variable NOx and O3 mixing ratios in the anvil outflow region
Mixing of lightning‐produced NOx and O3‐rich stratospheric air masses
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
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