Kenneth E. Pickering

Vertical distributions of lightning NOx for use in regional and global chemical transport models

We have constructed profiles of lightning NOχ mass distribution for use in specifying the effective lightning NOχ source in global and regional chemical transport models. The profiles have been estimated for midlatitude continental, tropical continental, and tropical marine regimes based on profiles computed for individual storms in each regime. In order to construct these profiles we have developed a parameterization for lightning occurrence, lightning type, flash placement, and NOχ production in a cloud-scale tracer transport model using variables computed in the two-dimensional Goddard Cumulus Ensemble (GCE) model. Wind fields from the GCE model are used to redistribute the lightning NOχ throughout the duration of the storm. Our method produces reasonable results in terms of computed flash rates and NOχ mixing ratios compared with observations. The profiles for each storm are computed by integrating the lightning NOχ mass across the cloud model domain for each model layer at the end of the storm. The results for all three regimes show a maximum in the mass profile in the upper troposphere, usually within 2–4 km of the tropopause. Downdrafts appear to be the strongest in the simulated midlatitude continental systems, evidenced by substantial lightning NOχ mass (up to 23%) in the lowest kilometer. Tropical systems, particularly those over marine areas, tended to have a greater fraction of intracloud flashes and weaker downdrafts, causing only minor amounts of NOχ to remain in the boundary layer following a storm. Minima appear in the profiles typically in the 2–5 km layer. Even though a substantial portion of the NOχ is produced by cloud-to-ground flashes in the lowest 6 km, at the end of the storm most of the NOχ is in the upper troposphere (55–75% above 8 km) in agreement with observations. With most of the effective lightning NOχ source in the upper troposphere where the NOχ lifetime is several days, substantial photochemical O3 production is expected in this layer downstream of regions of deep convection containing lightning. We demonstrate that the effect on upper tropospheric NOχ and O3 is substantial when the vertical distribution of the lightning NOχ source in a global model is changed from uniform to being specified by our profiles. Uncertainties in a number of aspects of our parameterization are discussed.

Thunderstorms: An Important Mechanism in the Transport of Air Pollutants

Acid deposition and photochemical smog are urban air pollution problems, and they remain localized as long as the sulfur, nitrogen, and hydrocarbon pollutants are confined to the lower troposphere (below about 1-kilometer altitude) where they are short-lived. If, however, the contaminants are rapidly transported to the upper troposphere, then their atmospheric residence times grow and their range of influence expands dramatically. Although this vertical transport ameliorates some of the effects of acid rain by diluting atmospheric acids, it exacerbates global tropospheric ozone production by redistributing the necessary nitrogen catalysts. Results of recent computer simulations suggest that thunderstorms are one means of rapid vertical transport. To test this hypothesis, several research aircraft near a midwestern thunderstrom measured carbon monoxide, hydrocarbons, ozone, and reactive nitrogen compounds. Their concentrations were much greater in the outflow region of the storm, up to 11 kilometers in altitude, than in surrounding air. Trace gas measurements can thus be used to track the motion of air in and around a cloud. Thunderstorms may transform local air pollution problems into regional or global atmospheric chemistry problems.

Convective transport of biomass burning emissions over Brazil during TRACE A

A series of large mesoscale convective systems that occurred during the Brazilian phase of GTE/TRACE A (Transport and Atmospheric Chemistry near the Equator-Atlantic) provided an opportunity to observe deep convective transport of trace gases from biomass burning. This paper reports a detailed analysis of flight 6, on September 27, 1992, which sampled cloud- and biomass-burning-perturbed regions north of Brasilia. High-frequency sampling of cloud outflow at 9-12 km from the NASA DC-8 showed enhancement of CO mixing ratios typically a factor of 3 above background (200- 300 parts per billion by volume (ppbv) versus 90 ppbv) and significant increases in NOx and hydrocarbons. Clear signals of lightning-generated NO were detected; we estimate that at least 40% of NO x at the 9.5-km level and 32% at 11.3 km originated from lightning. Four types of model studies have been performed to analyze the dynamical and photochemical characteristics of the series of convective events. (1) Regional simulations for the period have been performed with the NCAR/Penn State mesoscale model (MM5), including tracer transport of carbon monoxide, initialized with observations. Middle-upper tropospheric enhancements of a factor of 3 above background are reproduced. (2) A cloud-resolving model (the Goddard cumulus ensemble (GCE) model) has been run for one representative convective cell during the September 26-27 episode. (3) Photochemical calculations (the Goddard tropospheric chemical model), initialized with trace gas observations (e.g., CO, NO x, hydrocarbons, 03) observed in cloud outflow, show appreciable 0 3 formation postconvection, initially up to 7-8 ppbv O3/d. (4) Forward trajectories from cloud outflow levels (postconvective conditions) put the ozone-producing air masses in eastern Brazil and the tropical Atlantic within 2-4 days and over the Atlantic, Africa, and the Indian Ocean in 6-8 days. Indeed, 3-4 days after the convective episode (September 30, 1992), upper tropospheric levels in the Natal ozone sounding show an average increase of -30 ppbv (3 Dobson units (DU) integrated) compared to the September 28 sounding. Our simulated net 0 3 production rates in cloud outflow are a factor of 3 or more greater than those in air undisturbed by the storms. Integrated over the 8- to 16-km cloud outflow layer, the postconvection net 0 3 production (-5-6 DU over 8 days) accounts for -25% of the excess 03 (15-25 DU) over the South Atlantic. Comparison of TRACE A Brazilian ozonesondes and the frequency of deep convection with climatology (Kirchhoff et al., this issue) suggests that the late September 1992 conditions represented an unusually active period for both convection and upper tropospheric ozone formation.

Where did tropospheric ozone over southern Africa and the tropical Atlantic come from in October 1992? Insights from TOMS, GTE TRACE A, and SAFARI 1992

The seasonal tropospheric ozone maximum in the tropical South Atlantic, first recognized from satellite observations (Fishman et al., 1986, 1991), gave rise to the IGAC/ STARE/SAFARI 1992/TRACE A campaigns (International Global Atmospheric Chemistry/South Tropical Atlantic Regional Experiment/Southern African Fire Atmospheric Research Initiative/Transport and Atmospheric Chemistry Near the Equator- Atlantic) in September and October 1992. Along with a new TOMS-based method for deriving tropospheric column ozone, we used the TRACE A/SAFARI 1992 data set to put together a regional picture of the 0 3 distribution during this period. Sondes and aircraft profiling showed a troposphere with layers of high O3 (->90 ppbv) all the way to the tropopause. These features extend in a band from 0 o to 25oS, over the SE Indian Ocean, Africa, the Atlantic, and eastern South America. A combination of trajectory and photochemical modeling (the Goddard (GSFC) isentropic trajectory and tropospheric point model, respectively) shows a strong connection between regions of high ozone and concentrated biomass burning, the latter identified using satellite-derived fire counts (Justice et al., this issue). Back trajectories from a high-O3 tropical Atlantic region (column ozone at Ascension averaged 50 Dobson units (DU)) and forward trajectories from fire- rich and convectively active areas show that the Atlantic and southern Africa are supplied with O3 and O3-forming trace gases by midlevel easterlies and/or recirculating air from Africa, with lesser contributions from South American burning and urban pollution. Limited sampling in the mixed layer over Namibia shows possible biogenic sources of NO. High-level westerlies from Brazil (following deep convective transport of ozone precursors to the upper troposphere) dominate the upper tropospheric 03 budget over Natal, Ascension, and Okaukuejo (Namibia), although most enhanced O3 (75% or more) equatorward of 10oS was from Africa. Deep convection may be responsible for the timing of the seasonal tropospheric 0 3 maximum: Natal and Ascension show a 1- to 2-month lag relative to the period of maximum burning (cf. Baldy et al., this issue; Olson et al., this issue). Photochemical model calculations constrained with TRACE A and SAFARI airborne observations of O3 and 03 precursors (NOx, CO, hydrocarbons) show robust ozone formation (up to 15 ppbv O3/d or several DU/d) in a widespread, persistent, and well-mixed layer to 4 km. Slower but still positive net 03 formation took place throughout the tropical upper troposphere (cf. Pickering et al., this issue (a); Jacob et al., this issue). Thus whether it is faster rates of 0 3 formation in source regions with higher turnover rates or slower 03 production in long-lived stable layers ubiquitous in the TRACE A region, 10-30 DU tropospheric 03 above a -25-DU background can be accounted for. In summary, the 03 maximum studied in October 1992 was caused by a coincidence of abundant 03 precursors from biomass fires, a long residence time of stable air parcels over the eastern Atlantic and southern Africa, and deep convective transport of biomass burning products, with additional NO from lightning and occasionally biogenic sources.

Heating, moisture, and water budgets of tropical and midlatitude squall lines : comparisons and sensitivity to longwave radiation

Abstract A two-dimensional, time-dependent, and nonhydrostatic numerical cloud model is used to estimate the heating (Q1, moisture (Q2), and water budgets in the convective and stratiform regions for a tropical and a midlatitude squall line (EMEX and PRE-STORM). The model is anelastic and includes a parameterized three-class ice-phase microphysical scheme and longwave radiative transfer processes. A quantitative estimate of the impact of the longwave radiative cooling on the total surface precipitation as well as on the development and structure of these two squall lines is presented. It was found that the vertical eddy moisture fluxes are a major contribution to the model-derived Q2 budgets in both squall cases. A distinct midlevel minimum in the Q2 profile for the EMEX case is due to vertical eddy transport in the convective region. On the other hand, the contribution to the Q1 budget by the cloud-scale fluxes is minor for the EMEX case. In contrast, the vertical eddy heat flux is relatively important f...

Observational Evidence of Aerosol Enhancement of Lightning Activity and Convective Invigoration

Lightning activity over the West Pacific Ocean east of the Philippines is usually much less frequent than over the nearby maritime continents. However, in 2005 the Lightning Imaging Sensor (LIS) aboard the TRMM satellite observed anomalously high lightning activity in that area. In the same year the Moderate resolution Imaging Spectroradiometer (MODIS) measured anomalously high aerosol loading. The high aerosol loading was traced to volcanic activity, and not to any factor linked to meteorology, disentangling the usual convolution between aerosols and meteorology. We show that in general lightning activity is tightly correlated with aerosol loadings at both inter-annual and biweekly time scales. We estimate that a approximately 60% increase in aerosol loading leads to more than 150% increase in lightning flashes. Aerosols increase lightning activity through modification of cloud microphysics. Cloud ice particle sizes are reduced and cloud glaciation is delayed to colder temperature when aerosol loading is increased. TRMM precipitation radar measurements indicate that anomalously high aerosol loading is associated with enhanced cloud mixed phase activity and invigorated convection over the maritime ocean. These observed associations between aerosols, cloud microphysics, morphology and lightning activity are not related to meteorological variables or ENSO events. The results have important implications for understanding the variability of lightning and resulting aerosol-chemistry interactions.

The Deep Convective Clouds and Chemistry (DC3) Field Campaign

AbstractThe Deep Convective Clouds and Chemistry (DC3) field experiment produced an exceptional dataset on thunderstorms, including their dynamical, physical, and electrical structures and their impact on the chemical composition of the troposphere. The field experiment gathered detailed information on the chemical composition of the inflow and outflow regions of midlatitude thunderstorms in northeast Colorado, west Texas to central Oklahoma, and northern Alabama. A unique aspect of the DC3 strategy was to locate and sample the convective outflow a day after active convection in order to measure the chemical transformations within the upper-tropospheric convective plume. These data are being analyzed to investigate transport and dynamics of the storms, scavenging of soluble trace gases and aerosols, production of nitrogen oxides by lightning, relationships between lightning flash rates and storm parameters, chemistry in the upper troposphere that is affected by the convection, and related source character...

Convective transport over the central United States and its role in regional CO and ozone budgets

We have constructed a regional budget for boundary layer carbon monoxide over the central United States (32.5°–50°N, 90°–105°W), emphasizing a detailed evaluation of deep convective vertical fluxes appropriate for the month of June. Deep convective venting of the boundary layer (upward) dominates other components of the CO budget, e.g., downward convective transport, loss of CO by oxidation, anthropogenic emissions, and CO produced from oxidation of methane, isoprene, and anthropogenic nonmethane hydrocarbons (NMHCs). Calculations of deep convective venting are based on the method of Pickering et al. [1992a] which uses a satellite-derived deep convective cloud climatology along with transport statistics from convective cloud model simulations of observed prototype squall line events. This study uses analyses of convective episodes in 1985 and 1989 and CO measurements taken during several midwestern field campaigns. Deep convective venting of the boundary layer over this moderately polluted region provides a net (upward minus downward) flux of 18.1×108kg CO month−1 to the free troposphere during early summer, assuming the June statistics are typical. Shallow cumulus and synoptic-scale weather systems together make a comparable contribution (total net flux 16.2×108 kg CO month−1). Boundary layer venting of CO with other O3 precursors leads to efficient free tropospheric O3 formation. We estimate that deep convective transport of CO and other precursors over the central United States in early summer leads to a gross production of 0.66–1.1 Gmol O3 d−1 in good agreement with estimates of O3 production from boundary layer venting in a continental-scale model [Jacob et al., 1993a, b]. In this respect the central U.S. region acts as a “chimney” for the country, and presumably this O3 contributes to high background levels of O3 in the eastern United States and O3 export to the North Atlantic.

A cloud‐scale model study of lightning‐generated NO x in an individual thunderstorm during STERAO‐A

Understanding lightning NOx (NO 1 NO2) production on the cloud scale is key for developing better parameterizations of lightning NOx for use in regional and global chemical transport models. This paper attempts to further the understanding of lightning NOx production on the cloud scale using a cloud model simulation of an observed thunderstorm. Objectives are (1) to infer from the model simulations and in situ measurements the relative production rates of NOx by cloud-to-ground (CG) and intracloud (IC) lightning for the storm; (2) to assess the relative contributions in the storm anvil of convective transport of NOx from the boundary layer and NOx production by lightning; and (3) to simulate the effects of the lightning-generated NOx on subsequent photochemical ozone production. We use a two-dimensional cloud model that includes a parameterized source of lightning-generated NOx to study the production and advection of NOx associated with a developing northeast Colorado thunderstorm observed on July 12, 1996, during the Stratosphere-Troposphere Experiment—Radiation, Aerosols, Ozone (STERAO-A) field campaign. Model results are compared with the sum of NO measurements taken by aircraft and photostationary state estimates of NO2 in and around the anvil of the thunderstorm. The results show that IC lightning was the dominant source of NOx in this thunderstorm. We estimate from our simulations that the NOx production per CG flash (PCG) was of the order of 200 to 500 mol flash 21 .N O x production per IC flash (PIC) appeared to be half or more of that for a CG flash, a higher ratio of P IC/PCG than is commonly assumed. The results also indicate that the majority of NOx (greater than 80%) in the anvil region of this storm resulted from lightning as opposed to transport from the boundary layer. The effect of the lightning NOx on subsequent photochemical ozone production was assessed using a column chemical model initialized with values of NOx ,O 3, and hydrocarbons taken from a horizontally averaged vertical profile through the anvil of the simulated storm. The lightning NOx increased simulated ozone production rates by a maximum of over 7 ppbv d 21 in the upper troposphere downwind of this storm.

A space‐based, high‐resolution view of notable changes in urban NOx pollution around the world (2005–2014)

Nitrogen oxides (NOx = NO + NO2) are produced during combustion processes and, thus may serve as a proxy for fossil fuel-based energy usage and coemitted greenhouse gases and other pollutants. We use high-resolution nitrogen dioxide (NO2) data from the Ozone Monitoring Instrument (OMI) to analyze changes in urban NO2 levels around the world from 2005 to 2014, finding complex heterogeneity in the changes. We discuss several potential factors that seem to determine these NOx changes. First, environmental regulations resulted in large decreases. The only large increases in the United States may be associated with three areas of intensive energy activity. Second, elevated NO2 levels were observed over many Asian, tropical, and subtropical cities that experienced rapid economic growth. Two of the largest increases occurred over recently expanded petrochemical complexes in Jamnagar (India) and Daesan (Korea). Third, pollution transport from China possibly influenced the Republic of Korea and Japan, diminishing the impact of local pollution controls. However, in China, there were large decreases over Beijing, Shanghai, and the Pearl River Delta, which were likely associated with local emission control efforts. Fourth, civil unrest and its effect on energy usage may have resulted in lower NO2 levels in Libya, Iraq, and Syria. Fifth, spatial heterogeneity within several megacities may reflect mixed efforts to cope with air quality degradation. We also show the potential of high-resolution data for identifying NOx emission sources in regions with a complex mix of sources. Intensive monitoring of the worlds tropical/subtropical megacities will remain a priority, as their populations and emissions of pollutants and greenhouse gases are expected to increase significantly.