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Pickering, Kenneth E.

Publications and source records attributed to Pickering, Kenneth E..

At least 37 records · Page 2

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.

Pickering, Kenneth E.

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.

Duncan, Bryan N.

Lightning-Generated NO(x) Seen By OMI during NASA's TC-4 Experiment: First Results

We present here case studies identifying upper-tropospheric NO2 produced in convective storms during NASA's Tropical Composition, Cloud and Climate Coupling Experiment (TC~i)n July and August 2007. DC8 aircraft missions, flown from the mission base in Costa Rica, recorded in situ NO2 profiles near active storms and in relatively quiet areas. We combine these data with measurements from the Ozone Monitoring Instrument (OMI) on the Aura satellite to estimate the amount of NO2 produced by lightning (LN02) above background levels in the regions influenced by storms. In our analysis, improved off-line processing techniques are employed to minimize known artifacts in the OM1 data. Information on lightning flashes (primarily CG) observed by the surface network operated by the Instituto Costarricense de Electricidad are examined upwind of regions where OM1 indicates enhanced LNO2. Comparisons of the observed flash data with measurements by the TRMM/LIS satellite instrument are used to obtain the lightning detection efficiency for total flashes. Finally, using the NO/NO2 ratio estimated from DC-8 observations, we estimate the average NO(x) production per lightning flash for each case in this study. The magnitudes of the measured NO(x) enhancements are compared with those observed by the DC-8 and with similar OM1 measurements analyzed in mid-latitude experiments.

Bucsela, Eric

Production of NOx by Lightning and its Effects on Atmospheric Chemistry

Production of NO(x) by lightning remains the NO(x) source with the greatest uncertainty. Current estimates of the global source strength range over a factor of four (from 2 to 8 TgN/year). Ongoing efforts to reduce this uncertainty through field programs, cloud-resolved modeling, global modeling, and satellite data analysis will be described in this seminar. Representation of the lightning source in global or regional chemical transport models requires three types of information: the distribution of lightning flashes as a function of time and space, the production of NO(x) per flash, and the effective vertical distribution of the lightning-injected NO(x). Methods of specifying these items in a model will be discussed. For example, the current method of specifying flash rates in NASA's Global Modeling Initiative (GMI) chemical transport model will be discussed, as well as work underway in developing algorithms for use in the regional models CMAQ and WRF-Chem. A number of methods have been employed to estimate either production per lightning flash or the production per unit flash length. Such estimates derived from cloud-resolved chemistry simulations and from satellite NO2 retrievals will be presented as well as the methodologies employed. Cloud-resolved model output has also been used in developing vertical profiles of lightning NO(x) for use in global models. Effects of lightning NO(x) on O3 and HO(x) distributions will be illustrated regionally and globally.

Pickering, Kenneth E.

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.

Duncan, Bryan N.

Effects of Deep Convection on Atmospheric Chemistry

This presentation will trace the important research developments of the last 20+ years in defining the roles of deep convection in tropospheric chemistry. The role of deep convection in vertically redistributing trace gases was first verified through field experiments conducted in 1985. The consequences of deep convection have been noted in many other field programs conducted in subsequent years. Modeling efforts predicted that deep convection occurring over polluted continental regions would cause downstream enhancements in photochemical ozone production in the middle and upper troposphere due to the vertical redistribution of ozone precursors. Particularly large post-convective enhancements of ozone production were estimated for convection occurring over regions of pollution from biomass burning and urban areas. These estimates were verified by measurements taken downstream of biomass burning regions of South America. Models also indicate that convective transport of pristine marine boundary layer air causes decreases in ozone production rates in the upper troposphere and that convective downdrafts bring ozone into the boundary layer where it can be destroyed more rapidly. Additional consequences of deep convection are perturbation of photolysis rates, effective wet scavenging of soluble species, nucleation of new particles in convective outflow, and the potential fix stratosphere-troposphere exchange in thunderstorm anvils. The remainder of the talk will focus on production of NO by lightning, its subsequent transport within convective clouds . and its effects on downwind ozone production. Recent applications of cloud/chemistry model simulations combined with anvil NO and lightning flash observations in estimating NO Introduction per flash will be described. These cloud-resolving case-study simulations of convective transport and lightning NO production in different environments have yielded results which are directly applicable to the design of lightning parameterizations for global chemical transport models. The range of mean values (factor of 3) 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 using other methods, Results show that on a per flash basis, IC flashes are nearly as productive of NO as CG flashes. 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 of 2-9 TgN/year. 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. Simulations of the photochemistry over the 24 hours following a storm have been performed to determine the additional ozone production which can be attributed to lightning NO.

Pickering, Kenneth E.

Direct Measurements of the Convective Recycling of the Upper Troposphere

We present a statistical representation of the aggregate effects of deep convection on the chemistry and dynamics of the Upper Troposphere (UT) based on direct aircraft observations of the chemical composition of the UT over the Eastern United States and Canada during summer. These measurements provide new and unique observational constraints on the chemistry occurring downwind of convection and the rate at which air in the UT is recycled, previously only the province of model analyses. These results provide quantitative measures that can be used to evaluate global climate and chemistry models.

Bertram, Timothy H.

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.

Ott, Lesley E.

Improving Lightning NO(x) Parameterizations for Global Chemical Transport Models

Parameterization of lightning NO(x) in global chemical transport models requires a method to specify the temporal and geographic distribution of flash rates, an estimate of NO production per flash, and a method to specify the effective vertical distribution of NO production. Flash rate parameterizations using the upward convective cloud mass flux have been developed and tested for several GCM and assimilated meteorological data sets. This parameterization and others involving the cloud-top height and convective precipitation provide a generally acceptable climatological distribution of flashes after normalization with satellite data. However, considerable improvement in terms of geographic and temporal variability may be achieved in the future using cloud microphysics data available from next-generation GCMs. Cloud-resolving case-study simulations of convective transport and lightning NO production have yielded results which are directly applicable to the NO production per flash and the vertical NO distribution portions of the global model lightning parameterizations. In this work we have used cloud-resolving models (the Goddard Cumulus Ensemble Model (GCE) and MM5) 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-based lightning observations, has been used to constrain the amount of NO produced per flash. 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 in each of several case study storms. The resulting NO(x) 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. Estimates of mean NO production per flash vary by a factor of three from one simulated storm to another. 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. These profiles show a larger percentage of the total lightning NO(x) mass in the free troposphere than those suggested by Pickering et al. (1998).

Pickering, Kenneth E.

Air Quality Science and Regulatory Efforts Require Geostationary Satellite Measurements

Air quality scientists and regulatory agencies would benefit from the high spatial and temporal resolution trace gas and aerosol data that could be provided by instruments on a geostationary platform. More detailed time-resolved data from a geostationary platform could be used in tracking regional transport and in evaluating mesoscale air quality model performance in terms of photochemical evolution throughout the day. The diurnal cycle of photochemical pollutants is currently missing from the data provided by the current generation of atmospheric chemistry satellites which provide only one measurement per day. Often peak surface ozone mixing ratios are reached much earlier in the day during major regional pollution episodes than during local episodes due to downward mixing of ozone that had been transported above the boundary layer overnight. The regional air quality models often do not simulate this downward mixing well enough and underestimate surface ozone in regional episodes. Having high time-resolution geostationary data will make it possible to determine the magnitude of this lower-and mid-tropospheric transport that contributes to peak eight-hour average ozone and 24-hour average PM2.5 concentrations. We will show ozone and PM(sub 2.5) episodes from the CMAQ model and suggest ways in which geostationary satellite data would improve air quality forecasting. Current regulatory modeling is typically being performed at 12 km horizontal resolution. State and regional air quality regulators in regions with complex topography and/or land-sea breezes are anxious to move to 4-km or finer resolution simulations. Geostationary data at these or finer resolutions will be useful in evaluating such models.

Pickering, Kenneth E.

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.

Pickering, Kenneth E.

Lightning NO(x) 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-based 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 NO(x) 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 ICKG 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 of 2-9 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 HO(x), precursors leads to the generation of a HO(x), plume which substantially aids the downstream ozone production.

Pickering, Kenneth E.

Nitrogen Oxides and Ozones from B-747 Measurements (NOXAR) during POLINAT 2 and SONEX: Overview and Case-Studies on Continental and Marine Convection

In the framework of the project POLINAT 2 (Pollution in the North Atlantic Flight Corridor) we measured NO(x) (NO and NO2) and ozone on 98 flights through the North Atlantic Flight Corridor (NAFC) with a fully automated system permanently installed aboard an in-service Swissair B-747 airliner in the period of August to November 1997. The averaged NO, concentrations both in the NAFC and at the U.S. east coast were similar to that measured in autumn 1995 with the same system. The patchy occurrence of NO(x), enhancements up to 3000 pptv over several hundred kilometers (plumes), predominately found over the U.S. east coast lead to a log-normal NO(x) probability density function. In three case-studies we examine the origins of such plumes by combining back-trajectories with brightness temperature enhanced (IR) satellite imagery, with lightning observations from the U.S. National Lightning Detection Network (NLDN) or with the Optical Transient Detector (OTD) satellite. For frontal activity above the continental U.S., we demonstrate that the location of NO(x) plumes can be well explained with maps of convective influence. For another case we show that the number of lightning flashes in a cluster of marine thunderstorms is proportional to the NO(x) concentrations observed several hundred kilometers downwind of the anvil outflows and suggest that lightning was the dominant source. From the fact that in autumn the NO, maximum was found several hundred kilometers off the U.S. east coast, it can be inferred that thunderstorms triggered over the warm Gulf Stream current are an important source for the regional upper tropospheric NO(x) budget in autumn.

Jeker, Dominique

Nitrogen Oxides and Ozone from B-747 Measurements (NOXAR) During POLINAT-2 and SONEX: Overview and Case Studies on Continental and Marine Convection

In the framework of the project POLINAT 2 (Pollution in the North Atlantic Flight Corridor) we measured NO(x) (NO and NO2) and ozone on 85 flights through the North Atlantic Flight Corridor (NAFC) with a fully automated system permanently installed aboard an in-service Swissair B-747 airliner in the period of August to November 1997. The averaged NO(x) concentrations both in the NAFC and at the U.S. east coast were similar to that measured in autumn 1995 with the same system. The patchy occurrence of NO(x) enhancements up to 3000 pptv over several hundred kilometers (plumes), predominately found over the U.S. east coast lead to a log-normal NO(x) probability density function. In three case studies we examine the origins of such plumes by combining back-trajectories with brightness temperature enhanced (IR) satellite imagery, lightning observations from the U.S. National Lightning Detection Network (NLDN) and the Optical Transient Detector (OTD) satellite. We demonstrate that the location of NO(x) plumes can be well explained with maps of convective influence. We show that the number of lightning flashes in cluster of marine thunderstorms is proportional to the NO(x) concentrations observed several hundred kilometers downwind of the anvil outflows. From the fact that in autumn the NO(x) maximum was found several hundred kilometers off the U.S. east coast, it can be inferred that thunderstorms triggered over the warm Gulf Stream current are major sources for the regional upper tropospheric NO(x) budget in autumn.

Jeker, Dominique P.

Vertical transport by convective clouds: Comparisons of three modeling approaches

A preliminary comparison of the GEOS-1 (Goddard Earth Observing System) data assimilation system convective cloud mass fluxes with fluxes from a cloud-resolving model (the Goddard Cumulus Ensemble Model, GCE) is reported. A squall line case study (10-11 June 1985 Oklahoma PRESTORM episode) is the basis of the comparison. Regional (central U. S.) monthly total convective mass flux for June 1985 from GEOS-1 compares favorably with estimates from a statistical/dynamical approach using GCE simulations and satellite-derived cloud observations. The GEOS-1 convective mass fluxes produce reasonable estimates of monthly-averaged regional convective venting of CO from the boundary layer at least in an urban-influenced continental region, suggesting that they can be used in tracer transport simulations.

Pickering, Kenneth E.

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 deg - 50 deg N, 90 deg - 105 deg 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 pf 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 x 10(exp 8) kg CO/month to the free troposphere during early summer. Shallow cumulus and synoptic-scale weather systems together make a comparable contribution (total net flux 16.2 x 10(exp 8) kg CO/month). Boundary layer venting of CO with other O3 precursors leads to efficient free troposheric 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 in good agreement with estimates of O3 production from boundary layer venting in a continental-scale model (Jacob et al., 1993a, b). On this respect the central U.S. region acts as s `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.

Thompson, Anne M.

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.

Pickering, Kenneth E.

Enhancement of free tropospheric ozone production by deep convection

It is found from model simulations of trace gas and meteorological data from aircraft campaigns that deep convection may enhance the potential for photochemical ozone production in the middle and upper troposphere by up to a factor of 60. Examination of half a dozen individual convective episodes show that the degree of enhancement is highly variable. Factors affecting enhancement include boundary layer NO(x) mixing ratios, differences in the strength and structure of convective cells, as well as variation in the amount of background pollution already in the free troposphere.

Pickering, Kenneth E.