Assessing the Parameterization of Nitric Oxide Emissions By Lightning in a Chemical Transport Model with Nitric Acid Columns from the IASI Satellite Instrument

NASA Astrophysics Data System (ADS)

Cooper, M.; Martin, R.; Wespes, C.; Coheur, P. F.; Clerbaux, C.; Murray, L. T.

2014-12-01

Nitrogen oxides (NOx ≡ NO + NO2) in the free troposphere largely control the production of ozone (O3), an important greenhouse gas and atmospheric oxidant. As HNO3 is the dominant sink of tropospheric NOx, improved understanding of its production and loss mechanisms can help to better constrain NOx emissions, and in turn improve understanding of ozone production and its effect on climate. However, this understanding is inhibited by the scarcity of direct measurements of free tropospheric HNO3, particularly in the tropics. We interpret tropical tropospheric nitric acid columns from the IASI satellite instrument with a global chemical transport model (GEOS-Chem). Overall GEOS-Chem generally agrees with IASI, however we find that the simulation underestimates IASI nitric acid over Southeast Asia by a factor of two. The bias is confirmed by comparing the GEOS-Chem simulation with additional satellite (HIRDLS, ACE-FTS) and aircraft (PEM-Tropics A and PEM-West B) observations of the middle and upper troposphere. We show that this bias can be explained by the parameterization of lightning NOx emissions, primarily from the misrepresentation of concentrated subgrid lightning NOx plumes. We tested a subgrid lightning plume parameterization and found that an additional 0.5 Tg N with an ozone production efficiency of 15 mol/mol would reduce the regional nitric acid bias from 92% to 6% without perturbing the rest of the tropics. Other sensitivity studies such as modified NOx yield per flash, increased altitude of lightning NOx emissions, or changes to convective mass flux or wet deposition of nitric acid required unrealistic changes to reduce the bias. This work demonstrates the importance of a comprehensive lightning parameterization to constraining NOx emissions.

Quantifying emissions of CO and NOx using observations from MOPITT, OMI, TES, and OSIRIS

NASA Astrophysics Data System (ADS)

Zhang, X.; Jones, D. B. A.; Keller, M.; Walker, T. W.; Jiang, Z.; Henze, D. K.; Bourassa, A. E.; Degenstein, D. A.; Rochon, Y. J.

2016-12-01

We use the GEOS-Chem four-dimensional variational (4D-var) data assimilation with satellite observations of multiple chemical species to estimate emissions of CO and NOx, as well as the tropospheric concentrations of O3. In doing so, we utilize CO retrievals from The Measurements of Pollution In The Troposphere (MOPITT), O3 retrievals from the Tropospheric Emission Spectrometer (TES), O3 retrievals from the Optical Spectrograph and InfraRed Imager System (OSIRIS), and NO2 columns from the Ozone Monitoring Instrument (OMI). By integrating these data in the 4D-Var scheme, we obtain a chemical state in the model that is consistent with all of the data over the assimilation period. In this context, for example, we find that combining TES and OSIRIS improves O3, particularly in the tropical upper troposphere (by 10-20%), which leads to a reduction in the uncertainty of the NOx emission estimates. However, although assimilating multiple chemical species provides a stronger constraint on the chemical, state, there are still large uncertainties on the CO and NOx emission estimates, due to the dependence of the results on the selection of the assimilation window and how the datasets are weighted in the cost function.

Origin and Variability of Upper Tropospheric Nitrogen Oxides and Ozone at Northern Mid-Latitudes

NASA Technical Reports Server (NTRS)

Grewe, V.; Brunner, D.; Dameris, M.; Grenfell, J. L.; Hein, R.; Shindell, D.; Staehelin, J.

1999-01-01

Measurements of NO(x) and ozone performed during the NOXAR project are compared with results from the coupled chemistry-climate models ECHAM4.L39(DLR)/CHEM and GISS-model. The measurements are based on flights between Europe and the East coast of America and between Europe and the Far East in the latitude range 40 deg N to 65 deg N. The comparison concentrates on tropopause altitudes and reveals strong longitudinal variations of seasonal mean NO,, of 200 pptv. Either model reproduced strong variations 3 km below but not at the tropopause, indicating a strong missing NO(x) or NO(y) sink over remote areas, e.g. NO(x) to HNO3 conversion by OH from additional OH sources or HNO3 wash-out. Vertical profiles show maximum NO(x) values 2-3 km below the tropopause with a strong seasonal cycle. ECHAM4.L39(DLR)/CHEM reproduces a maximum, although located at the tropopause with a less pronounced seasonal cycle, whereas the GISS model reproduces the seasonal cycle but not the profile's shape due to its coarser vertical resolution. A comparison of NO(x) frequency distributions reveals that both models are capable of reproducing the observed variability, except that ECHAM4.L39(DLR)/CHEM shows no very high NO(x) mixing ratios. Ozone mean values, vertical profiles and frequency distributions are much better reproduced in either model, indicating that the NO(x) frequency distribution, namely the most frequent NO(x) mixing ratio, is more important for the tropospheric photochemical ozone production than its mean value. Both models show that among all sources, NO(x) from lightning contributes most to the seasonal cycle of NO(x) at tropopause altitudes. The impact of lightning in the upper troposphere on NO(x) does not vary strongly with altitude, whereas the impact of surface emissions decreases with altitude. However, the models show significant differences in lightning induced NO(x) concentrations, especially in winter, which may be related to the different treatment of the lower stratospheric coupling between dynamics and chemistry.

Production of Lightning NO(x) and its Vertical Distribution Calculated from 3-D Cloud-scale Chemical Transport Model Simulations

NASA Technical Reports Server (NTRS)

Ott, Lesley; Pickering, Kenneth; Stenchikov, Georgiy; Allen, Dale; DeCaria, Alex; Ridley, Brian; Lin, Ruei-Fong; Lang, Steve; Tao, Wei-Kuo

2009-01-01

A 3-D cloud scale chemical transport model that includes a parameterized source of lightning NO(x), based on observed flash rates has been used to simulate six midlatitude and subtropical thunderstorms observed during four field projects. Production per intracloud (P(sub IC) and cloud-to-ground (P(sub CG)) flash is estimated by assuming various values of P(sub IC) and P(sub CG) for each storm and determining which production scenario yields NO(x) mixing ratios that compare most favorably with in-cloud aircraft observations. We obtain a mean P(sub CG) value of 500 moles NO (7 kg N) per flash. The results of this analysis also suggest that on average, P(sub IC) may be nearly equal to P(sub CG), which is contrary to the common assumption that intracloud flashes are significantly less productive of NO than are cloud-to-ground flashes. This study also presents vertical profiles of the mass of lightning NO(x), after convection based on 3-D cloud-scale model simulations. The results suggest that following convection, a large percentage of lightning NO(x), remains in the middle and upper troposphere where it originated, while only a small percentage is found near the surface. The results of this work differ from profiles calculated from 2-D cloud-scale model simulations with a simpler lightning parameterization that were peaked near the surface and in the upper troposphere (referred to as a "C-shaped" profile). The new model results (a backward C-shaped profile) suggest that chemical transport models that assume a C-shaped vertical profile of lightning NO(x) mass may place too much mass neat the surface and too little in the middle troposphere.

Tracking LNOx Downwind to Investigate Driving Production Physics

NASA Astrophysics Data System (ADS)

Lapierre, J. L.; Pusede, S.

2016-12-01

Emissions of nitrogen oxides (NOx) influence atmospheric oxidation chemistry and drive ozone production. In the upper troposphere, lightning production (LNOx) is believed to contribute as much as 70% of the total NOx. Therefore, accurate, process-driven constraints on LNOx are required to understand the global NOx and ozone burden. However, estimates of the amount of NOx produced per lightning flash remain highly uncertain, ranging across multiple orders of magnitude ( 10-1000 moles NOx/flash). Satellite measurements provide unique advantages to study LNOx due to their extensive spatial coverage of the Earth, but despite the mechanism by which lightning produces NOx being generally known, correlations between satellite NO2 and measured flash counts are often observed to be poor. Here, we combine NO2 measurements from the Ozone Monitoring Instrument (OMI), lightning data from the National Lightning Detection Network (NLDN), and wind data from the NCEP North American Regional Reanalysis (NARR) over a 4 year period (2012-2015) to study observed relationships between the occurrence and physical characteristics of lightning (e.g., intracloud/cloud-to-ground ratio, polarity, peak current, and multiplicity) with elevated NO2 columns. We investigate the observed spatial mismatch between high flash rates and elevated upper tropospheric NO2, highlight a number of individual storms as case studies, and describe the winds and chemistry that dislocate LNOx from storms. We then use these new constraints on LNOx to investigate the physical drivers of LNOx production rates.

On the Relationship Between Observed NLDN Lightning Strikes and Modeled Convective Precipitation Rates: Parameterization of Lightning NOx Production in CMAQ

EPA Science Inventory

In the middle and upper troposphere, lightning is the most important source of nitrogen oxides (NO X = NO + NO 2), which play an essential role in the production of ozone (O 3) and influence the oxidizing capacity of the troposphere (Murray 2016). Despite much effort in both obse...

On the Relationship between Observed NLDN Lightning ...

EPA Pesticide Factsheets

Lightning-produced nitrogen oxides (NOX=NO+NO2) in the middle and upper troposphere play an essential role in the production of ozone (O3) and influence the oxidizing capacity of the troposphere. Despite much effort in both observing and modeling lightning NOX during the past decade, considerable uncertainties still exist with the quantification of lightning NOX production and distribution in the troposphere. It is even more challenging for regional chemistry and transport models to accurately parameterize lightning NOX production and distribution in time and space. The Community Multiscale Air Quality Model (CMAQ) parameterizes the lightning NO emissions using local scaling factors adjusted by the convective precipitation rate that is predicted by the upstream meteorological model; the adjustment is based on the observed lightning strikes from the National Lightning Detection Network (NLDN). For this parameterization to be valid, the existence of an a priori reasonable relationship between the observed lightning strikes and the modeled convective precipitation rates is needed. In this study, we will present an analysis leveraged on the observed NLDN lightning strikes and CMAQ model simulations over the continental United States for a time period spanning over a decade. Based on the analysis, new parameterization scheme for lightning NOX will be proposed and the results will be evaluated. The proposed scheme will be beneficial to modeling exercises where the obs

Aerosol indirect effects on lightning in the generation of induced NOx and tropospheric ozone over an Indian urban metropolis

NASA Astrophysics Data System (ADS)

Saha, Upal; Maitra, Animesh; Talukdar, Shamitaksha; Jana, Soumyajyoti

Lightning flashes, associated with vigorous convective activity, is one of the most prominent weather phenomena in the tropical atmosphere. High aerosol loading is indirectly associated with the increase in lightning flash rates via the formation of tropospheric ozone during the pre-monsoon and monsoon over the tropics. Tropospheric ozone, an important greenhouse pollutant gas have impact on Earth’s radiation budget and play a key role in changing the atmospheric circulation patterns. Lightning-induced NOx is a primary pollutant found in photochemical smog and an important precursor for the formation of tropospheric ozone. A critical analysis is done to study the indirect effects of high aerosol loading on the formation of tropospheric ozone via lightning flashes and induced NOx formation over an urban metropolitan location Kolkata (22°32'N, 88°20'E), India during the period 2001-2012. The seasonal variation of lightning flash rates (LFR), taken from TRMM-LIS 2.5o x 2.5o gridded dataset, show that the LFR was observed to be intensified in the pre-monsoon (March-May) and high in monsoon (June-September) months over the region. Aerosol Optical Depth (AOD) at 555nm, taken from MISR 0.5o x 0.5o gridded level-3 dataset, plays an indirect effect on the increase in LFR during the pre-monsoon and monsoon months and has positive correlations between them during these periods. This is also justified from the seasonal variation of the increase in LFR due to the increase in AOD over the region during 2001-2012. The calibrated GOME and OMI/AURA satellite data analysis shows that the tropospheric ozone, formed as a result of lightning-induced NOx and due to the increased AOD at 555 nm, also increases during the pre-monsoon and monsoon months. The seasonal variation of lightning-induced tropospheric NOx, taken from SCIAMACHY observations also justified the fact that the pre-monsoon and monsoon LFR solely responsible for the generation of induced NOx over the region. The increase in lightning activity is caused by the indirect influx of aerosols, especially in the upper troposphere. This is due to the warming-effect of aerosol forcing via its effect on tropospheric ozone production. Due to the increased production of O3 by lightning-induced NOx and high aerosol loading in the pre-monsoon and monsoon months, the positive climate feedback indicates a warmer climate. As a consequence, convective activity as well as lightning flashes may increase due to this indirect effect of AOD over the region. The generation of induced NOx has a positive correlation (r = 0.723) with the LFR during 2001-2012 over Kolkata. Thus, our results have significant implications for understanding the tropospheric ozone forcing by investigating the coupled aerosol-cloud-chemistry system on the generation of lightning and lightning-induced NOx over the urban metropolis.

Nitric Acid Particles in Cold Thick Ice Clouds Observed at Global Scale: Link with Lightning, Temperature, and Upper Tropospheric Water Vapor

NASA Technical Reports Server (NTRS)

Chepfer, H.; Minnis, P.; Dubuisson, P.; Chiriaco, M.; Sun-Mack, S.; Riviere, E. D.

2007-01-01

Signatures of nitric acid particles (NAP) in cold thick ice clouds have been derived from satellite observations. Most NAP are detected in the Tropics (9 to 20% of clouds with T less than 202.5 K). Higher occurrences were found in the rare mid-latitudes very cold clouds. NAP occurrence increases as cloud temperature decreases and NAP are more numerous in January than July. Comparisons of NAP and lightning distributions show that lightning is the main source of the NOx, which forms NAP in cold clouds. Qualitative comparisons of NAP with upper tropospheric humidity distributions suggest that NAP play a role in the dehydration of the upper troposphere when the tropopause is colder than 195K.

Nitric acid particles in cold thick ice clouds observed at global scale: Link with lightning, temperature, and upper tropospheric water vapor

NASA Astrophysics Data System (ADS)

Chepfer, H.; Minnis, P.; Dubuisson, P.; Chiriaco, M.; Sun-Mack, S.; RivièRe, E. D.

2007-03-01

Signatures of nitric acid particles (NAP) in cold thick ice clouds have been derived from satellite observations. Most NAP are detected in the tropics (9 to 20% of clouds with T < 202.5 K). Higher occurrences were found in the rare midlatitudes very cold clouds. NAP occurrence increases as cloud temperature decreases, and NAP are more numerous in January than July. Comparisons of NAP and lightning distributions show that lightning seems to be the main source of the NOx, which forms NAP in cold clouds over continents. Qualitative comparisons of NAP with upper tropospheric humidity distributions suggest that NAP may play a role in the dehydration of the upper troposphere when the tropopause is colder than 195 K.

Enhancement of free tropospheric ozone production by deep convection

NASA Technical Reports Server (NTRS)

Pickering, Kenneth E.; Thompson, Anne M.; Scala, John R.; Tao, Wei-Kuo; Simpson, Joanne

1994-01-01

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.

Photochemistry and transport of tropospheric ozone and its precursors in urban and remote environments

NASA Astrophysics Data System (ADS)

Anderson, Daniel Craig

Tropospheric ozone (O3) adversely affects human health, reduces crop yields, and contributes to climate forcing. To limit these effects, the processes controlling O3 abundance as well as that of its precursor molecules must be fully characterized. Here, I examine three facets of O 3 production, both in heavily polluted and remote environments. First, using in situ observations from the DISCOVER-AQ field campaign in the Baltimore/Washington region, I evaluate the emissions of the O 3 precursors CO and NOx (NOx = NO + NO2) in the National Emissions Inventory (NEI). I find that CO/NOx emissions ratios derived from observations are 21% higher than those predicted by the NEI. Comparisons to output from the CMAQ model suggest that CO in the NEI is accurate within 15 +/- 11%, while NOx emissions are overestimated by 51-70%, likely due to errors in mobile sources. These results imply that ambient ozone concentrations will respond more efficiently to NOx controls than current models suggest. I then investigate the source of high O3 and low H2O structures in the Tropical Western Pacific (TWP). A combination of in situ observations, satellite data, and models show that the high O3 results from photochemical production in biomass burning plumes from fires in tropical Southeast Asia and Central Africa; the low relative humidity results from large-scale descent in the tropics. Because these structures have frequently been attributed to mid-latitude pollution, biomass burning in the tropics likely contributes more to the radiative forcing of climate than previously believed. Finally, I evaluate the processes controlling formaldehyde (HCHO) in the TWP. Convective transport of near surface HCHO leads to a 33% increase in upper tropospheric HCHO mixing ratios; convection also likely increases upper tropospheric CH 3OOH to ~230 pptv, enough to maintain background HCHO at ~75 pptv. The long-range transport of polluted air, with NO four times the convectively controlled background, intensifies the conversion of HO2 to OH, increasing OH by a factor of 1.4. Comparisons between the global chemistry model CAM-Chem and observations show that consistent underestimates of HCHO by CAM-Chem throughout the troposphere result from underestimates in both NO and acetaldehyde.

A Comprehensive Data Composite of NO and NOy in the Upper Troposphere and Lower Stratosphere from CARIBIC Airborne Measurements

NASA Astrophysics Data System (ADS)

Stratmann, G.; Ziereis, H.; Stock, P.; Brenninkmeijer, C. A. M.; Zahn, A.; Rauthe-Schoech, A.; Schlager, H.

2015-12-01

As a key precursor for tropospheric ozone, nitrogen oxides (NOx) play an important role in atmospheric chemistry. The NOx distribution in the upper troposphere and lower stratosphere (UTLS) is controlled by different sources and processes, such as long-range transport, uplift of emissions from the boundary layer, lightning, and air traffic emissions. The combination of comparatively short lifetime, variety of sources, and complex chemistry entails large spatial variations in the abundance of nitrogen oxides. Insufficient knowledge of the NOx background concentrations in the UTLS implicates uncertainties in the determination of the ozone production, which depends non-linear on the background NOxmixing ratios. To evaluate model simulations, a sound observational data base of nitrogen oxides in the UTLS is required. Within the framework of CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) nitrogen oxide measurements are performed regularly aboard a passenger aircraft. A total of 330 flights were conducted from May 2005 through April 2013 between Frankfurt/Germany and destinations in the USA, Canada, Brazil, Venezuela, Chile, Argentina, Colombia, South Africa, China, South Korea, Japan, India, Thailand, and the Philippines. We present data averages of NO and NOy for the different regions and for different seasons. At mid-latitudes, observed NOy and NO generally show clear seasonal cycles in the upper troposphere with a maximum in summer and a minimum in winter. Mean NOy mixing ratios vary between 1.36 nmol/mol in summer and 0.27 nmol/mol in winter. Mean NO mixing ratios range between 0.05 nmol/mol and 0.22 nmol/mol. Regions in the sub-tropics and tropics show no consistent seasonal dependence of the NO and NOyabundance. These measurements represent one of the most comprehensive NO and NOy dataset presently available for the tropopause region and is a suitable basis for establishing a climatology. It can be used for the evaluation of global chemistry-climate models.

Impact of Surface Emissions to the Zonal Variability of Tropical Tropospheric Ozone and Carbon Monoxide for November 2004

NASA Technical Reports Server (NTRS)

Bowman, K. W.; Jones, D.; Logan, J.; Worden, H.; Boersma, F.; Chang, R.; Kulawik, S.; Osterman, G.; Worden, J.

2008-01-01

The chemical and dynamical processes governing the zonal variability of tropical tropospheric ozone and carbon monoxide are investigated for November 2004 using satellite observations, in-situ measurements, and chemical transport models in conjunction with inverse-estimated surface emissions. Vertical ozone profile estimates from the Tropospheric Emission Spectrometer (TES) and ozone sonde measurements from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network show the so called zonal 'wave-one' pattern, which is characterized by peak ozone concentrations (70-80 ppb) centered over the Atlantic, as well as elevated concentrations of ozone over Indonesia and Australia (60-70 ppb) in the lower troposphere. Observational evidence from TES CO vertical profiles and Ozone Monitoring Instrument (OMI) NO2 columns point to regional surface emissions as an important contributor to the elevated ozone over Indonesia. This contribution is investigated with the GEOS-Chem chemistry and transport model using surface emission estimates derived from an optimal inverse model, which was constrained by TES and Measurements Of Pollution In The Troposphere (MOPITT) CO profiles (Jones et al., 2007). These a posteriori estimates, which were over a factor of 2 greater than climatological emissions, reduced differences between GEOS-Chem and TES ozone observations by 30-40% and led to changes in GEOS-Chem upper tropospheric ozone of up to 40% over Indonesia. The remaining residual differences can be explained in part by upper tropospheric ozone produced from lightning NOx in the South Atlantic. Furthermore, model simulations from GEOS-Chem indicate that ozone over Indonesian/Australian is more sensitive to changes in surface emissions of NOx than ozone over the tropical Atlantic.

The role of chemistry in under-predictions of NO2 in the upper troposphere

NASA Astrophysics Data System (ADS)

Henderson, B. H.; Pinder, R. W.; Goliff, W. S.; Stockwell, W. R.; Fahr, A.; Sarwar, G.; Hutzell, W. T.; Mathur, R.; Vizuete, W.; Cohen, R. C.

2009-12-01

Global and regional atmospheric models under-predict upper troposphere NO2 compared to satellite and aircraft observations. The upper tropospheric under-prediction of NO2 could be a function of emissions, transport, chemistry or some combination. Previous researchers have linked poor performance in the model to over-prediction of the OH and under-prediction of the HO2 by chemistry (Olson et al. 2006, Bertram et al. 2007). This study isolates upper tropospheric chemistry to evaluate the chemical contribution to NO2 under-predictions and to diagnose OH and HO2 discrepancies.

We use a 0-dimensional time dependent model to evaluate seven chemical mechanisms. Because chamber data representing upper tropospheric conditions does not exist, we evaluate the predictions based against an observation-based aging model. Following Bertram et al (2007), we use the NOx:HNO3 ratio to categorize the chemical age of thousands of 10 second average observations between 8 and 10km. Measurements of 10 inorganics and 32 hydrocarbons are translated to model species for each of seven chemical mechanisms. We chose mechanisms ranging from condensed to semi-explicit. The seven mechanisms' design scopes range from urban to global scale. Results include simulations from Model for OZone And Related chemical Tracers (MOZART), Carbon Bond 05 (CB05), State Air Pollution Research Center (SAPRC) 99, SAPRC 07, GEOS-Chem, Regional Atmospheric Chemical Mechanism version 2, and the LEEDS Master Chemical Mechanism.

Results from each chemical mechanism are compared to aircraft observations and to those obtained with other chemical mechanisms. Each mechanism is then further evaluated using integrated reaction rate analysis to identify sources of NO2 bias. We find that the largest contributors to the NO2 bias are over-predictions of PAN and HNO3. The formation of PAN is sensitive to the acetone photolysis rate. The conversion of NOx to HNO3 is most sensitive to hydroxyl radical concentrations. Hydroxyl radical sources and sinks have been quantified for each chemical mechanism using IRR analysis. Based on our modeling experience and results, we make recommendations for better simulating upper tropospheric photochemistry and we identify future research needs.

Bertram et al. Direct Measurements of the Convective Recycling of the Upper Troposphere. Science (2007)
Olson et al. A reevaluation of airborne HOx observations from NASA field campaigns. J Geophys Res-Atmos (2006) vol. 111 pp. D10301

Reactive nitrogen budget during the NASA SONEX Mission

NASA Astrophysics Data System (ADS)

Talbot, R. W.; Dibb, J. E.; Scheuer, E. M.; Kondo, Y.; Koike, M.; Singh, H. B.; Salas, L. B.; Fukui, Y.; Ballenthin, J. O.; Meads, R. F.; Miller, T. M.; Hunton, D. E.; Viggiano, A. A.; Blake, D. R.; Blake, N. J.; Atlas, E.; Flocke, F.; Jacob, D. J.; Jaegle, L.

The SASS Ozone and Nitrogen Oxides Experiment (SONEX) over the North Atlantic during October/November 1997 offered an excellent opportunity to examine the budget of reactive nitrogen in the upper troposphere (8-12 km altitude). The median measured total reactive nitrogen (NOy) mixing ratio was 425 parts per trillion by volume (pptv). A data set merged to the HNO3 measurement time resolution was used to calculate NOy (NOy sum) by summing the reactive nitrogen species (a combination of measured plus modeled results) and comparing it to measured NOy (NOy meas.). Comparisons were done for tropospheric air (O3 <100 parts per billion by volume (ppbv)) and stratospherically influenced air (O3 > 100 ppbv) with both showing good agreement between NOy sum and NOy meas. (slope >0.9 and r² ≈ 0.9). The total reactive nitrogen budget in the upper troposphere over the North Atlantic appears to be dominated by a mixture of NOx (NO + NO2), HNO3, and PAN. In tropospheric air median values of NOx/NOy were ≈ 0.25, HNO3/NOy ≈ 0.35 and PAN/NOy ≈ 0.17. Particulate NO3- and alkyl nitrates together composed <10% of NOy, while model estimated HNO4 averaged 12%. For the air parcels sampled during SONEX, there does not appear to be a large reservoir of unidentified NOy compounds.

Sources of Springtime Tropospheric Ozone Over North China: A Modeling Analysis of Ozonesonde and Satellite Observations

NASA Astrophysics Data System (ADS)

Liu, H.; Chan, C.; Huang, J.; Zhang, Y.; Choi, H.; Crawford, J. H.; Considine, D. B.; Zheng, X.; Oltmans, S. J.; Liu, S. C.; Zhang, L.; Liu, X.; Thouret, V.

2012-12-01

Tropospheric ozone concentrations and emissions of NOx have both increased significantly over China as a result of rapid industrialization during the past decade. These trends degrade local and regional air quality and have important effects on background tropospheric ozone and surface ozone over downwind North Pacific and North America. In-situ observations of tropospheric ozone over China are therefore essential to testing and improving our understanding of the impact of Asian anthropogenic (versus natural) emissions and various chemical, physical, and dynamical processes on both regional and global tropospheric ozone. Despite their critical importance, in-situ observations of tropospheric ozone profiles over China have been few and far between in most of the country. To investigate the ensemble of processes that control the distribution, variability, and sources of springtime tropospheric ozone over China and its surrounding regions, an intensive ozonesonde sounding campaign, called Transport of Air Pollutants and Tropospheric Ozone over China (TAPTO-China), was conducted at nine locations across China in the springs of 2004 (South China) and 2005 (North China). In this paper, we use a global 3-D model of tropospheric chemistry (GEOS-Chem) to examine the characteristics of distribution and variability and quantify various sources of tropospheric ozone over North China by analysis of intensive ozonesonde data obtained at four stations in North / Northwest China during the second phase of TAPTO-China (April-May 2005). These four stations include Xining (36.43N, 101.45E), Beijing (39.80N, 116.18E), Longfengshan (44.44N, 127.36E), and Aletai (47.73N, 88.08E). We drive GEOS-Chem with two sets of assimilated meteorological observations (GEOS-4 and GEOS-5) from the Goddard Earth Observing System (GEOS) of the NASA Global Modeling and Assimilation Office (GAMO), allowing us to examine the impacts of variability in meteorology. We show that the observed tropospheric ozone mixing ratios exhibit strong spatio-temporal variability. The model generally simulates well the ozonesonde observations but tends to underestimate ozone in the upper troposphere over Beijing and Longfengshan. We find that Asian fossil fuel emissions, stratospheric ozone, African lightning NOx emissions, as well as intercontinental transport are the main contributors to tropospheric ozone over North China in spring. While the lower-tropospheric ozone is largely influenced by Asian fossil fuel emissions (except over Aletai, Northwest China), lightning NOx emissions have a larger impact on the upper-tropospheric ozone than Asian fossil fuel emissions (except over Longfengshan, Northeast China). Model simulations suggest that the European fossil fuel emissions contribute more to the lower-tropospheric ozone over Aletai than the Asian fossil fuel emissions. We will also show that tropospheric ozone measurements by Tropospheric Emission Spectrometer (TES) aboard the NASA EOS Aura satellite can be used to study tropospheric ozone variability at Xining.

Nitrogen oxides in the global upper troposphere interpreted with cloud-sliced NO2 from the Ozone Monitoring Instrument

NASA Astrophysics Data System (ADS)

Marais, Eloise A.; Jacob, Daniel J.; Choi, Sungyeon; Joiner, Joanna; Belmonte-Rivas, Maria; Cohen, Ronald C.; Ryerson, Thomas B.; Weinheimer, Andrew J.; Volz-Thomas, Andreas

2017-04-01

Nitrogen oxides (NOx ≡ NO + NO2) are long lived in the upper troposphere (UT), and so have a large impact on ozone formation where ozone is a powerful greenhouse gas. Measurements of UT NOx are limited to summertime aircraft campaigns predominantly in North America. There are year-round NOx measurements from instruments onboard commercial aircraft, but NO2 measurements are susceptible to large interferences. Satellites provide global coverage, but traditional space-based NO2 observations only provide one piece of vertical information in the troposphere. New cloud-sliced satellite NO2 products offer additional vertical information by retrieving partial NO2 columns above clouds and further exploit differences in cloud heights to calculate UT NO2 mixing ratios. Two new cloud-sliced NO2 products from the Ozone Monitoring Instrument (OMI; 2004 launch) provide seasonal UT NO2 data centered at 350 hPa for 2005-2007 (NASA product) and 380 hPa for 2006 only (KNMI). Differences between the products include spectral fitting to obtain NO2 along the viewing path (slant column), the air mass factor calculation to convert slant columns to true vertical columns, treatment of the stratospheric NO2 component, and the choice of cloud products. The resultant NASA NO2 mixing ratios are 30% higher than KNMI NO2 and are consistent with summertime aircraft NO2 observations over North America. Comparison between NASA NO2 and the GEOS-Chem chemical transport model exposes glaring inadequacies in the model. In summer in the eastern US lightning NOx emissions are overestimated by at least a factor of 2, corroborated by comparison of GEOS-Chem and MOZAIC aircraft observations of reactive nitrogen (NOy). Too fast heterogeneous hydrolysis of dinitrogen pentoxide (N2O5) leads to an underestimate in UT NO2 in winter across the northern hemisphere. Absence of interannual variability in lightning flashes in the lightning NOx parameterization induces biases in UT NO2 in the tropics due to anomalous lightning activity linked to the El Niño Southern Oscillation. Ongoing work is to use GEOS-Chem to investigate the implications of updated representation of UT NOx on ozone.

Why do Models Overestimate Surface Ozone in the Southeastern United States?

NASA Technical Reports Server (NTRS)

Travis, Katherine R.; Jacob, Daniel J.; Fisher, Jenny A.; Kim, Patrick S.; Marais, Eloise A.; Zhu, Lei; Yu, Karen; Miller, Christopher C.; Yantosca, Robert M.; Sulprizio, Melissa P.;

Why do models overestimate surface ozone in the Southeast United States?

NASA Astrophysics Data System (ADS)

Travis, Katherine R.; Jacob, Daniel J.; Fisher, Jenny A.; Kim, Patrick S.; Marais, Eloise A.; Zhu, Lei; Yu, Karen; Miller, Christopher C.; Yantosca, Robert M.; Sulprizio, Melissa P.; Thompson, Anne M.; Wennberg, Paul O.; Crounse, John D.; St. Clair, Jason M.; Cohen, Ronald C.; Laughner, Joshua L.; Dibb, Jack E.; Hall, Samuel R.; Ullmann, Kirk; Wolfe, Glenn M.; Pollack, Illana B.; Peischl, Jeff; Neuman, Jonathan A.; Zhou, Xianliang

2016-11-01

Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NOx ≡ NO + NO2) and biogenic isoprene. Model estimates of surface ozone concentrations tend to be biased high in the region and this is of concern for designing effective emission control strategies to meet air quality standards. We use detailed chemical observations from the SEAC4RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model at 0.25° × 0.3125° horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NOx from the US Environmental Protection Agency (EPA) is too high. This finding is based on SEAC4RS observations of NOx and its oxidation products, surface network observations of nitrate wet deposition fluxes, and OMI satellite observations of tropospheric NO2 columns. Our results indicate that NEI NOx emissions from mobile and industrial sources must be reduced by 30-60 %, dependent on the assumption of the contribution by soil NOx emissions. Upper-tropospheric NO2 from lightning makes a large contribution to satellite observations of tropospheric NO2 that must be accounted for when using these data to estimate surface NOx emissions. We find that only half of isoprene oxidation proceeds by the high-NOx pathway to produce ozone; this fraction is only moderately sensitive to changes in NOx emissions because isoprene and NOx emissions are spatially segregated. GEOS-Chem with reduced NOx emissions provides an unbiased simulation of ozone observations from the aircraft and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NOx oxidation products. However, the model is still biased high by 6 ± 14 ppb relative to observed surface ozone in the Southeast US. Ozonesondes launched during midday hours show a 7 ppb ozone decrease from 1.5 km to the surface that GEOS-Chem does not capture. This bias may reflect a combination of excessive vertical mixing and net ozone production in the model boundary layer.

Why do Models Overestimate Surface Ozone in the Southeastern United States?

PubMed Central

Travis, Katherine R.; Jacob, Daniel J.; Fisher, Jenny A.; Kim, Patrick S.; Marais, Eloise A.; Zhu, Lei; Yu, Karen; Miller, Christopher C.; Yantosca, Robert M.; Sulprizio, Melissa P.; Thompson, Anne M.; Wennberg, Paul O.; Crounse, John D.; St Clair, Jason M.; Cohen, Ronald C.; Laughner, Joshua L.; Dibb, Jack E.; Hall, Samuel R.; Ullmann, Kirk; Wolfe, Glenn M.; Pollack, Illana B.; Peischl, Jeff; Neuman, Jonathan A.; Zhou, Xianliang

2018-01-01

Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NOx ≡ NO + NO2) and biogenic isoprene. Model estimates of surface ozone concentrations tend to be biased high in the region and this is of concern for designing effective emission control strategies to meet air quality standards. We use detailed chemical observations from the SEAC4RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model at 0.25°×0.3125° horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NOx from the US Environmental Protection Agency (EPA) is too high. This finding is based on SEAC4RS observations of NOx and its oxidation products, surface network observations of nitrate wet deposition fluxes, and OMI satellite observations of tropospheric NO2 columns. Our results indicate that NEI NOx emissions from mobile and industrial sources must be reduced by 30–60%, dependent on the assumption of the contribution by soil NOx emissions. Upper tropospheric NO2 from lightning makes a large contribution to satellite observations of tropospheric NO2 that must be accounted for when using these data to estimate surface NOx emissions. We find that only half of isoprene oxidation proceeds by the high-NOx pathway to produce ozone; this fraction is only moderately sensitive to changes in NOx emissions because isoprene and NOx emissions are spatially segregated. GEOS-Chem with reduced NOx emissions provides an unbiased simulation of ozone observations from the aircraft, and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NOx oxidation products. However, the model is still biased high by 8±13 ppb relative to observed surface ozone in the Southeast US. Ozonesondes launched during midday hours show a 7 ppb ozone decrease from 1.5 km to the surface that GEOS-Chem does not capture. This bias may reflect a combination of excessive vertical mixing and net ozone production in the model boundary layer. PMID:29619045

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

NASA Technical Reports Server (NTRS)

Allen, Dale; Pickering, Kenneth; Pinder, Robert; Koshak, William; Pierce, Thomas

2011-01-01

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.

Evidence of Convection as a Dominant Source of Condensation Nuclei in the Northern Midlatitude Upper Troposphere

NASA Technical Reports Server (NTRS)

Wang, Y.; Liu, S. C.; Anderson, B. E.; Kondo, Y.; Gregory, G. L.; Sachse, G. W.; Vay, S. A.; Blake, D.; Singh, H. B.; Thompson, A. M.

1999-01-01

We examine concurrent upper tropospheric measurements of CN (diameter greater than 4 nm). NO, and NO(Y) during the SONEX Experiment over the North Atlantic (Oct.-Nov., 1997). Elevated CN and NO(Y) concentrations observed in the upper troposphere are attributed largely to enhancements in convective outflows. We estimate that less than 7% of observed high-CN plumes (greater than 10000 /cc) may be attributed to aircraft emissions. Dilution of high-CN convective and aircraft plumes appears to be much more rapid than losses of NO(X) and CN by oxidation and coagulation, respectively, and accounts for much of observed CN concentrations. When taking into account of different time scales against dilution for observable aircraft and convective high-CN plumes (estimated to be 1:4), the contribution by aircraft emissions to CN concentrations is significant, about 20% of the convective source. We find no evidence that particle formation in convective plumes is limited by OH oxidation of SO2.

Evaluating Lightning-generated NOx (LNOx) Parameterization based on Cloud Top Height at Resolutions with Partially-resolved Convection for Upper Tropospheric Chemistry Studies

NASA Astrophysics Data System (ADS)

Wong, J.; Barth, M. C.; Noone, D. C.

2012-12-01

Lightning-generated nitrogen oxides (LNOx) is an important precursor to tropospheric ozone production. With a meteorological time-scale variability similar to that of the ozone chemical lifetime, it can nonlinearly perturb tropospheric ozone concentration. Coupled with upper-air circulation patterns, LNOx can accumulate in significant amount in the upper troposphere with other precursors, thus enhancing ozone production (see attached figure). While LNOx emission has been included and tuned extensively in global climate models, its inclusions in regional chemistry models are seldom tested. Here we present a study that evaluates the frequently used Price and Rind parameterization based on cloud-top height at resolutions that partially resolve deep convection using the Weather Research and Forecasting model with Chemistry (WRF-Chem) over the contiguous United States. With minor modifications, the parameterization is shown to generate integrated flash counts close to those observed. However, the modeled frequency distribution of cloud-to-ground flashes do not represent well for storms with high flash rates, bringing into question the applicability of the intra-cloud/ground partitioning (IC:CG) formulation of Price and Rind in some studies. Resolution dependency also requires attention when sub-grid cloud-tops are used instead of the originally intended grid-averaged cloud-top. LNOx passive tracers being gathered by monsoonal upper tropospheric anticyclone.

In-situ NO and NO2 profiles measured onboard passenger aircraft over Frankfurt airport in Germany

NASA Astrophysics Data System (ADS)

Berkes, Florian; Houben, Norbert; Blomel, Torben; Tappertzhofen, Marlon; Volz-Thomas, Andreas; Petzold, Andreas

2017-04-01

NOx (sum of NO and NO2) play a central role in atmospheric chemistry related to ozone and oxidation capacity (OH and NO3 radicals). The most important sources of NOx in the upper troposphere are lightning, and transport from the boundary layer (combustion processes, from biomass burning, agriculture, and industry/transport/aircraft emissions). In-situ measurements of NOx from the upper troposphere and lower stratosphere (UTLS) down to the surface are rare, but important for understanding the local photochemistry and for the assessment of the impact of aviation on the budgets of greenhouse gases such as ozone. The European Research Infrastructure IAGOS (In-service Aircraft for a Global Observing System) operates a global-scale monitoring system for atmospheric temperature, trace gases, aerosols and clouds at high spatial resolution by passenger aircraft. The IAGOS NOx instrument is designed for the autonomous measurement of nitrogen oxides over serval months. The measurement principle is based on the well-established chemiluminescence technique, using one channel with sequential measurements of NO and NOx every 50 s. Here, we present vertical profiles of nitrogen oxides from the UTLS down to the surface for day and night time conditions obtained over 12 months in 2015 and 2016. The analysis focuses mainly on Europe, the region with the largest amount of profiles. Other regions (North America, South America and East Asia) will also be discussed. Typically, NO and NO2 varies in the low ppt range in the UT, slightly increasing towards the pressure altitude of 200 hPa. Down to the surface, the values of NO and of NO2 increase up to several ppb. These profiles combined with in-situ water vapor and cloud parameters will be valuable for validation of model and of satellite data in the future.

Ozone production potential following convective redistribution of biomass burning emissions

NASA Technical Reports Server (NTRS)

Pickering, Kenneth E.; Thompson, Anne M.; Scala, John R.; Tao, Wei-Kuo; Simpson, Joanne

1992-01-01

The effects of deep convection on the potential for forming ozone in the free troposphere have been simulated for regions where the trace gas composition is influenced by biomass burning. Cloud photochemical and dynamic simulations based on observations in the 1980 and 1985 Brazilian campaigns form the basis of a sensitivity study of the ozone production potential under differing conditions. It is seen that there is considerably more ozone formed in the middle and upper troposphere when convection has redistributed hydrocarbons, NO(x), and CO compared to the example of no convection.

Lightning and Other Influences On Tropical Tropospheric Ozone: Empirical Studies of Covariation

NASA Technical Reports Server (NTRS)

Chatfield, Robert B.; Guan, Hong; Hudson, Robert D.; Witte, Jacquelyne C.

2003-01-01

Tropical and subtropical tropospheric ozone are important radiatively active species, with particularly large effects in the upper third of the troposphere. Temporal variability of O3 has proved difficult to simulate day by day in process models. Thus, individual roles of lightning, biomass burning, and other pollution in providing precursor NO(x), radicals, and chain carriers (CO, hydrocarbons) remain unquantified by simulation, and it is theoretically reasonable that individual roles are magnified by a joint synergy. We use wavelet analysis and Burg-algorithm maximum entropy spectral analyses to describe time-scales and correlation of ozone with proxies for processes controlling its concentration. Our empirical studies link time variations apparent in several datasets: the SHADOZ (Southern Hemisphere Additional Ozonesondes) network stations (Nairobi, Fiji), and auxiliary series with power to explain ozone-determining processes, with some interpretation based on the TTO (Tropical Tropospheric Ozone) product derived from TOMS (the Total Ozone Mapping Spectrometer). The auxiliary series are The OTD/LIS(Optical Transient Detector/Lightning Imaging Sensor) measurements of the lightning NO(x) source, the OLR (Outgoing Longwave Radiation)measurement of high-topped clouds, and standard meteorological variables from the United States NCEP (National Centers for Environmental Prediction) and Data Assimilation Office analyses. Concentrating on equatorial ozone, we compare the statistical evidence on the variability of tropospheric ozone. Important variations occur on approximately two-week, two-month (Madden-Julian Oscillation) and annual scales, and relations with OLR suggest controls associated with continental clouds. Hence we are now using the Lightning Imaging Sensor data set to indicate NO(x) sources. We report initial results defining relative roles of the process mentioned affecting O3 using their covariance properties.

Aircraft measurements of NO and NOy at 12 km over the Pacific Ocean

NASA Technical Reports Server (NTRS)

Koike, M.; Kondo, Y.; Makino, Y.; Sugimura, Y.

1994-01-01

Measurements of nitric oxide (NO) and total reactive nitrogen (NOy) at altitudes about 12 km were made from two aircraft missions over the central and western Pacific Ocean at latitudes between 65 deg N and 65 deg S during the International Strato-Tropospheric Air Chemistry (INSTAC) program. NO measurements were performed during the first mission in late February and early march 1990, while NOy measurements were performed during the second mission in October 1990. Lowest NO and NOy mixing ratios in the upper troposphere were observed near the equator to be about 30 to approximately 70pptv and 150 to approximately 220pptv, respectively. NOy mixing ratios in the upper troposphere were higher in the northern middle latitude than in the southern middle latitude; 300 to approximately 900pptv in 30 deg N to approximately 50 deg N and 250 to approximately 400pptv around 25 deg S and 50 deg S possibly due to the transport of the polluted air from the boundary layer and the emissions from the commercial aircraft in the northern middle latitudes. Near the equator up to 40 deg S, the NO values showed very high variability and reached between 200 and 2000 pptv. NOy(pptv)/ozone(ppbv) ratios in the upper troposphere were between about 3 and 20 and these values seem to be higher in the lower latitude except for the polluted air in the northern middle latitude. These NOy/ozone ratios in the equatorial upper troposphere are higher than those in the lower stratosphere observed by others. These features of NO and NOy in the equatorial upper troposphere suggest that NOx is produced possibly by the lightning.

Unusually high soil nitrogen oxide emissions influence air quality in a high-temperature agricultural region

PubMed Central

Oikawa, P. Y.; Ge, C.; Wang, J.; Eberwein, J. R.; Liang, L. L.; Allsman, L. A.; Grantz, D. A.; Jenerette, G. D.

2015-01-01

Fertilized soils have large potential for production of soil nitrogen oxide (NOx=NO+NO2), however these emissions are difficult to predict in high-temperature environments. Understanding these emissions may improve air quality modelling as NOx contributes to formation of tropospheric ozone (O3), a powerful air pollutant. Here we identify the environmental and management factors that regulate soil NOx emissions in a high-temperature agricultural region of California. We also investigate whether soil NOx emissions are capable of influencing regional air quality. We report some of the highest soil NOx emissions ever observed. Emissions vary nonlinearly with fertilization, temperature and soil moisture. We find that a regional air chemistry model often underestimates soil NOx emissions and NOx at the surface and in the troposphere. Adjusting the model to match NOx observations leads to elevated tropospheric O3. Our results suggest management can greatly reduce soil NOx emissions, thereby improving air quality. PMID:26556236

Estimates of the changes in tropospheric chemistry which result from human activity and their dependence on NO(x) emissions and model resolution

NASA Technical Reports Server (NTRS)

Kanakidou, Maria; Crutzen, Paul J.; Zimmermann, Peter H.

1994-01-01

As a consequence of the non-linear behavior of the chemistry of the atmosphere and because of the short lifetime of nitrogen oxides (NO(x)), two-dimensional models do not give an adequate description of the production and destruction rates of NO(x) and their effects on the distributions of the concentration of ozone and hydroxyl radical. In this study, we use a three-dimensional model to evaluate the contribution of increasing NO(x) emissions from industrial activity and biomass burning to changes in the chemical composition of the troposphere. By comparing results obtained from longitudinally-uniform and longitudinally-varying emissions of NO(x), we demonstrate that the geographical representation of the NO(x) emissions is crucial in simulating tropospheric chemistry.

On the Sources and Sinks of Atmospheric VOCs: An Integrated Analysis of Recent Aircraft Campaigns over North America

NASA Astrophysics Data System (ADS)

Chen, X.; Millet, D. B.; Singh, H. B.; Wisthaler, A.

2017-12-01

We present an integrated analysis of the atmospheric VOC budget over North America using a high-resolution GEOS-Chem simulation and observations from a large suite of recent aircraft campaigns. Here, the standard model simulation is expanded to include a more comprehensive VOC treatment encompassing the best current understanding of emissions and chemistry. Based on this updated framework, we find in the model that biogenic emission dominate VOC carbon sources over North America (accounting for 71% of total primary emissions), and this is especially the case from a reactivity perspective (with biogenic VOCs accounting for 90% of reactivity-weighted emissions). Physical processes and chemical degradation make comparable contributions to the removal of VOC carbon over North America. We further apply this simulation to explore the impacts of different primary VOC sources on atmospheric chemistry in terms of OH reactivity and key atmospheric chemicals including NOx, HCHO, glyoxal, and ozone. The airborne observations show that the majority of detected VOC carbon is carried by oxygenated VOC throughout the North American troposphere, and this tendency is well captured by the model. Model-measurement comparisons along the campaign flight tracks show that the total observed VOC abundance is generally well-predicted by the model within the boundary layer (with some regionally-specific biases) but severely underestimated in the upper troposphere. The observations imply significant missing sources in the model for upper tropospheric methanol, acetone, peroxyacetic acid, and glyoxal, and for organic acids in the lower troposphere. Elemental ratios derived from airborne high-resolution mass spectrometry show only modest change in the ensemble VOC carbon oxidation state with aging (in NOx:NOy space), and the model successfully captures this behavior.

Nitrogen oxides and ozone in the tropopause region of the Northern Hemisphere: Measurements from commercial aircraft in 1995/1996 and 1997

NASA Astrophysics Data System (ADS)

Brunner, Dominik; Staehelin, Johannes; Jeker, Dominique; Wernli, Heini; Schumann, Ulrich

2001-11-01

Measurements of nitrogen oxides (NO and NO2) and ozone (O3) were performed from a Swissair B-747 passenger aircraft in two extended time periods (May 1995 to May 1996, August to November 1997) in the framework of the Swiss NOXAR and the European POLINAT 2 project. The measurements were obtained on a total of 623 flights between Europe and destinations in the United States and the Far East. NO2 measurements were obtained only after December 1995 and were less precise than the NO measurements. Therefore daytime NO2 values were derived from measured NO and O3 concentrations assuming photostationary equilibrium. The completed NOx data set (measured NO, measured NO2 during night, and calculated NO2 during day) includes a complete annual cycle and is the most extensive and representative data set currently available for the upper troposphere (UT) and the lower stratosphere (LS) covering a significant proportion of the northern hemisphere between 15°N and 65°N. NOx concentrations in midlatitudes (30°-60°N) showed a marked seasonal variation both in the UT and the LS with a maximum in summer (median/mean values of 159/264 pptv in UT, 199/237 pptv in LS) and a minimum in winter (51/99 pptv in UT, 67/91 pptv in LS). Mean NOx concentrations were generally much higher than the respective median values, in particular in the UT, which reflects the important contribution from comparatively few very high concentrations observed in large-scale convection/lightning and small-scale aircraft plumes. Seasonal mean NOx concentrations in the UT were up to 3-4 times higher over continental regions than over the North Atlantic during summer. Lightning production of NO and convective vertical transport from the polluted boundary layer thus appear to have dominated the upper tropospheric NOx budget over these continental regions, particularly during summer. Ozone concentrations at aircraft cruising levels typically varied by an order of magnitude due to the strong vertical gradient in the LS. Seasonal mean values were dominated by large-scale dynamical processes controlling the altitude of the tropopause and the O3 abundance in the LS. O3 in the UT in midlatitudes showed a broad maximum between June and August, typical of observations in the free troposphere.

Drivers of the tropospheric ozone budget throughout the 21st century under the medium-high climate scenario RCP 6.0

NASA Astrophysics Data System (ADS)

Revell, L. E.; Tummon, F.; Stenke, A.; Sukhodolov, T.; Coulon, A.; Rozanov, E.; Garny, H.; Grewe, V.; Peter, T.

2015-01-01

Because tropospheric ozone is both a~greenhouse gas and harmful air pollutant, it is important to understand how anthropogenic activities may influence its abundance and distribution through the 21st century. Here, we present model simulations performed with the chemistry-climate model SOCOL, in which spatially disaggregated chemistry and transport tracers have been implemented in order to better understand the distribution and projected changes in tropospheric ozone. We examine the influences of ozone precursor emissions (nitrogen oxides (NOx), carbon monoxide (CO) and volatile organic compounds (VOCs)), climate change and stratospheric ozone recovery on the tropospheric ozone budget, in a~simulation following the climate scenario Representative Concentration Pathway (RCP) 6.0. Changes in ozone precursor emissions have the largest effect, leading to a global-mean increase in tropospheric ozone which maximises in the early 21st century at 23%. The increase is most pronounced at northern midlatitudes, due to regional emission patterns: between 1990 and 2060, northern midlatitude tropospheric ozone remains at constantly large abundances: 31% larger than in 1960. Over this 70 year period, attempts to reduce emissions in Europe and North America do not have an effect on zonally-averaged northern midlatitude ozone because of increasing emissions from Asia, together with the longevity of ozone in the troposphere. A~simulation with fixed anthropogenic ozone precursor emissions of NOx, CO and non-methane VOCs at 1960 conditions shows a 6 % increase in global-mean tropospheric ozone, and an 11% increase at northern midlatitudes. This increase maximises in the 2080s, and is mostly caused by methane, which maximises in the 2080s following RCP 6.0, and plays an important role in controlling ozone directly, and indirectly through its influence on other VOCs and CO. Enhanced flux of ozone from the stratosphere to the troposphere as well as climate change-induced enhancements in lightning NOx emissions also increase the tropospheric ozone burden, although their impacts are relatively small. Overall, the results show that ozone in the future is governed largely by changes in methane and NOx; methane induces an increase in tropospheric ozone that is approximately one-third of that caused by NOx. Climate impacts on ozone through changes in tropospheric temperature, humidity and lightning NOx remain secondary compared with emission strategies relating to anthropogenic emissions of NOx, such as fossil fuel burning. Therefore, emission policies globally have a critical role to play in determining tropospheric ozone evolution through the 21st century.

Top-down NOX emissions over European cities from LOTOS-EUROS simulated and OMI observed tropospheric NO2 columns using the Exponentially Modified Gaussian approach

NASA Astrophysics Data System (ADS)

Verstraeten, Willem W.; Folkert Boersma, K.; Douros, John; Williams, Jason E.; Eskes, Henk H.; Delcloo, Andy

2017-04-01

High nitrogen oxides concentrations at the surface (NOX = NO + NO2) impact humans and ecosystem badly and play a key role in tropospheric chemistry. Surface NOX emissions drive major processes in regional and global chemistry transport models (CTM). NOX contributes to the formation of acid rain, act as aerosol precursors and is an important trace gas for the formation of tropospheric ozone (O3). Via tropospheric O3, NOX indirectly affects the production of the hydroxyl radical which controls the chemical lifetime of key atmospheric pollutants and reactive greenhouse gases. High NOX emissions are mainly observed in polluted regions produced by anthropogenic combustion from industrial, traffic and household activities typically observed in large and densely populated urban areas. Accurate NOX inventories are essential, but state-of the- art emission databases may vary substantially and uncertainties are high since reported emissions factors may differ in order of magnitude and more. To date, the modelled NO2 concentrations and lifetimes have large associated uncertainties due to the highly non-linear small-scale chemistry that occurs in urban areas and uncertainties in the reaction rate data, missing nitrogen (N) species and volatile organic compounds (VOC) emissions, and incomplete knowledge of nitrogen oxides chemistry. Any overestimation in the chemical lifetime may mask missing NOX chemistry in current CTM's. By simultaneously estimating both the NO2 lifetime and concentrations, for instance by using the Exponentially Modified Gaussian (EMG), a better surface NOX emission flux estimate can be obtained. Here we evaluate if the EMG methodology can reproduce the emissions input from the tropospheric NO2 columns simulated by the LOTOS-EUROS (Long Term Ozone Simulation-European Ozone Simulation) CTM model. We apply the EMG methodology on LOTOS-EUROS simulated tropospheric NO2 columns for the period April-September 2013 for 21 selected European urban areas under windy conditions (surface wind speeds > 3 m s-1). We then compare the top-down derived surface NOX emissions with the 2011 MACC-III emission inventory, used in the LOTOS-EUROS model as input to simulate the NO2 columns. We also apply the EMG methodology on OMI (Ozone Monitoring Instrument) tropospheric NO2 column data, providing us with real-time observation-based estimates of midday NO2 lifetime and NOX emissions over 21 European cities in 2013. Results indicate that the top-down derived NOX emissions from LOTOS-EUROS (respectively OMI) are comparable with the MACC-III inventory with a R2 of 0.99 (respectively R2 = 0.79). For St-Petersburg and Moscow the top-down NOX estimates from 2013 OMI data are biased low compared to the MACC-III inventory which uses a 2011 NOX emissions update.

Characteristics of intercontinental transport of tropospheric ozone from Africa to Asia

NASA Astrophysics Data System (ADS)

Han, Han; Liu, Jane; Yuan, Huiling; Zhuang, Bingliang; Zhu, Ye; Wu, Yue; Yan, Yuhan; Ding, Aijun

2018-03-01

In this study, we characterize the transport of ozone from Africa to Asia through the analysis of the simulations of a global chemical transport model, GEOS-Chem, from 1987 to 2006. The receptor region Asia is defined within 5-60° N and 60-145° E, while the source region Africa is within 35° S-15° N and 20° W-55° E and within 15-35° N and 20° W-30° E. The ozone generated in the African troposphere from both natural and anthropogenic sources is tracked through tagged ozone simulation. Combining this with analysis of trajectory simulations using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model, we find that the upper branch of the Hadley cell connects with the subtropical westerlies in the Northern Hemisphere (NH) to form a primary transport pathway from Africa to Asia in the middle and upper troposphere throughout the year. The Somali jet that runs from eastern Africa near the equator to the Indian subcontinent in the lower troposphere is the second pathway that appears only in NH summer. The influence of African ozone mainly appears over Asia south of 40° N. The influence shows strong seasonality, varying with latitude, longitude, and altitude. In the Asian upper troposphere, imported African ozone is largest from March to May around 30° N (12-16 ppbv) and lowest during July-October around 10° N ( ˜ 2 ppbv). In the Asian middle and lower troposphere, imported African ozone peaks in NH winter between 20 and 25° N. Over 5-40° N, the mean fractional contribution of imported African ozone to the overall ozone concentrations in Asia is largest during NH winter in the middle troposphere ( ˜ 18 %) and lowest in NH summer throughout the tropospheric column ( ˜ 6 %). This seasonality mainly results from the collective effects of the ozone precursor emissions in Africa and meteorology and chemistry in Africa, in Asia and along the transport pathways. The seasonal swing of the Hadley circulation and subtropical westerlies along the primary transport pathway plays a dominant role in modulating the seasonality. There is more imported African ozone in the Asian upper troposphere in NH spring than in winter. This is likely due to more ozone in the NH African upper troposphere generated from biogenic and lightning NOx emissions in NH spring. The influence of African ozone on Asia appears larger in NH spring than in autumn. This can be attributed to both higher altitudes of the elevated ozone in Africa and stronger subtropical westerlies in NH spring. In NH summer, African ozone hardly reaches Asia because of the blocking by the Saharan High, Arabian High, and Tibetan High on the transport pathway in the middle and upper troposphere, in addition to the northward swing of the subtropical westerlies. The seasonal swings of the intertropical convergence zone (ITCZ) in Africa, coinciding with the geographic variations of the ozone precursor emissions, can further modulate the seasonality of the transport of African ozone, owing to the functions of the ITCZ in enhancing lightning NOx generation and uplifting ozone and ozone precursors to upper layers. The strength of the ITCZ in Africa is also found to be positively correlated with the interannual variation of the transport of African ozone to Asia in NH winter. Ozone from NH Africa makes up over 80 % of the total imported African ozone over Asia in most altitudes and seasons. The interhemispheric transport of ozone from southern hemispheric Africa (SHAF) is most evident in NH winter over the Asian upper troposphere and in NH summer over the Asian lower troposphere. The former case is associated with the primary transport pathway in NH winter, while the latter case is associated with the second transport pathway. The intensities of the ITCZ in Africa and the Somali jet can each explain ˜ 30 % of the interannual variations in the transport of ozone from SHAF to Asia in the two cases.

Top-down NOX Emissions of European Cities Derived from Modelled and Spaceborne Tropospheric NO2 Columns

NASA Astrophysics Data System (ADS)

Verstraeten, W. W.; Boersma, K. F.; Douros, J.; Williams, J. E.; Eskes, H.; Delcloo, A. W.

2017-12-01

High nitrogen oxides (NOX = NO + NO2) concentrations near the surface impact humans and ecosystems badly and play a key role in tropospheric chemistry. NO2 is an important precursor of tropospheric ozone (O3) which in turn affects the production of the hydroxyl radical controlling the chemical lifetime of key atmospheric pollutants and reactive greenhouse gases. Combustion from industrial, traffic and household activities in large and densely populated urban areas result in high NOX emissions. Accurate mapping of these emissions is essential but hard to do since reported emissions factors may differ from real-time emissions in order of magnitude. Modelled NO2 levels and lifetimes also have large associated uncertainties and overestimation in the chemical lifetime which may mask missing NOX chemistry in current chemistry transport models (CTM's). The simultaneously estimation of both the NO2 lifetime and as well as the concentrations by applying the Exponentially Modified Gaussian (EMG) method on tropospheric NO2 columns lines densities should improve the surface NOX emission estimates. Here we evaluate if the EMG methodology applied on the tropospheric NO2 columns simulated by the LOTOS-EUROS (Long Term Ozone Simulation-European Ozone Simulation) CTM can reproduce the NOX emissions used as model input. First we process both the modelled tropospheric NO2 columns for the period April-September 2013 for 21 selected European urban areas under windy conditions (averaged vertical wind speeds between surface and 500 m from ECMWF > 2 m s-1) as well as the accompanying OMI (Ozone Monitoring Instrument) data providing us with real-time observation-based estimates of midday NO2 columns. Then we compare the top-down derived surface NOX emissions with the 2011 MACC-III emission inventory, used in the CTM as input to simulate the NO2 columns. For cities where NOX emissions can be assumed as originating from one large source good agreement is found between the top-down derived NOX emissions from CTM and OMI with the MACC-III inventory. For cities where multiple sources of NOX are observed (e.g. Brussels, London), an adapted methodology is required. For some cities such as St-Petersburg and Moscow the top-down NOX estimates from 2013 OMI data are biased low compared to the MACC-III inventory which uses a 2011 NOX emissions update.

Chemical Characteristics of Continental Outflow Over the Tropical South Atlantic Ocean from Brazil and Africa

NASA Technical Reports Server (NTRS)

Talbot, R. W.; Bradshaw, J. D.; Sandholm, S. T.; Smyth, S.; Blake, D. R.; Blake, N. R.; Sachse, G. W.; Collins, J. E.; Heikes, B. G.; Anderson, B. E.;

Evaluation of improved operational standard tropospheric NO2 retrievals from Ozone Monitoring Instrument using in situ and surface-based NO2 observations

NASA Astrophysics Data System (ADS)

Celarier, E. A.; Lamsal, L.; Krotkov, N. A.; Bucsela, E. J.; Herman, J. R.; Dickerson, R. R.; He, H.; Brent, L. C.; Retscher, C.; Swartz, W. H.; Gleason, J. F.

2011-12-01

Nitrogen oxides are key actors in air quality and climate change. Column observations of tropospheric NO2 from the nadir-veiwing satellite sensors have been widely used to understand sources and chemistry of NOx. We have implemented several improvements to the operational algorithm developed at NASA GSFC and retrieved tropospheric NO2. Here we evaluate the new product using in situ surface measurements at the SEARCH, AQS/EPA, and NAPS networks, in situ aircraft (DISCOVER-AQ and RAMMPP), and ground-based PANDORA and DOAS measurements. The agreement among these data is within the uncertainty of measurements. The new OMI tropospheric NO2 product available at high spatial resolution is valuable to evaluate chemical transport models, to examine spatial and temporal pattern of NOx emissions, to provide top-down constraints to surface NOx emissions, and to estimate NOx lifetimes.

Drivers of the tropospheric ozone budget throughout the 21st century under the medium-high climate scenario RCP 6.0

NASA Astrophysics Data System (ADS)

Revell, L. E.; Tummon, F.; Stenke, A.; Sukhodolov, T.; Coulon, A.; Rozanov, E.; Garny, H.; Grewe, V.; Peter, T.

2015-05-01

Because tropospheric ozone is both a greenhouse gas and harmful air pollutant, it is important to understand how anthropogenic activities may influence its abundance and distribution through the 21st century. Here, we present model simulations performed with the chemistry-climate model SOCOL, in which spatially disaggregated chemistry and transport tracers have been implemented in order to better understand the distribution and projected changes in tropospheric ozone. We examine the influences of ozone precursor emissions (nitrogen oxides (NOx), carbon monoxide (CO) and volatile organic compounds (VOCs)), climate change (including methane effects) and stratospheric ozone recovery on the tropospheric ozone budget, in a simulation following the climate scenario Representative Concentration Pathway (RCP) 6.0 (a medium-high, and reasonably realistic climate scenario). Changes in ozone precursor emissions have the largest effect, leading to a global-mean increase in tropospheric ozone which maximizes in the early 21st century at 23% compared to 1960. The increase is most pronounced at northern midlatitudes, due to regional emission patterns: between 1990 and 2060, northern midlatitude tropospheric ozone remains at constantly large abundances: 31% larger than in 1960. Over this 70-year period, attempts to reduce emissions in Europe and North America do not have an effect on zonally averaged northern midlatitude ozone because of increasing emissions from Asia, together with the long lifetime of ozone in the troposphere. A simulation with fixed anthropogenic ozone precursor emissions of NOx, CO and non-methane VOCs at 1960 conditions shows a 6% increase in global-mean tropospheric ozone by the end of the 21st century, with an 11 % increase at northern midlatitudes. This increase maximizes in the 2080s and is mostly caused by methane, which maximizes in the 2080s following RCP 6.0, and plays an important role in controlling ozone directly, and indirectly through its influence on other VOCs and CO. Enhanced flux of ozone from the stratosphere to the troposphere as well as climate change-induced enhancements in lightning NOx emissions also increase the tropospheric ozone burden, although their impacts are relatively small. Overall, the results show that under this climate scenario, ozone in the future is governed largely by changes in methane and NOx; methane induces an increase in tropospheric ozone that is approximately one-third of that caused by NOx. Climate impacts on ozone through changes in tropospheric temperature, humidity and lightning NOx remain secondary compared with emission strategies relating to anthropogenic emissions of NOx, such as fossil fuel burning. Therefore, emission policies globally have a critical role to play in determining tropospheric ozone evolution through the 21st century.

A New Retrieval Algorithm for OMI NO2: Tropospheric Results and Comparisons with Measurements and Models

NASA Technical Reports Server (NTRS)

Swartz, W. H.; Bucesla, E. J.; Lamsal, L. N.; Celarier, E. A.; Krotkov, N. A.; Bhartia, P, K,; Strahan, S. E.; Gleason, J. F.; Herman, J.; Pickering, K.

2012-01-01

Nitrogen oxides (NOx =NO+NO2) are important atmospheric trace constituents that impact tropospheric air pollution chemistry and air quality. We have developed a new NASA algorithm for the retrieval of stratospheric and tropospheric NO2 vertical column densities using measurements from the nadir-viewing Ozone Monitoring Instrument (OMI) on NASA's Aura satellite. The new products rely on an improved approach to stratospheric NO2 column estimation and stratosphere-troposphere separation and a new monthly NO2 climatology based on the NASA Global Modeling Initiative chemistry-transport model. The retrieval does not rely on daily model profiles, minimizing the influence of a priori information. We evaluate the retrieved tropospheric NO2 columns using surface in situ (e.g., AQS/EPA), ground-based (e.g., DOAS), and airborne measurements (e.g., DISCOVER-AQ). The new, improved OMI tropospheric NO2 product is available at high spatial resolution for the years 200S-present. We believe that this product is valuable for the evaluation of chemistry-transport models, examining the spatial and temporal patterns of NOx emissions, constraining top-down NOx inventories, and for the estimation of NOx lifetimes.

Relationship of peroxyacetyl nitrate to active and total odd nitrogen at northern high latitudes: influence of reservoir species on NOx and O3

NASA Technical Reports Server (NTRS)

Singh, H. B.; Herlth, D.; O'Hara, D.; Zahnle, K.; Bradshaw, J. D.; Sandholm, S. T.; Talbot, R.; Crutzen, P. J.; Kanakidou, M.

1992-01-01

Measurements of peroxyacetyl nitrate (PAN), NO, NO2, HNO3, NOy (total odd nitrogen), and O3 were made in the high-latitude troposphere over North America and Greenland (35 degrees to 82 degrees N) during the Arctic Boundary Layer Expedition (ABLE 3A) (July-August 1988) throughout 0-to 6-km altitudes. These data are analyzed to quantitatively describe the relationships between various odd nitrogen species and assess their significance to global tropospheric chemistry. In the free troposphere, PAN was as much as 25 times more abundant than NOx. PAN to NOx ratio increased with increasing altitude and latitude. PAN was found to be the single most abundant reactive nitrogen species in the free troposphere and constituted a major fraction of NOy, PAN to NOy ratios were about 0.1 in the boundary layer and increased to 0.4 in the free troposphere. A 2-D global photochemical model with C1-C3 hydrocarbon chemistry is used to compare model predictions with measured results. A sizable portion (approximately 50%) of the gaseous reactive nitrogen budget is unaccounted for, and unknown organic nitrates and pernitrates are expected to be present. Model calculations (August 1, 70 degrees N) show that a major fraction of the observed NOx (50 to 70% of median) may find its source in the available PAN reservoir. PAN and the unknown reservoir species may have the potential to control virtually the entire NOx availability of the high latitude troposphere. It is predicted that the summer NOx and O3 mixing ratios in the Arctic/sub-Arctic troposphere would be considerably lower in the absence of the ubiquitous PAN reservoir. Conversely, this PAN reservoir may be responsible for the observed temporal increase in tropospheric O3 at high latitudes.

Why do Models Overestimate Surface Ozone in the Southeastern United States?

NASA Astrophysics Data System (ADS)

Travis, K.; Jacob, D.; Fisher, J. A.; Kim, S.; Marais, E. A.; Zhu, L.; Yu, K.; Miller, C. E.; Yantosca, R.; Payer Sulprizio, M.; Thompson, A. M.; Wennberg, P. O.; Crounse, J.; St Clair, J. M.; Cohen, R. C.; Laughner, J.; Dibb, J. E.; Hall, S. R.; Ullmann, K.; Wolfe, G.; Pollack, I. B.; Peischl, J.; Neuman, J. A.; Zhou, X.

2016-12-01

Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NOx = NO + NO2) and biogenic isoprene. Model estimates of surface ozone concentrations tend to be biased high in the region and this is of concern for designing effective emission control strategies to meet air quality standards. We use detailed chemical observations from the SEAC4RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model at 0.25°×0.3125° horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NO­x from the US Environmental Protection Agency (EPA) is too high in the Southeast and nationally by a factor of 2. This finding is based on SEAC4RS observations of NOx and its oxidation products, surface network observations of nitrate wet deposition fluxes, and OMI satellite observations of tropospheric NO2 columns. Upper tropospheric NO2 from lightning makes a large contribution to the satellite observations that must be accounted for when using these data to estimate surface NOx emissions. We find that only half of isoprene oxidation proceeds by the high-NOx pathway to produce ozone; this fraction is only moderately sensitive to changes in NOx emissions because isoprene and NOx emissions are spatially segregated. GEOS-Chem with reduced NOx emissions provides an unbiased simulation of ozone observations from the aircraft, and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NOx oxidation products. However, the model is still biased high by 8±13 ppb relative to observed surface ozone in the Southeast US. Ozonesondes launched during midday hours show a 7 ppb ozone decrease from 1.5 km to the surface that GEOS-Chem does not capture. This may be caused by excessively dry conditions in the model, representing another factor important in the simulation of surface ozone.

Reactive nitrogen over the tropical western Pacific: Influence from lightning and biomass burning during BIBLE A

NASA Astrophysics Data System (ADS)

Koike, M.; Kondo, Y.; Kita, K.; Nishi, N.; Liu, S. C.; Blake, D.; Ko, M.; Akutagawa, D.; Kawakami, S.; Takegawa, N.; Zhao, Y.; Ogawa, T.

2002-02-01

The Biomass Burning and Lightning Experiment phase A (BIBLE A) aircraft campaign was carried out over the tropical western Pacific in September and October 1998. During this period, biomass burning activity in Indonesia was quite weak. Mixing ratios of NOx and NOy in air masses that had crossed over the Indonesian islands within 3 days prior to the measurement (Indonesian air masses) were systematically higher than those in air masses originating from the central Pacific (tropical air masses). Sixty percent of the Indonesian air masses at 9-13 km (upper troposphere, UT) originated from the central Pacific. The differences in NOy mixing ratio between these two types of air masses were likely due to processes that occurred while air masses were over the Islands. Evidence presented in this paper suggests convection carries material from the surface, and NO is produced from lightning. At altitudes below 3 km (lower troposphere, LT), typical gradient of NOx and NOy to CO (dNOy/dCO and dNOx/dCO) was smaller than that in the biomass burning plumes and in urban areas, suggesting that neither source has a dominant influence. When the CO-NOx and CO-NOy relationships in the UT are compared to the reference relationships chosen for the LT, the NOx and NOy values are higher by 40-60 pptv (80% of NOx) and 70-100 pptv (50% of NOy). This difference is attributed to in situ production of NO by lightning. Analyses using air mass trajectories and geostationary meteorological satellite (GMS) derived cloud height data show that convection over land, which could be accompanied by lightning activity, increases the NOx values, while convection over the ocean generally lowers the NOx level. These processes are found to have a significant impact on the O3 production rate over the tropical western Pacific.

Reactive nitrogen over the tropical western Pacific: Influence from lightning and biomass burning during BIBLE A

NASA Astrophysics Data System (ADS)

Koike, M.; Kondo, Y.; Kita, K.; Nishi, N.; Liu, S. C.; Blake, D.; Ko, M.; Akutagawa, D.; Kawakami, S.; Takegawa, N.; Zhao, Y.; Ogawa, T.

2003-02-01

The Biomass Burning and Lightning Experiment phase A (BIBLE A) aircraft campaign was carried out over the tropical western Pacific in September and October 1998. During this period, biomass burning activity in Indonesia was quite weak. Mixing ratios of NOx and NOy in air masses that had crossed over the Indonesian islands within 3 days prior to the measurement (Indonesian air masses) were systematically higher than those in air masses originating from the central Pacific (tropical air masses). Sixty percent of the Indonesian air masses at 9-13 km (upper troposphere, UT) originated from the central Pacific. The differences in NOy mixing ratio between these two types of air masses were likely due to processes that occurred while air masses were over the Islands. Evidence presented in this paper suggests convection carries material from the surface, and NO is produced from lightning. At altitudes below 3 km (lower troposphere, LT), typical gradient of NOx and NOy to CO (dNOy/dCO and dNOx/dCO) was smaller than that in the biomass burning plumes and in urban areas, suggesting that neither source has a dominant influence. When the CO-NOx and CO-NOy relationships in the UT are compared to the reference relationships chosen for the LT, the NOx and NOy values are higher by 40-60 pptv (80% of NOx) and 70-100 pptv (50% of NOy). This difference is attributed to in situ production of NO by lightning. Analyses using air mass trajectories and geostationary meteorological satellite (GMS) derived cloud height data show that convection over land, which could be accompanied by lightning activity, increases the NOx values, while convection over the ocean generally lowers the NOx level. These processes are found to have a significant impact on the O3 production rate over the tropical western Pacific.

The Governing Processes and Timescales of Stratosphere-to-Troposphere Transport and its Contribution to Ozone in the Arctic Troposphere

NASA Technical Reports Server (NTRS)

Liang, Q.; Douglass, A. R.; Duncan, B. N.; Stolarski, R. S.; Witte, J. C.

2009-01-01

We used the seasonality of a combination of atmospheric trace gases and idealized tracers to examine stratosphere-to-troposphere transport and its influence on tropospheric composition in the Arctic. Maximum stratosphere-to-troposphere transport of CFCs and O3 occurs in April as driven by the Brewer-Dobson circulation. Stratosphere-troposphere exchange (STE) occurs predominantly between 40 deg N to 80 deg N with stratospheric influx in the mid-latitudes (30-70 deg N) accounting for 67.81 percent of the air of stratospheric origin in the Northern Hemisphere extratropical troposphere. Transport from the lower stratosphere to the lower troposphere (LT) takes three months on average, one month to cross the tropopause, the second month to travel from the upper troposphere (UT) to the middle troposphere (MT), and the third month to reach the LT. During downward transport, the seasonality of a trace gas can be greatly impacted by wet removal and chemistry. A comparison of idealized tracers with varying lifetimes suggests that when initialized with the same concentrations and seasonal cycles at the tropopause, trace gases that have shorter lifetimes display lower concentrations, smaller amplitudes, and earlier seasonal maxima during transport to the LT. STE contributes to O3 in the Arctic troposphere directly from the transport of O3 and indirectly from the transport of NOy . Direct transport of O3 from the stratosphere accounts for 78 percent of O3 in the Arctic UT with maximum contributions occurring from March to May. The stratospheric contribution decreases significantly in the MT/LT (20.25 percent of total O3) and shows a very weak March.April maximum. Our NOx budget analysis in the Arctic UT shows that during spring and summer, the stratospheric injection of NO y-rich air increases NOx concentrations above the 20 pptv threshold level, thereby shifting the Arctic UT from a regime of net photochemical ozone loss to one of net production with rates as high as +16 ppbv/month.

Interpretation of TOMS Observations of Tropical Tropospheric Ozone with a Global Model and In Situ Observations

NASA Technical Reports Server (NTRS)

Martin, Randall V.; Jacob, Daniel J.; Logan, Jennifer A.; Bey, Isabelle; Yantosca, Robert M.; Staudt, Amanda C.; Fiore, Arlene M.; Duncan, Bryan N.; Liu, Hongyu; Ginoux, Paul

2004-01-01

We interpret the distribution of tropical tropospheric ozone columns (TTOCs) from the Total Ozone Mapping Spectrometer (TOMS) by using a global three-dimensional model of tropospheric chemistry (GEOS-CHEM) and additional information from in situ observations. The GEOS-CHEM TTOCs capture 44% of the variance of monthly mean TOMS TTOCs from the convective cloud differential method (CCD) with no global bias. Major discrepancies are found over northern Africa and south Asia where the TOMS TTOCs do not capture the seasonal enhancements from biomass burning found in the model and in aircraft observations. A characteristic feature of these northern topical enhancements, in contrast to southern tropical enhancements, is that they are driven by the lower troposphere where the sensitivity of TOMS is poor due to Rayleigh scattering. We develop an efficiency correction to the TOMS retrieval algorithm that accounts for the variability of ozone in the lower troposphere. This efficiency correction increases TTOC's over biomass burning regions by 3-5 Dobson units (DU) and decreases them by 2-5 DU over oceanic regions, improving the agreement between CCD TTOCs and in situ observations. Applying the correction to CCD TTOCs reduces by approximately DU the magnitude of the "tropical Atlantic paradox" [Thompson et al, 2000], i.e. the presence of a TTOC enhancement over the southern tropical Atlantic during the northern African biomass burning season in December-February. We reproduce the remainder of the paradox in the model and explain it by the combination of upper tropospheric ozone production from lightning NOx, peristent subsidence over the southern tropical Atlantic as part of the Walker circulation, and cross-equatorial transport of upper tropospheric ozone from northern midlatitudes in the African "westerly duct." These processes in the model can also account for the observed 13-17 DU persistent wave-1 pattern in TTOCs with a maximum above the tropical Atlantic and a minimum over the tropical Pacific during all seasons. The photochemical effects of mineral dust have only a minor role on the modeled distribution of TTOCs, including over northern Africa, due to multiple competing effects. The photochemical effects of mineral dust globally decease annual mean OH concentrations by 9%. A global lightning NOx source of 6 Tg N yr(sup -1) in the model produces a simulation that is most consistent with TOMS and in situ observations.

Influence of the North American monsoon on Southern California tropospheric ozone levels during summer in 2013 and 2014

NASA Astrophysics Data System (ADS)

Granados-Muñoz, Maria Jose; Johnson, Matthew S.; Leblanc, Thierry

2017-06-01

The impact of the North American (NA) monsoon on tropospheric ozone variability in Southern California is investigated using lidar measurements at Jet Propulsion Laboratory-Table Mountain Facility, California, and the chemical-transport model GEOS-Chem. Routine lidar observations obtained in July-August 2013-2014 reveal a consistent ozone enhancement of 23 ppbv in the free troposphere (6-9 km), when ozone-rich air is transported along the western edge of the upper level anticyclone associated with the NA monsoon from regions where maximum lightning-induced NOx production occurs. When the high-pressure system shifts to the southeast, a zonal westerly flow of the air parcels reaching the Table Mountain Facility (TMF) occurs, prohibiting the lightning-induced ozone enhanced air to reach TMF. This modulation of tropospheric ozone by the position of the NA monsoon anticyclone could have implications on long-term ozone trends associated with our changing climate, due to the expected widening of the tropical belt affecting the strength and position of the anticyclone.

Application of satellite observations for timely updates to global anthropogenic NOx emission inventories

NASA Astrophysics Data System (ADS)

Lamsal, L. N.; Martin, R. V.; Padmanabhan, A.; van Donkelaar, A.; Zhang, Q.; Sioris, C. E.; Chance, K.; Kurosu, T. P.; Newchurch, M. J.

2011-03-01

Anthropogenic emissions of nitrogen oxides (NOx) can change rapidly due to economic growth or control measures. Bottom-up emissions estimated using source-specific emission factors and activity statistics require years to compile and can become quickly outdated. We present a method to use satellite observations of tropospheric NO2 columns to estimate changes in NOx emissions. We use tropospheric NO2 columns retrieved from the SCIAMACHY satellite instrument for 2003-2009, the response of tropospheric NO2 columns to changes in NOx emissions determined from a global chemical transport model (GEOS-Chem), and the bottom-up anthropogenic NOx emissions for 2006 to hindcast and forecast the inventories. We evaluate our approach by comparing bottom-up and hindcast emissions for 2003. The two inventories agree within 6.0% globally and within 8.9% at the regional scale with consistent trends in western Europe, North America, and East Asia. We go on to forecast emissions for 2009. During 2006-2009, anthropogenic NOx emissions over land increase by 9.2% globally and by 18.8% from East Asia. North American emissions decrease by 5.7%.

Source attribution of tropospheric ozone

NASA Astrophysics Data System (ADS)

Butler, T. M.

2015-12-01

Tropospheric ozone is a harmful pollutant with adverse effects on human health and ecosystems. As well as these effects, tropospheric ozone is also a powerful greenhouse gas, with an anthropogenic radiative forcing one quarter of that of CO2. Along with methane and atmospheric aerosol, tropospheric ozone belongs to the so-called Short Lived Climate forcing Pollutants, or SLCP. Recent work has shown that efforts to reduce concentrations of SLCP in the atmosphere have the potential to slow the rate of near-term climate change, while simultaneously improving public health and reducing crop losses. Unlike many other SLCP, tropospehric ozone is not directly emitted, but is instead influenced by two distinct sources: transport of air from the ozone-rich stratosphere; and photochemical production in the troposphere from the emitted precursors NOx (oxides of nitrogen), CO (Carbon Monoxide), and VOC (volatile organic compounds, including methane). Better understanding of the relationship between ozone production and the emissions of its precursors is essential for the development of targeted emission reduction strategies. Several modeling methods have been employed to relate the production of tropospheric ozone to emissions of its precursors; emissions perturbation, tagging, and adjoint sensitivity methods all deliver complementary information about modelled ozone production. Most studies using tagging methods have focused on attribution of tropospheric ozone production to emissions of NOx, even though perturbation methods have suggested that tropospheric ozone is also sensitive to VOC, particularly methane. In this study we describe the implementation into a global chemistry-climate model of a scheme for tagging emissions of NOx and VOC with an arbitrary number of labels, which are followed through the chemical reactions of tropospheric ozone production in order to perform attribution of tropospehric ozone to its emitted precursors. Attribution is performed to both geographical regions and to emission sectors. Source-receptor relationships are defined for intercontinental transport of ozone and its precursors, and the relative contributions of NOx, methane, CO, NMVOC, and stratosphere-troposphere exchange to tropospheric background ozone are determined.

Decreasing Lower Tropospheric Ozone over the North China Plain Observed by IASI: Looking for Explanations

NASA Astrophysics Data System (ADS)

Dufour, G.; Eremenko, M.; Lachâtre, M.; Hauglustaine, D.; Fortems-Cheiney, A.; Cuesta, J.; Zhang, Y.; Cai, Z.; Liu, Y.; Xu, X.; Lin, W.; Cooper, O. R.

2017-12-01

China, and especially the North China Plain (NCP), is a highly polluted region. Emission reductions have been applied since about 10 years, starting with SO2 emissions in 2006 and with NOx emissions in 2010. Recent satellite observations series show a decrease of NO2 tropospheric columns since 2013 and attributed to the NOx emissions reduction. The question of the impact of such reduction on ozone is then arising. In this study, we use the capabilities of the IASI satellite instrument to retrieve 2 semi-independent columns of ozone in the lower (surface-6km asl) and the upper (6-12km) troposphere - the lower tropospheric (LT) column having a sensitivity maximum at 3-4 km - and we evaluate the variability and trend of LT ozone over the NCP for 2008-2016. Deseasonalized monthly timeseries show two distinct periods: a first period (2008-2012) with no significant trend (slope of the linear fit < -0.1 %/yr) and a second period (2013-2016) with a highly significant negative trend of -1.2 %/yr, leading to an overall trend of -0.77 %/yr for 2008-2016. A first temptation is to attribute this decrease to the NOx emissions changes. However, negative trends have not been reported from background surface measurements in this Chinese region. Furthermore recent work made within the framework of the TOAR initiative reveals discrepancies in the sign of the trends of tropospheric column ozone derived from infrared and ultraviolet satellite instruments. As yet there is no conclusive explanation for the discrepancy. We then investigate the IASI retrieval stability and robustness in terms of vertical sensitivity, interferences with large aerosol loading, and comparing with surface and ozonesonde measurements and the IASI instrument aboard the Metop-B satellite. One issue arises concerning the temporal sampling of IASI that may induce significant change in the trend derived from surface stations. We also explore the possible variables, other than emissions, which could explain the observed negative trends using both a statistical regression model and simulations from global and regional chemistry transport models.

Convective transport of biomass burning emissions over Brazil during TRACE A

NASA Astrophysics Data System (ADS)

Pickering, Kenneth E.; Thompson, Anne M.; Wang, Yansen; Tao, Wei-Kuo; McNamara, Donna P.; Kirchhoff, Volker W. J. H.; Heikes, Brian G.; Sachse, Glen W.; Bradshaw, John D.; Gregory, Gerald L.; Blake, Donald R.

1996-10-01

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 NOx 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, NOx, hydrocarbons, O3) observed in cloud outflow, show appreciable O3 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 O3 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 O3 production (˜5-6 DU over 8 days) accounts for ˜25% of the excess O3 (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.

The gradient of meteorological and chemical variables across the tropopause

NASA Technical Reports Server (NTRS)

Dickerson, Russell R.; Doddridge, Bruce G.; Poulida, Olga; Owens, Melody A.

1994-01-01

The downward transport of air through the tropopause can bring substantial amounts of ozone and reactive nitrogen into the upper troposphere. In this cold region of the atmosphere, O3 is particularly effective as a greenhouse gas. As part of the North Dakota Thunderstorm Project in June 1989, the NCAR Sabreliner made five flights through the tropopause. We measured ozone, nitric oxide (NO), total reactive nitrogen (NO(y)), carbon monoxide (CO), and water vapor (H2)), and took grab samples for hydrocarbon (HC) analysis. Hydrocarbons, CO, and H2O, species with sources primarily at the earth's surface, showed a strong concentration decrease with increasing altitude, while O3 and NO(y), species with a source in the stratosphere, showed a strong concentration increase with increasing altitude. Stratospheric concentrations of NO(x), NO(y), and H2O were all high relative to winter observations made during NASA's AASE. We suggest that midlatitude thunderstorms may inject wet, NO-rich air into the lower stratosphere. Calculation based on measured ratios of NO(x) and NO(y) to O3 yield a total flux of reactive nitrogen from the Northern Hemisphere stratosphere into the troposphere of 1 to 2 Tg(N) yr(exp -1) with about 8 percent in the form of NO(x). This value is higher than reported estimates of total stratospheric nitrogen fixation.

Tropospheric Trace Gas Interactions with Aerosols

NASA Technical Reports Server (NTRS)

Penner, Joyce E.; Maddrea, George L., Jr. (Technical Monitor)

2002-01-01

Tropospheric aerosols are of considerable environmental importance. They modify the radiative budget of Earth by scattering and absorbing radiation, and by providing nuclei for cloud formation. Additionally, they provide surfaces for heterogeneous and multiphase reactions that affect tropospheric chemistry. For example, Dentener and Crutzen (1993) showed that reactions of N2O5 and NO3 with sulfate aerosols may significantly alter the tropospheric concentrations of NO(x), O3, and OH by converting NOx to HNO3 which is rapidly removed by precipitation. Zhang et al. (1994) assumed these same reactions would occur on dust aerosols and showed that dust outbreaks may reduce NO(x) levels by up to 50%. Dentener et al. (1996) studied the possible effect of reactions on dust on sulfate, nitrate, and O3 concentration. Heterogeneous and multiphase reactions on aerosols may also perturb the sulfur cycle the chlorine cycle and the bromine cycle. Because these reactions can release free chlorine and free bromine they might lead to the destruction of ozone in the marine boundary layer that may be important to include in models of tropospheric chemistry. The goal of our proposed work is to examine the role of heterogeneous and multiphase reactions in the tropospheric cycles of reactive nitrogen and sulfur.

Free tropospheric ozone production following entrainment of urban plumes into deep convection

NASA Technical Reports Server (NTRS)

Pickering, Kenneth E.; Thompson, Anne M.; Scala, John R.; Tao, Wei-Kuo; Dickerson, Russell R.; Simpson, Joanne

1992-01-01

It is shown that rapid vertical transport of air from urban plumes through deep convective clouds can cause substantial enhancement of the rate of O3 production in the free troposphere. Simulation of convective redistribution and subsequent photochemistry of an urban plume from Oklahoma City during the 1985 PRESTORM campaign shows enhancement of O3 production in the free tropospheric cloud outflow layer by a factor of almost 4. In contrast, simulation of convective transport of an urban plume from Manaus, Brazil, into a prestine free troposphere during GTE/ABLE 2B (1987), followed by a photochemical simulation, showed enhancement of O3 production by a factor of 35. The reasons for the different enhancements are (1) intensity of cloud vertical motion; (2) initial boundary layer O3 precursor concentrations; and (3) initial amount of background free tropospheric NO(x). Convective transport of ozone precursors to the middle and upper troposphere allows the resulting O3 to spread over large geographic regions, rather than being confined to the lower troposphere where loss processes are much more rapid. Conversely, as air with lower NO descends and replaces more polluted air, there is greater O3 production efficiency per molecule of NO in the boundary layer following convective transport. As a result, over 30 percent more ozone could be produced in the entire tropospheric column in the first 24 hours following convective transport of urban plumes.

The high-resolution version of TM5-MP for optimized satellite retrievals: description and validation

NASA Astrophysics Data System (ADS)

Williams, Jason E.; Folkert Boersma, K.; Le Sager, Phillipe; Verstraeten, Willem W.

2017-02-01

We provide a comprehensive description of the high-resolution version of the TM5-MP global chemistry transport model, which is to be employed for deriving highly resolved vertical profiles of nitrogen dioxide (NO2), formaldehyde (CH2O), and sulfur dioxide (SO2) for use in satellite retrievals from platforms such as the Ozone Monitoring Instrument (OMI) and the Sentinel-5 Precursor, and the TROPOspheric Monitoring Instrument (tropOMI). Comparing simulations conducted at horizontal resolutions of 3° × 2° and 1° × 1° reveals differences of ±20 % exist in the global seasonal distribution of 222Rn, being larger near specific coastal locations and tropical oceans. For tropospheric ozone (O3), analysis of the chemical budget terms shows that the impact on globally integrated photolysis rates is rather low, in spite of the higher spatial variability of meteorological data fields from ERA-Interim at 1° × 1°. Surface concentrations of O3 in high-NOx regions decrease between 5 and 10 % at 1° × 1° due to a reduction in NOx recycling terms and an increase in the associated titration term of O3 by NO. At 1° × 1°, the net global stratosphere-troposphere exchange of O3 decreases by ˜ 7 %, with an associated shift in the hemispheric gradient. By comparing NO, NO2, HNO3 and peroxy-acetyl-nitrate (PAN) profiles against measurement composites, we show that TM5-MP captures the vertical distribution of NOx and long-lived NOx reservoirs at background locations, again with modest changes at 1° × 1°. Comparing monthly mean distributions in lightning NOx and applying ERA-Interim convective mass fluxes, we show that the vertical re-distribution of lightning NOx changes with enhanced release of NOx in the upper troposphere. We show that surface mixing ratios in both NO and NO2 are generally underestimated in both low- and high-NOx scenarios. For Europe, a negative bias exists for [NO] at the surface across the whole domain, with lower biases at 1° × 1° at only ˜ 20 % of sites. For NO2, biases are more variable, with lower (higher) biases at 1° × 1° occurring at ˜ 35 % ( ˜ 20 %) of sites, with the remainder showing little change. For CH2O, the impact of higher resolution on the chemical budget terms is rather modest, with changes of less than 5 %. The simulated vertical distribution of CH2O agrees reasonably well with measurements in pristine locations, although column-integrated values are generally underestimated relative to satellite measurements in polluted regions. For SO2, the performance at 1° × 1° is principally governed by the quality of the emission inventory, with limited improvements in the site-specific biases, with most showing no significant improvement. For the vertical column, improvements near strong source regions occur which reduce the biases in the integrated column. For remote regions missing biogenic source terms are inferred.

Response of the global climate to changes in atmospheric chemical composition due to fossil fuel burning

NASA Technical Reports Server (NTRS)

Cess, R. D.; Hameed, S.; Hogan, J. S.

1980-01-01

Tropospheric ozone and methane might increase in the future as the result of increasing anthropogenic emissions of CO, NOx and CH4 due to fossil fuel burning. Since O3 and CH4 are both greenhouse gases, increases in their concentrations could augment global warming due to larger future amounts of atmospheric CO2. To test this possible climatic impact, a zonal energy-balance climate model has been combined with a vertically-averaged tropospheric chemical model. The latter model includes all relevant chemical reactions which affect species derived from H2O, O2, CH4 and NOx. The climate model correspondingly incorporates changes in the infrared heating of the surface-troposphere system resulting from chemically induced changes in tropospheric ozone and methane. This coupled climate-chemical model indicates that global climate is sensitive to changes in emissions of CO, NOx and CH4, and that future increases in these emissions could enhance global warming due to increasing atmospheric CO2.

Variation of a Lightning NOx Indicator for National Climate Assessment

NASA Technical Reports Server (NTRS)

Koshak, William J.; McCaul, Eugene W., Jr.; Peterson, Harold S.; Vant-Hull, Brian

2014-01-01

During the past couple of years, an analysis tool was developed by the NASA Marshall Space Flight Center (MSFC) for the National Climate Assessment (NCA) program. The tool monitors and examines changes in lightning characteristics over the conterminous US (CONUS) on a continual basis. In this study, we have expanded the capability of the tool so that it can compute a new climate assessment variable that is called the Lightning NOx Indicator (LNI). Nitrogen oxides (NOx = NO + NO2) are known to indirectly influence our climate, and lightning NOx is the most important source of NOx in the upper troposphere (particularly in the tropics). The LNI is derived using Lightning Imaging Sensor (LIS) data and is computed by summing up the product of flash area x flash brightness over all flashes that occur in a particular region and period. Therefore, it is suggested that the LNI is a proxy to lightning NOx production. Specifically, larger flash areas are consistent with longer channel length and/or more energetic channels, and hence more NOx production. Brighter flashes are consistent with more energetic channels, and hence more NOx production. The location of the flash within the thundercloud and the optical scattering characteristics of the thundercloud are of course complicating factors. We analyze LIS data for the years 2003-2013 and provide geographical plots of the time-evolution of the LNI in order to determine if there are any significant changes or trends between like seasons, or from year to year.

Response of the global climate to changes in atmospheric chemical composition due to fossil fuel burning

NASA Technical Reports Server (NTRS)

Hameed, S.; Cess, R. D.; Hogan, J. S.

1980-01-01

Recent modeling of atmospheric chemical processes (Logan et al, 1978; Hameed et al, 1979) suggests that tropospheric ozone and methane might significantly increase in the future as the result of increasing anthropogenic emissions of CO, NO(x), and CH4 due to fossil fuel burning. Since O3 and CH4 are both greenhouse gases, increases in their concentrations could augment global warming due to larger future amounts of atmospheric CO2. To test the possible climatic impact of changes in tropospheric chemical composition, a zonal energy-balance climate model has been combined with a vertically averaged tropospheric chemical model. The latter model includes all relevant chemical reactions which affect species derived from H2O, O2, CH4, and NO(x). The climate model correspondingly incorporates changes in the infrared heating of the surface-troposphere system resulting from chemically induced changes in tropospheric ozone and methane. This coupled climate-chemical model indicates that global climate is sensitive to changes in emissions of CO, NO(x) and CH4, and that future increases in these emissions could augment global warming due to increasing atmospheric CO2.

NOy and O3 in the Asian Monsoon Anticyclone: Uncertainties associated with the Convection and Lightning in a Global Model

NASA Astrophysics Data System (ADS)

Pozzer, A.; Ojha, N.; Tost, H.; Joeckel, P.; Fischer, H.; Ziereis, H.; Zahn, A.; Tomsche, L.; Lelieveld, J.

2017-12-01

The impacts of Asian monsoon on the tropospheric chemistry are difficult to simulate in numerical models due to the lack of accurate emission inventories over the Asian region and the strong influence of parameterized processes such as convection and lightning. Further, the lack of observational data over the region during the monsoon period reduce drastically the capability to evaluate numerical models. Here, we combine simulations using the global EMAC (ECHAM5/MESSy2 Atmospheric Chemistry) model with the observational dataset based on the OMO campaign (July-August 2015) to study the tropospheric composition in the Asian monsoon anticyclone. The results of the simulations capture the C-shape of the CO vertical profiles, typically observed during the summer monsoon. The observed spatio-temporal variations in O3, CO, and NOy are reproduced by EMAC, with a better correlation in the upper troposphere (UT). However, the model overestimates NOy and O3 mixing ratios in the anticyclone by 25% and 35%, respectively. A series of numerical experiments showed the strong lightning emissions in the model as the source of this overestimation, with the anthropogenic NOx sources (in Asia) and global soil emissions having lower impact in the UT. A reduction of the lightning NOx emission by 50% leads to a better agreement between the model and OMO observations of NOy and O3. The uncertainties in the lightning emissions are found to considerably influence the OH distribution in the UT over India and downwind. The study reveals existing uncertainties in the estimations of monsoon impact on the tropospheric composition, and highlights the need to constrain numerical simulations with state-of-the-art observations for deriving the budget of trace species of climatic relevance.

Sulfate geoengineering impact on methane transport and lifetime: results from the Geoengineering Model Intercomparison Project (GeoMIP)

NASA Astrophysics Data System (ADS)

Visioni, Daniele; Pitari, Giovanni; Aquila, Valentina; Tilmes, Simone; Cionni, Irene; Di Genova, Glauco; Mancini, Eva

2017-09-01

Sulfate geoengineering (SG), made by sustained injection of SO2 in the tropical lower stratosphere, may impact the CH4 abundance through several photochemical mechanisms affecting tropospheric OH and hence the methane lifetime. (a) The reflection of incoming solar radiation increases the planetary albedo and cools the surface, with a tropospheric H2O decrease. (b) The tropospheric UV budget is upset by the additional aerosol scattering and stratospheric ozone changes: the net effect is meridionally not uniform, with a net decrease in the tropics, thus producing less tropospheric O(1D). (c) The extratropical downwelling motion from the lower stratosphere tends to increase the sulfate aerosol surface area density available for heterogeneous chemical reactions in the mid-to-upper troposphere, thus reducing the amount of NOx and O3 production. (d) The tropical lower stratosphere is warmed by solar and planetary radiation absorption by the aerosols. The heating rate perturbation is highly latitude dependent, producing a stronger meridional component of the Brewer-Dobson circulation. The net effect on tropospheric OH due to the enhanced stratosphere-troposphere exchange may be positive or negative depending on the net result of different superimposed species perturbations (CH4, NOy, O3, SO4) in the extratropical upper troposphere and lower stratosphere (UTLS). In addition, the atmospheric stabilization resulting from the tropospheric cooling and lower stratospheric warming favors an additional decrease of the UTLS extratropical CH4 by lowering the horizontal eddy mixing. Two climate-chemistry coupled models are used to explore the above radiative, chemical and dynamical mechanisms affecting CH4 transport and lifetime (ULAQ-CCM and GEOSCCM). The CH4 lifetime may become significantly longer (by approximately 16 %) with a sustained injection of 8 Tg-SO2 yr-1 starting in the year 2020, which implies an increase of tropospheric CH4 (200 ppbv) and a positive indirect radiative forcing of sulfate geoengineering due to CH4 changes (+0.10 W m-2 in the 2040-2049 decade and +0.15 W m-2 in the 2060-2069 decade).

SONEX airborne mission and coordinated POLINAT-2 activity: Overview and accomplishments

NASA Astrophysics Data System (ADS)

Singh, Hanwant B.; Thompson, Anne M.; Schlager, H.

The SASS (Subsonic Assessment) Ozone and NOx Experiment (SONEX) was an airborne field campaign conducted in October-November 1997 in the vicinity of the North Atlantic Flight Corridor to study the impact of aircraft emissions on NOx and ozone (O3). A fully instrumented NASA DC-8 aircraft was used as the primary SONEX platform. SONEX activities were closely coordinated with the European POLINAT-2 (Pollution from Aircraft Emissions in the North Atlantic Flight Corridor) program, which used a Falcon-20 aircraft. Both campaigns focused on the upper troposphere/“lowermost” stratosphere (UT/LS) as the region of greatest interest. Specific sampling goals were achieved with the aid of a state-of-the art modeling and meteorological support system, which allowed targeted sampling of air parcels with desired characteristics. A substantial impact of aircraft emissions on NOx, O3, and CN in the UT/LS of the study region is shown to be present. This mission provided direct support for the highly nonlinear nature of the NOx-O3 chemistry. The results are being published in Special Sections of GRL and JGR. This overview provides a context within which these publications can be understood.

Using Satellite Remote Sensing and Modelling for Insights into N02 Air Pollution and NO2 Emissions

NASA Technical Reports Server (NTRS)

Lamsal, L. N.; Martin, R. V.; Krotkov, N. A.; Bucsela, E. J.; Celarier, E. A.; vanDonkelaar, A.; Parrish, D.

2012-01-01

Nitrogen oxides (NO(x)) are key actors in air quality and climate change. Satellite remote sensing of tropospheric NO2 has developed rapidly with enhanced spatial and temporal resolution since initial observations in 1995. We have developed an improved algorithm and retrieved tropospheric NO2 columns from Ozone Monitoring Instrument. Column observations of tropospheric NO2 from the nadir-viewing satellite sensors contain large contributions from the boundary layer due to strong enhancement of NO2 in the boundary layer. We infer ground-level NO2 concentrations from the OMI satellite instrument which demonstrate significant agreement with in-situ surface measurements. We examine how NO2 columns measured by satellite, ground-level NO2 derived from satellite, and NO(x) emissions obtained from bottom-up inventories relate to world's urban population. We perform inverse modeling analysis of NO2 measurements from OMI to estimate "top-down" surface NO(x) emissions, which are used to evaluate and improve "bottom-up" emission inventories. We use NO2 column observations from OMI and the relationship between NO2 columns and NO(x) emissions from a GEOS-Chem model simulation to estimate the annual change in bottom-up NO(x) emissions. The emission updates offer an improved estimate of NO(x) that are critical to our understanding of air quality, acid deposition, and climate change.

High resolution modeling of the upper troposphere and lower stratosphere region over the Arctic - GEM-AC simulations for the future climate with and without aviation emissions.

NASA Astrophysics Data System (ADS)

Porebska, Magdalena; Struzewska, Joanna; Kaminski, Jacek W.

2016-04-01

Upper troposphere and lower stratosphere (UTLS) region is a layer around the tropopause. Perturbation of the chemical composition in the UTLS region can impact physical and dynamical processes that can lead to changes in cloudiness, precipitation, radiative forcing, stratosphere-troposphere exchange and zonal flow. The objective of this study is to investigate the potential impacts of aviation emissions on the upper troposphere and lower stratosphere. In order to assess the impact of the aviation emissions we will focus on changes in atmospheric dynamic due to changes in chemical composition in the UTLS over the Arctic. Specifically, we will assess perturbations in the distribution of the wind, temperature and pressure fields in the UTLS region. Our study will be based on simulations using a high resolution chemical weather model for four scenarios of current (2006) and future (2050) climate: with and without aircraft emissions. The tool that we use is the GEM-AC (Global Environmental Multiscale with Atmospheric Chemistry) chemical weather model where air quality, free tropospheric and stratospheric chemistry processes are on-line and interactive in an operational weather forecast model of Environment Canada. In vertical, the model domain is defined on 70 hybrid levels with model top at 0.1 mb. The gas-phase chemistry includes detailed reactions of Ox, NOx, HOx, CO, CH4, ClOx and BrO. Also, the model can address aerosol microphysics and gas-aerosol partitioning. Aircraft emissions are from the AEDT 2006 database developed by the Federal Aviation Administration (USA) and the future climate simulations are based on RCP8.5 projection presented by the IPCC in the fifth Assessment Report AR5. Results from model simulations on a global variable grid with 0.5o x 0.5o uniform resolution over the Arctic will be presented.

Aerosol indirect effect on tropospheric ozone via lightning

NASA Astrophysics Data System (ADS)

Yuan, Tianle; Remer, Lorraine A.; Bian, Huisheng; Ziemke, Jerald R.; Albrecht, Rachel; Pickering, Kenneth E.; Oreopoulos, Lazaros; Goodman, Steven J.; Yu, Hongbin; Allen, Dale J.

2012-09-01

Tropospheric ozone (O3) is a pollutant and major greenhouse gas and its radiative forcing is still uncertain. Inadequate understanding of processes related to O3 production, in particular those natural ones such as lightning, contributes to this uncertainty. Here we demonstrate a new effect of aerosol particles on O3production by affecting lightning activity and lightning-generated NOx (LNOx). We find that lightning flash rate increases at a remarkable rate of 30 times or more per unit of aerosol optical depth. We provide observational evidence that indicates the observed increase in lightning activity is caused by the influx of aerosols from a volcano. Satellite data analyses show O3is increased as a result of aerosol-induced increase in lightning and LNOx, which is supported by modle simulations with prescribed lightning change. O3production increase from this aerosol-lightning-ozone link is concentrated in the upper troposphere, where O3 is most efficient as a greenhouse gas. In the face of anthropogenic aerosol increase our findings suggest that lightning activity, LNOx and O3, especially in the upper troposphere, have all increased substantially since preindustrial time due to the proposed aerosol-lightning-ozone link, which implies a stronger O3 historical radiative forcing. Aerosol forcing therefore has a warming component via its effect on O3 production and this component has mostly been ignored in previous studies of climate forcing related to O3and aerosols. Sensitivity simulations suggest that 4-8% increase of column tropospheric ozone, mainly in the tropics, is expected if aerosol-lighting-ozone link is parameterized, depending on the background emission scenario. We note, however, substantial uncertainties remain on the exact magnitude of aerosol effect on tropospheric O3 via lightning. The challenges for obtaining a quantitative global estimate of this effect are also discussed. Our results have significant implications for understanding past and projecting future tropospheric O3forcing as well as wildfire changes and call for integrated investigations of the coupled aerosol-cloud-chemistry system.

Vertical distribution and sources of tropospheric ozone over South China in spring 2004: Ozonesonde measurements and modeling analysis

NASA Astrophysics Data System (ADS)

Zhang, Y.; Liu, H.; Crawford, J. H.; Considine, D. B.; Chan, C.; Scientific Team Of Tapto

2010-12-01

The Transport of Air Pollutant and Tropospheric Ozone over China (TAPTO-China) science initiative is a two-year (TAPTO 2004 and 2005) field measurement campaign to help improve our understanding of the physical and chemical processes that control the tropospheric ozone budget over the Chinese subcontinent (including the Asian Pacific rim) and its surrounding SE Asia. In this paper, we use two state-of-the-art 3-D global chemical transport models (GEOS-Chem and Global Modeling Initiative or GMI) to examine the characteristics of vertical distribution and quantify the sources of tropospheric ozone by analysis of TAPTO in-situ ozonesonde data obtained at five stations in South China during spring (April and May) 2004: Lin’an (30.30N, 119.75E), Tengchong (25.01N, 98.30E), Taipei (25.0N, 121.3E), Hong Kong (22.21N, 114.30E) and Sanya (18.21N, 110.31E). The observed tropospheric ozone concentrations show strong spatial and temporal variability, which is largely captured by the models. The models simulate well the observed vertical gradients of tropospheric ozone at higher latitudes but are too low at lower latitudes. Model tagged ozone simulations suggest that stratosphere has a large impact on the upper and middle troposphere (UT/MT) at Lin’an and Tengchong. Continental SE Asian biomass burning emissions are maximum in March but still contribute significantly to the photochemical production of tropopheric ozone in South China in early April. Asian anthropogenic emissions are the major contribution to lower tropospheric ozone at all stations. On the other hand, there are episodes of influence from European/North American anthropogenic emissions. For example, model tagged ozone simulations show that over Lin’an in April 2004, stratosphere contributes 20% (13 ppbv) at 5 km, Asian boundary layer contributes 70% (46 ppbv) to ozone in the boundary layer, European boundary layer contributes 5% (3-4 ppbv) at 1.2 km, and North American boundary layer contributes 4.5% (3 ppbv) at 1.2 km. Lastly, our analysis suggests that lightning NOx emissions have substantial impact on the UT/MT ozone over South China. We argue that model underestimate of ozone concentrations, especially at lower latitudes, is likely due to too low lightning NOx emissions.

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

NASA Technical Reports Server (NTRS)

Jeker, Dominique P.; Pfister, Lenny; Brunner, Dominik; Boccippio, Dennis J.; Pickering, Kenneth E.; Thompson, Anne M.; Wernli, Heini; Selkirk, Rennie B.; Kondo, Yutaka; Koike, Matoke

1997-01-01

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.

Applications of OMI Tropospheric NO(Sub 2) Data: Air Quality Trends in the US and Lightning NO(x) Source Strength

NASA Technical Reports Server (NTRS)

Pickering, Kenneth; Prados, Ana; Bucsela, Eric

2010-01-01

This talk will be presented in two parts: 1) an analysis of tropospheric column NO2 trends in the eastern half of the United States over the period 2005 to 2009 and 2) estimation of lightning NO(x) production rates based on OMI observations and lightning flash rate data. The air quality trends in the eastern US will be determined for specific subregions using tropospheric column NO2 data from OMI for 2005 through 2008 and from GOME-2 for 2007 through 2009. This period is characterized by significant NO(x) emission reductions at power plants within most of this region. The air quality trends will be compared with those estimated from continuous emission monitoring data from the power plants compiled by the US Environmental Protection Agency. OMI NO2 data have also been used to estimate lightning NOx production per flash in selected storms near Costa Rica and Panama during the 2007 NASA TC4 field campaign and over the continental US, Gulf of Mexico, and western Atlantic during the summers of 2005 and 2006. The lightning signal is extracted from the OMI data through a custom retrieval in which an NO2 profile representative of convective outflow is used in the airmass factor calculation and the background NO2 column is subtracted from the tropospheric column. When combined with NO(x)/NO2 ratios from the NASA GMT model and observed flash rates, the resulting estimates of NO(x) production per flash are comparable to those estimated obtained from analyses of aircraft data and cloud-resolving modeling.

Tropospheric Ozone Over North America

NASA Astrophysics Data System (ADS)

Oltmans, S. J.; Thompson, A. M.; Cooper, O. R.; Merrill, J. T.; Tarasick, D. W.; Newchurch, M. J.

2007-05-01

Ozone in the troposphere plays a significant role as an absorber of infrared radiation (greenhouse gas), in the cleansing capacity of the atmosphere as a precursor of hydroxol radical formation, and a regulated air pollutant capable of deleterious health and ecosystem effects. Knowledge of the ozone budget in the troposphere over North America (NA) is required to properly understand the various mechanisms that contribute to the measured distribution and to develop and test models capable of simulating and predicting this key player in atmospheric chemical and physical processes. Recent field campaigns including the 2004 and 2006 INTEX Ozone Network Studies (IONS) http:croc.gsfc.nasa.gov/intexb/ions06.html that have included intensive ozone profile measurements from ozonesondes provide a unique data set for describing tropospheric ozone over a significant portion of the North American continent. These campaigns have focused on the spring and summer seasons when tropospheric ozone over NA is particularly influenced by long-range transport processes, significant photochemical ozone production resulting from both anthropogenic and natural (lightning) precursor emissions, and exchange with the stratosphere. This study uses ozone profiles measured over NA in the latitude band from approximately 12-60N, extending from the tropics to the high mid latitudes, to describe the seasonal behavior of tropospheric ozone over NA with an emphasis on the spring and summer. This includes the variability within seasons at a particular site as well as the contrasts between the seasons. Emphasis is placed on the variations among the sites including latitudinal and longitudinal gradients and how these differ through the seasons and with altitude in the troposphere. Regional differences are most pronounced during the summer season likely reflecting the influence of a wider variation in processes influencing the tropospheric ozone distribution including lightning NOX production in the upper troposphere and active photochemistry from human emitted precursors in the lower troposphere. In all seasons, including the summer, transfer from the stratosphere significantly influences the upper tropospheric distribution at mid latitude (35-55N) locations. Although the seasonal maximum is found in spring in most locations and throughout much of the troposphere, this season tends to show less geographic variability compared to the summer. The FLEXPART Lagrangian tracer model is used to help identify processes associated with distinctive profile characteristics in the ozonesonde measurements.

Correction to "Asian chemical Outflow to the Pacific in Spring: Origins, Pathways, and Budgets" by Isabelle Bey et al.

NASA Technical Reports Server (NTRS)

Bey, Isabelle; Jacob, Daniel J.; Logan, Jennifer A.; Yantosca, Robert M.

2003-01-01

We analyze the Asian outflow of CO, ozone, and nitrogen oxides (NOx) to the Pacific in spring by using the GEOS-CHEM global three-dimensional model of tropospheric chemistry and simulating the Pacific Exploratory Mission-West (PEM-West B) aircraft mission in February-March 1994. The GEOS-CHEM model uses assimilated meteorological fields from the NASA Goddard Earth Observing System (GEOS). It reproduces relatively well the main features of tropospheric ozone, CO, and reactive nitrogen species observed in PEM-West B, including latitudinal and vertical gradients of the Asian pollution outflow over the western Pacific although simulated concentrations of CO tend to be too low (possibly because biogenic sources are underestimated). We use CO as a long-lived tracer to diagnose the processes contributing to the outflow. The highest concentrations in the outflow are in the boundary layer (0-2 km), but the strongest outflow fluxes are in the lower free troposphere (2-5 km) and reflect episodic lifting of pollution over central and eastern China ahead of eastward moving cold fronts. This frontal lifting, followed by westerly transport in the lower free troposphere, is the principal process responsible for export of both anthropogenic and biomass burning pollution from Asia. Anthropogenic emissions from Europe and biomass burning emissions from Africa make also major contributions to the Asian outflow over the western Pacific; European sources dominate in the lower troposphere north of 40 degrees N, while African sources are important in the upper troposphere at low latitudes. For the period of PEM-West B (February-March) we estimate that fossil fuel combustion and biomass burning make comparable contributions to the budgets of CO, ozone, and NO, in the Asian outflow. We find that 13% of NO, emitted in Asia is exported as NO, or PAN, a smaller fraction than for the United States because of higher aerosol concentrations that promote heterogeneous conversion of NOx to HNO3. Production and export of ozone from Asia in spring is much greater than from the United States because of the higher photochemical activity.

Sensitivity of Methane Lifetime and Transport to Sulfate Geoengineering

NASA Astrophysics Data System (ADS)

Aquila, V.; Pitari, G.; Tilmes, S.; Cionni, I.; de Luca, N.; Di Genova, G.; Iachetti, D.

2014-12-01

Sulfate geoengineering, made by sustained injection of SO2 in the tropical lower stratosphere, may impact the abundance of tropospheric methane through several photochemical mechanisms affecting the tropospheric OH abundance and hence the methane lifetime. Changes of the stratospheric Brewer-Dobson circulation also play a role in the upper tropospheric CH4 transport. Three mechanisms lead to lower OH concentrations and a longer CH4 lifetime: (a) solar radiation scattering increases the planetary albedo and cools the surface, with a tropospheric water vapor decrease as a response to this cooling. (b) The tropospheric UV budget is upset by the additional aerosol scattering and stratospheric ozone changes: the net effect is meridionally not uniform, with a net decrease in the tropics, thus producing less tropospheric O(1D). (c) The extra-tropical downwelling motion from the lower stratosphere tends to increase the sulfate aerosol surface area density available for heterogeneous chemical reactions in the mid-upper troposphere, thus reducing the amount of NOx and tropospheric O3 production. On the other hand, the tropical lower stratosphere is warmed by solar and planetary radiation absorption by the aerosols. The heating rates perturbation are strongly latitude dependent, producing a significant change of the pole-to-equator temperature gradient and mean zonal wind distribution, with a net increase of tropical upwelling. A stronger meridional component of the Brewer-Dobson circulation increases the extra-tropical stratosphere to troposphere transport of CH4 poorer air, resulting in less CH4 transported in the UTLS. The net effect on tropospheric OH may be positive or negative depending on the net result of different superimposed species perturbations in the UTLS, i.e. CH4 (negative), NOy and O3 (positive). Three climate-chemistry coupled models are used here to explore the above radiative, chemical and dynamical mechanisms affecting the methane lifetime (ULAQ-CCM, GEOSCCM, CCSM-CAM4). First results show that the CH4 lifetime may become significantly longer (by about 10%) with a sustained injection of 2.5 Tg-S/yr started in year 2020, which implies an increase of tropospheric CH4 (200 ppbv) and a positive indirect radiative forcing of sulfate geoengineering due to CH4 changes (+0.1 W/m2 in the 2045).

Radiative forcing from aircraft NOx emissions: Mechanisms and seasonal dependence

NASA Astrophysics Data System (ADS)

Stevenson, David S.; Doherty, Ruth M.; Sanderson, Michael G.; Collins, William J.; Johnson, Colin E.; Derwent, Richard G.

2004-09-01

A chemistry-climate model has been applied to study the radiative forcings generated by aircraft NOx emissions through changes in ozone and methane. Four numerical experiments, where an extra pulse of aircraft NOx was emitted into the model atmosphere for a single month (January, April, July, or October), were compared to a control experiment, allowing the aircraft impact to be isolated. The extra NOx produces a short-lived (few months) pulse of ozone that generates a positive radiative forcing. However, the NOx and O3 both generate OH, which leads to a reduction in CH4. A detailed analysis of the OH budget reveals the spatial structure and chemical reactions responsible for the generation of the OH perturbation. Methane's long lifetime means that the CH4 anomaly decays slowly (perturbation lifetime of 11.1 years). The negative CH4 anomaly also has an associated negative O3 anomaly, and both of these introduce a negative radiative forcing. There are important seasonal differences in the response of O3 and CH4 to aircraft NOx, related to the annual cycle in photochemistry; the O3 radiative forcing calculations also have a seasonal dependence. The long-term globally integrated annual mean net forcing calculated here is approximately zero, although earlier work suggests a small net positive forcing. The model design (e.g., upper tropospheric chemistry, convection parameterization) and experimental setup (pulse magnitude and duration) may somewhat influence the results: further work with a range of models is required to confirm these results quantitatively.

Lightning Applications in Weather and Climate Research

NASA Astrophysics Data System (ADS)

Price, Colin G.

2013-11-01

Thunderstorms, and lightning in particular, are a major natural hazard to the public, aviation, power companies, and wildfire managers. Lightning causes great damage and death every year but also tells us about the inner working of storms. Since lightning can be monitored from great distances from the storms themselves, lightning may allow us to provide early warnings for severe weather phenomena such as hail storms, flash floods, tornadoes, and even hurricanes. Lightning itself may impact the climate of the Earth by producing nitrogen oxides (NOx), a precursor of tropospheric ozone, which is a powerful greenhouse gas. Thunderstorms themselves influence the climate system by the redistribution of heat, moisture, and momentum in the atmosphere. What about future changes in lightning and thunderstorm activity? Many studies show that higher surface temperatures produce more lightning, but future changes will depend on what happens to the vertical temperature profile in the troposphere, as well as changes in water balance, and even aerosol loading of the atmosphere. Finally, lightning itself may provide a useful tool for tracking climate change in the future, due to the nonlinear link between lightning, temperature, upper tropospheric water vapor, and cloud cover.

HEPPA-II model-measurement intercomparison project: EPP indirect effects during the dynamically perturbed NH winter 2008-2009

NASA Astrophysics Data System (ADS)

Funke, Bernd; Ball, William; Bender, Stefan; Gardini, Angela; Harvey, V. Lynn; Lambert, Alyn; López-Puertas, Manuel; Marsh, Daniel R.; Meraner, Katharina; Nieder, Holger; Päivärinta, Sanna-Mari; Pérot, Kristell; Randall, Cora E.; Reddmann, Thomas; Rozanov, Eugene; Schmidt, Hauke; Seppälä, Annika; Sinnhuber, Miriam; Sukhodolov, Timofei; Stiller, Gabriele P.; Tsvetkova, Natalia D.; Verronen, Pekka T.; Versick, Stefan; von Clarmann, Thomas; Walker, Kaley A.; Yushkov, Vladimir

2017-03-01

We compare simulations from three high-top (with upper lid above 120 km) and five medium-top (with upper lid around 80 km) atmospheric models with observations of odd nitrogen (NOx = NO + NO2), temperature, and carbon monoxide from seven satellite instruments (ACE-FTS on SciSat, GOMOS, MIPAS, and SCIAMACHY on Envisat, MLS on Aura, SABER on TIMED, and SMR on Odin) during the Northern Hemisphere (NH) polar winter 2008/2009. The models included in the comparison are the 3-D chemistry transport model 3dCTM, the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model, FinROSE, the Hamburg Model of the Neutral and Ionized Atmosphere (HAMMONIA), the Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA), the modelling tools for SOlar Climate Ozone Links studies (SOCOL and CAO-SOCOL), and the Whole Atmosphere Community Climate Model (WACCM4). The comparison focuses on the energetic particle precipitation (EPP) indirect effect, that is, the polar winter descent of NOx largely produced by EPP in the mesosphere and lower thermosphere. A particular emphasis is given to the impact of the sudden stratospheric warming (SSW) in January 2009 and the subsequent elevated stratopause (ES) event associated with enhanced descent of mesospheric air. The chemistry climate model simulations have been nudged toward reanalysis data in the troposphere and stratosphere while being unconstrained above. An odd nitrogen upper boundary condition obtained from MIPAS observations has further been applied to medium-top models. Most models provide a good representation of the mesospheric tracer descent in general, and the EPP indirect effect in particular, during the unperturbed (pre-SSW) period of the NH winter 2008/2009. The observed NOx descent into the lower mesosphere and stratosphere is generally reproduced within 20 %. Larger discrepancies of a few model simulations could be traced back either to the impact of the models' gravity wave drag scheme on the polar wintertime meridional circulation or to a combination of prescribed NOx mixing ratio at the uppermost model layer and low vertical resolution. In March-April, after the ES event, however, modelled mesospheric and stratospheric NOx distributions deviate significantly from the observations. The too-fast and early downward propagation of the NOx tongue, encountered in most simulations, coincides with a temperature high bias in the lower mesosphere (0.2-0.05 hPa), likely caused by an overestimation of descent velocities. In contrast, upper-mesospheric temperatures (at 0.05-0.001 hPa) are generally underestimated by the high-top models after the onset of the ES event, being indicative for too-slow descent and hence too-low NOx fluxes. As a consequence, the magnitude of the simulated NOx tongue is generally underestimated by these models. Descending NOx amounts simulated with medium-top models are on average closer to the observations but show a large spread of up to several hundred percent. This is primarily attributed to the different vertical model domains in which the NOx upper boundary condition is applied. In general, the intercomparison demonstrates the ability of state-of-the-art atmospheric models to reproduce the EPP indirect effect in dynamically and geomagnetically quiescent NH winter conditions. The encountered differences between observed and simulated NOx, CO, and temperature distributions during the perturbed phase of the 2009 NH winter, however, emphasize the need for model improvements in the dynamical representation of elevated stratopause events in order to allow for a better description of the EPP indirect effect under these particular conditions.

Characterization of Regional Marginal Abatement Cost Curves for NOx that Incorporate Control Measures, Renewable Energy, Energy Efficiency and Fuel Switching

EPA Science Inventory

Anthropogenic nitrogen oxides (NOx) are emitted when fossil fuels are combusted. In the atmosphere, NOx reacts with volatile organic compounds (VOCs) to produce tropospheric ozone, a component of photochemical smog. In most parts of the country, strategies for reducing ozone gene...

Chemical Data Assimilation Estimates of Continental US Ozone and Nitrogen Budgets during INTEX-A

NASA Technical Reports Server (NTRS)

Pierce, Robert B.; Schaack, Todd K.; Al-Saadi, Jassim A.; Fairlie, T. Duncan; Kittaka, Chieko; Lingenfelser, Gretchen; Natarajan, Murali; Olson, Jennifer; Soja, Amber; Zapotocny, Tom;

Nitrogen oxides in the troposphere - Global and regional budgets

NASA Technical Reports Server (NTRS)

Logan, J. A.

1983-01-01

The cycle of nitrogen oxides in the troposphere is discussed from both global and regional perspectives. Global sources for NO(x) are estimated to be of magnitude 50 (+ or - 25) x 10 to the 12th gm N/yr. Nitrogen oxides are derived from combustion of fossil fuels (40 percent) and biomass burning (25 percent) with the balance from lightning and microbial activity in soils. Estimates for the rate of removal of NOx based on recent atmospheric and precipitation chemistry data are consistent with global source strengths derived here. Industrial and agricultural activities provide approximately two thirds of the global source for NOx. In North America, sources from combustion of fossil fuels exceed natural sources by a factor of 3-13. Wet deposition removes about one third of the combustion source of NOx over North America, while dry deposition removes a similar amount. The balance is exported from the continent. Deposition of nitrate in precipitation over eastern Canada and the western Atlantic is clearly influenced by sources of NOx in the eastern United States.

Chemical Characteristics of Continental Outflow from Asia to the Troposphere over the Western Pacific Ocean during September - October 1991: Results from PEM-West A

NASA Technical Reports Server (NTRS)

Talbot, R. W.; Dibb, J. E.; Klemm, K. I.; Bradshaw, J. D.; Sandholm, S. T.; Blake, D. R.; Sachse, G. W.; Collins, J.; Heikes, B. G.; Gregory, G. L.;

Is there a quantifiable relationship between lightning and nitrate deposition in the subtropics?

NASA Astrophysics Data System (ADS)

Langenbrunner, B.; Hastings, M. G.; Spak, S.; Petersen, W. A.

2009-12-01

Lightning is a significant natural source of nitrogen oxides (NOx). The high temperatures that occur in a lightning channel fix atmospheric N2, producing nitrogen monoxide (NO) that quickly forms NO2 (NOx = NO + NO2). Lightning-produced NOx (LNOx) dominates NOx concentrations in the upper troposphere, which affect tropospheric ozone and OH concentrations and in turn the oxidizing capacity of the atmosphere. The main sink for NOx in the atmosphere is formation of nitric acid (HNO3) and subsequent deposition of nitrate (NO3-). A widely accepted estimate for the global LNOx production rate is ~5±3 TgN/yr (uncertainty of 1-20 TgN/yr). The global source term for NOx is an estimated 50 TgN/yr. Global chemical transport model studies have found that LNOx contributes to NO3- deposition (wet+dry) that is nearly equal over both land and ocean, with the greatest deposition between 30°N and 30°S. Models also predict that lightning can be the dominant source of NO3- deposition in areas where industrial sources are limited. Is it possible that an empirical relationship exists between NO3- deposition and lightning? Using 10 years of deposition, lightning, and meteorological data, we investigate the relationship between lightning and NO3- in the subtropics and assess meteorological variables that contribute significantly to the distribution of LNOx and NO3-. For NO3- deposition, we use weekly, monthly, and event-based wet deposition data from 8 coastal sites in Florida, the US Virgin Islands, and Puerto Rico (NADP); satellite and ground-based lightning data in the same region is from TRMM and Unidata; meteorology is obtained from the NCEP/NCAR Reanalysis. We use multiple linear regression in an attempt to explain variance among historical NO3- data, lightning and meteorology. We expect certain meteorological variables—particularly those related to transport and deposition—to help illuminate a relation between lightning and NO3-. The relation between NOx emissions and NO3- deposition is unclear, as is the ability to constrain NO3- sources to any given location and decouple anthropogenic versus natural effects. Our investigation addresses such questions as: from daily and monthly rain data, can total, average, or extreme precipitation events explain temporal/spatial NO3- distribution? Using numerical weather models, can regional meteorology predict NO3- deposition related to LNOx? Moreover, could such a prediction distinguish between free troposphere and planetary boundary layer sources of NO3-? How much of NO3- deposition is due to local LNOx sources versus regional transport? Quantifying the relationship between lightning and NO3- will be useful in evaluating atmospheric chemistry models, and such results could provide insight in predicting lightning-influenced NO3- deposition under future climate change scenarios. Furthermore, elucidating LNOx's impact on NO3- would provide a means to better constrain natural and anthropogenic effects on the global N cycle.

Analysis of alternative pathways for reducing nitrogen oxide emissions

EPA Science Inventory

Strategies for reducing tropospheric ozone typically include modifying combustion processes to reduce the formation of nitrogen oxides (NOx) and applying control devices that remove NOx from the exhaust gases of power plants, industrial sources and vehicles. For portions of the ...

Influence of the North Atlantic Oscillation on European tropospheric composition: an observational and modelling study

NASA Astrophysics Data System (ADS)

Pope, R.; Chipperfield, M.

2017-12-01

The North Atlantic Oscillation (NAO) has a strong influence on winter-time North Atlantic and European circulation patterns. Under the positive phase of the NAO (NAO+), intensification of the climatological Icelandic low and Azores high pressure systems results in strong westerly flow across the Atlantic into Europe. Under the NAO negative phase (NAO-), there is a weakening of this meridional pressure gradient resulting in a southerly shift in the westerlies flow towards the sub-tropical Atlantic. Therefore, NAO+ and NAO- introduce unstable stormy and drier stable conditions into Europe, respectively. Under NAO+ conditions, the strong westerlies tend to enhance transport of European pollution (e.g. nitrogen oxides) away from anthropogenic source regions. While during NAO-, the more stable conditions lead to a build up of pollutants. However, secondary pollutants (i.e. tropospheric ozone) show the opposite signal where NAO+, while transporting primary pollutants away, introduces Atlantic ozone enriched air into Europe. Here ozone can form downwind of pollution from continental North America and be transported into Europe via the westerly flow. Under NAO-, this westerly ozone transport is reduced yielding lower European ozone concentrations also depleted further by ozone loss through the reaction with NOx, which has accumulated over the continent. Peroxyacetyl nitrate (PAN), observed in the upper troposphere - lower stratosphere (UTLS) by satellite, peaks over Iceland/Southern Greenland in NAO-, between 200-100 hPa, consistent with trapping by an anticyclone at this altitude. During NAO+, PAN is enhanced over the sub-tropical Atlantic and Arctic. Model simulations show that enhanced PAN over Iceland/Southern Greenland in NAO- is associated with vertical transport from the troposphere into the UTLS, while peak Arctic PAN in NAO+ is its accumulation given the strong northerly meridional transport in the UTLS. UTLS ozone spatial anomalies, relative to the winter-time average, are anti-correlated with that of PAN. Even though PAN is a source of NOx, which can influence the ozone budget chemically, we show here that these anti-correlations are likely linked primary to UTLS circulation and troposphere-stratosphere exchanges.

Lightning NOx Estimates from Space-Based Lightning Imagers

NASA Technical Reports Server (NTRS)

Koshak, William J.

2017-01-01

The intense heating of air by a lightning channel, and subsequent rapid cooling, leads to the production of lightning nitrogen oxides (NOx = NO + NO2) as discussed in Chameides [1979]. In turn, the lightning nitrogen oxides (or "LNOx" for brevity) indirectly influences the Earth's climate because the LNOx molecules are important in controlling the concentration of ozone (O3) and hydroxyl radicals (OH) in the atmosphere. Climate is most sensitive to O3 in the upper troposphere, and LNOx is the most important source of NOx in the upper troposphere at tropical and subtropical latitudes; hence, lightning is a useful parameter to monitor for climate assessments. The National Climate Assessment (NCA) program was created in response to the Congressionally-mandated Global Change Research Act (GCRA) of 1990. Thirteen US government organizations participate in the NCA program which examines the effects of global change on the natural environment, human health and welfare, energy production and use, land and water resources, human social systems, transportation, agriculture, and biological diversity. The NCA focuses on natural and human-induced trends in global change, and projects major trends 25 to 100 years out. In support of the NCA, the NASA Marshall Space Flight Center (MSFC) continues to assess lightning-climate inter-relationships. This activity applies a variety of NASA assets to monitor in detail the changes in both the characteristics of ground- and space- based lightning observations as they pertain to changes in climate. In particular, changes in lightning characteristics over the conterminous US (CONUS) continue to be examined by this author using data from the Tropical Rainfall Measuring Mission Lightning Imaging Sensor. In this study, preliminary estimates of LNOx trends derived from TRMM/LIS lightning optical energy observations in the 17 yr period 1998-2014 are provided. This represents an important first step in testing the ability to make remote retrievals of LNOx from a satellite-based lightning sensor. As is shown, the methodology can also be directly applied to more recently launched lightning mappers, such as the Geostationary Lightning Mapper, and the International Space Station LIS.

Tropospheric HONO Distribution and Chemistry in the Southeastern U.S.

NASA Astrophysics Data System (ADS)

Zhou, X.; Ye, C.; Pu, D.; Stutz, J.; Festa, J.; Spolaor, M.; Weinheimer, A. J.; Campos, T. L.; Haggerty, J. A.; Cantrell, C. A.; Mauldin, L.; Guenther, A. B.; Hornbrook, R. S.; Apel, E. C.; Jensen, J. B.

2014-12-01

During the NOMADSS field campaign, nitrous acid (HONO) and particulate nitrate (pNO3) was measured on NCAR C-130 research aircraft during five research flights over the Southeast U.S. Aerosol samples were also collected on Teflon filters for the determination of pNO3 photolysis rate constants in the laboratory. Daytime HONO concentrations range from low ppt in free troposphere to 10-20 ppt in the boundary layer in the background air masses, to up to 40 ppt in the industrial and urban plumes. While daytime HONO sink is well defined, dominated by its photolysis, daytime sources vary in different types of air masses: pNO3 photolysis appears to be the major HONO source in the background terrestrial air masses in both the boundary layer and the free troposphere. With an average pNO3 photolysis rate constant of (2.8±1.7)×10-4 s-1, p-NO3 photolysis becomes to be an effective pathway to recycle HNO3 to NOx in the troposphere, with HONO as a dominant intermediate product. Within the high-NOx industrial plumes encountered, HONO is predominantly produced by secondary formation processes involving NOx as the precursor. Away from ground surface, no significant nighttime HONO accumulation exists in the background terrestrial air mass.

Evaluating the Potential Importance of Monoterpene Degradation for Global Acetone Production

NASA Astrophysics Data System (ADS)

Kelp, M. M.; Brewer, J.; Keller, C. A.; Fischer, E. V.

2015-12-01

Acetone is one of the most abundant volatile organic compounds (VOCs) in the atmosphere, but estimates of the global source of acetone vary widely. A better understanding of acetone sources is essential because acetone serves as a source of HOx in the upper troposphere and as a precursor to the NOx reservoir species peroxyacetyl nitrate (PAN). Although there are primary anthropogenic and pyrogenic sources of acetone, the dominant acetone sources are thought to be from direct biogenic emissions and photochemical production, particularly from the oxidation of iso-alkanes. Recent work suggests that the photochemical degradation of monoterpenes may also represent a significant contribution to global acetone production. We investigate that hypothesis using the GEOS-Chem chemical transport model. In this work, we calculate the emissions of eight terpene species (α-pinene, β-pinene, limonene, Δ3-carene, myrcene, sabinene, trans-β-ocimene, and an 'other monoterpenes' category which contains 34 other trace species) and couple these with upper and lower bound literature yields from species-specific chamber studies. We compare the simulated acetone distributions against in situ acetone measurements from a global suite of NASA aircraft campaigns. When simulating an upper bound on yields, the model-to-measurement comparison improves for North America at both the surface and in the upper troposphere. The inclusion of acetone production from monoterpene degradation also improves the ability of the model to reproduce observations of acetone in East Asian outflow. However, in general the addition of monoterpenes degrades the model comparison for the Southern Hemisphere.

The Impact of Upper Tropospheric Humidity from Microwave Limb Sounder on the Midlatitude Greenhouse Effect

NASA Technical Reports Server (NTRS)

Hu, Hua; Liu, W. Timothy

1998-01-01

This paper presents an analysis of upper tropospheric humidity, as measured by the Microwave Limb Sounder, and the impact of the humidity on the greenhouse effect in the midlatitudes. Enhanced upper tropospheric humidity and an enhanced greenhouse effect occur over the storm tracks in the North Pacific and North Atlantic. In these areas, strong baroclinic activity and the large number of deep convective clouds transport more water vapor to the upper troposphere, and hence increase greenhouse trapping. The greenhouse effect increases with upper tropospheric humidity in areas with a moist upper troposphere (such as areas over storm tracks), but it is not sensitive to changes in upper tropospheric humidity in regions with a dry upper troposphere, clearly demonstrating that there are different mechanisms controlling the geographical distribution of the greenhouse effect in the midlatitudes.

Airborne Measurements of NO, NO2, and NO(y) as Related to NASA's Pacific Exploratory Mission

NASA Technical Reports Server (NTRS)

Sandholm, Scott

1997-01-01

The Tropospheric Trace Gas and Airborne Measurements Group's (TTGAMG) efforts on NASA GTE (Global Tropospheric Experiment) PEM (Pacific Exploratory Mission) West A & B field campaign primarily involved the acquisition of NO, NO2 and NO(y) measurements, as well as the subsequent analysis and interpretation of the data base obtained during the PEM West field campaign. These investigations focused on the distribution of trace gases, sources and sinks of ozone, ozone producing precursors with a heavy emphasize on ozone's photochemical state, and the partitioning of the molecules within the NO(y) family over the north western Pacific Ocean. The two components of PEM West were focused on observing air masses as they reached the Asian Continent (PEM West A) or as the air mass departed the Asian Continent (PEM West B). NO(x) concentrations play a pivotal role in controlling the photochemical lifetime of ozone in these environments, and understanding the NO(x) species partitioning is paramount. The transport of NO(x) into the regions, in the form of longer lived NO(y) family members, was examined in relation to the comparison of natural occurring sources of NO(x) (i.e., lightning and stratosphere/troposphere exchange) to those produced as a result of anthropogenic activity (i.e., biomass burning and aircraft emissions). The TTGAMG's measurements of NOx and NO(y), in conjunction with other investigators' measurements of PAN (H. B. Singh's group) and HNO3 (R. W. Talbot's group), have been used to assess the total reactive odd nitrogen levels over the study regions, the partitioning of the reactive odd nitrogen species in their various forms, and the usefulness of the NO, measurement and its measurement technique. The TTGAMG's primary PEM West objectives were the characterization of the factors controlling the distribution and fate of reactive odd nitrogen compounds over the western Pacific Ocean and an analysis of the concentration of various trace gases in the troposphere as the air mass aged by both dynamical mixing and photochemical processes in the troposphere.

Summertime distribution of PAN and other reactive nitrogen species in the northern high-latitude atmosphere of eastern Canada

NASA Technical Reports Server (NTRS)

Singh, H. B.; Herlth, D.; O'Hara, D.; Zahnle, K.; Bradshaw, J. D.; Sandholm, S. T.; Talbot, R.; Gregory, G. L.; Sachse, G. W.; Blake, D. R.

1994-01-01

Aircraft measurements of key reactive nitrogen species (NO, NO2, HNO3, PAN, PPN, NO3(-), NO(y)), C1 to C6 hydrocarbons, acetone, O3, chemical tracers (C2Cl4, CO), and important meteorological parameters were performed over eastern Canada during July to August 1990 at altitudes between 0 and 6 km as part of an Arctic Boundary Layer Expedition (ABLE3B). In the free troposphere, PAN was found to be the single most abundant reactive nitrogen species constituting a major fraction of NO(y) and was significantly more abundant than NO(x) and HNO3. PAN and O3 were well correlated both in their fine and gross structures. Compared to data previously collected in the Arctic/subarctic atmosphere over Alaska (ABLE3A), the lower troposphere (0-4 km) over eastern Canada was found to contain larger reactive nitrogen and anthropogenic tracer concentrations. At higher altitudes (4-6 km) the atmospheric composition was in many ways similar to what was seen over Alaska and supports the view that a large-scale reservoir of PAN (and NO(y)) is present in the upper troposphere over the entire Arctic/subarctic region. The reactive nitrogen budget based on missions conducted from the North Bay site (missions 2-10) showed a small shortfall, whereas the budget for data collected from the Goose Bay operation (missions 11-19) showed essential balance. It is calculated that 15-20 ppt of the observed NO(x) may find its source from the available PAN reservoir. Meteorological considerations as well as relationships between reactive nitrogen and tracer species suggest that the atmosphere over eastern Canada during summer is greatly influenced by forest fires and transported industrial pollution.

Source Attribution of Tropospheric Ozone using a Global Model

NASA Astrophysics Data System (ADS)

Coates, J.; Lupascu, A.; Butler, T. M.; Zhu, S.

2016-12-01

Tropospheric ozone is both a short-lived climate forcing pollutant and a radiatively active greenhouse gas. Ozone is not directly emitted into the troposphere but photochemically produced from chemical reactions involving nitrogen oxides (NOx) and volatile organic compounds (VOCs). Emissions of ozone precursors (NOx and VOCs) have both natural and anthropogenic sources and may be transported away from their sources to produce ozone downwind. Also, transport of ozone from the stratosphere into the troposphere also influences tropospheric ozone levels in some regions. Attributing ozone concentrations to the contributions from different sources would indicate the effects of locally emitted or transported precursors on ozone levels in specific regions. This information could be used to inform the emission reduction strategies of ozone precursors by indicating which emission sources could be targeted for effective reductions thus reducing the burden of ozone pollution. We use a "tagging" approach within the CESM global model to attribute ozone levels to their source emissions. We use different tags to quantify the impact from natural (soils, lightning, stratospheric transport) and anthropogenic (aircraft, biomass burning) sources of NOx and VOCs (including methane) on ozone levels. These source sectors of different global regions are assigned based on the global emissions specified by HTAPv2.2. Using these results, we develop a transboundary source-receptor relationship of ozone concentration to its precursor emission regions. Additionally, the transport of ozone precursors from regional anthropogenic sources is analysed to illustrate the extent to which mitigation strategies of regional emissions aid in mitigating global ozone levels.

An intercomparison of results from ferrous sulphate and photolytic converter techniques for measurements of NO(x) made during the NASA GTE/CITE 1 aircraft program

NASA Technical Reports Server (NTRS)

Ridley, B. A.; Carroll, M. A.; Torres, A. L.; Condon, E. P.; Sachse, G. W.; Hill, G. F.; Gregory, G. L.

1988-01-01

Two techniques designed for measurements of NO(x (NO + NO2) were intercompared during aircraft flights made in the spring of 1984 in the middle free troposphere over the eastern Pacific Ocean and southwestern U.S. One NO chemiluminescence instrument was equipped with a ferrous sulphate converter, another with a photolytic converter. The ferrous sulphate-equipped instrument was apparently much less specific for NO2. It registered levels about three times larger than the photolytic converter and gave NO2/NO ratios that were much larger than photochemical calculations would indicate as reasonable. Additionally, the results imply that active NO(x) was only 10-20 percent of the total odd nitrogen in the middle free troposphere.

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

NASA Technical Reports Server (NTRS)

Duncan, Bryan N.; Yoshida, Yasuko; Olson, Jennifer R.; Sillman, Sanford; Martin, Randall V.; Lamsal, Lok; Hu, Yongtao; Pickering, Kenneth E.; Retscher, Christian; Allen, Dale J.;

Global Ozone and Reactive Nitrogen : Composition, Chemistry and Sources

NASA Technical Reports Server (NTRS)

Sing, Hanwant B.; Bradshaw, J.; Davis, D.; Gregory, G.; Talbot, R.

1994-01-01

Ozone plays a central role in the chemistry of the atmosphere both as an ultraviolet shield and as a source of hydroxyl radicals (OH), a potent initiator of atmospheric chemistry. There is evidence to suggest that the ozone abundance in the troposphere (0-10 km) has doubled since the industrial revolution and continues to increase to date. The principle reason for this increase is thought to be the increasing emissions of nitrogen oxides (NO(x)) from anthropogenic activities. Although NO(x) is highly reactive and its products such as HN03 are easily removed by deposition, it now appears that its chemistry is quite complex and it can be transported over long distances via its conversion to a variety of nitrates and penetrates. The sources of atmospheric NO(x) include free tropospheric sources such as lightning and subsonic aircraft, as well as surface emissions which are transported to the free troposphere via convective processes. Recent experimental and theoretical studies have tried to unravel the chemistry of reactive nitrogen species, its sources, and their role in ozone formation. In this presentation we shall describe the results from these studies.

Towards Improving Satellite Tropospheric NO2 Retrieval Products: Impacts of the spatial resolution and lighting NOx production from the a priori chemical transport model

NASA Astrophysics Data System (ADS)

Smeltzer, C. D.; Wang, Y.; Zhao, C.; Boersma, F.

2009-12-01

Polar orbiting satellite retrievals of tropospheric nitrogen dioxide (NO2) columns are important to a variety of scientific applications. These NO2 retrievals rely on a priori profiles from chemical transport models and radiative transfer models to derive the vertical columns (VCs) from slant columns measurements. In this work, we compare the retrieval results using a priori profiles from a global model (TM4) and a higher resolution regional model (REAM) at the OMI overpass hour of 1330 local time, implementing the Dutch OMI NO2 (DOMINO) retrieval. We also compare the retrieval results using a priori profiles from REAM model simulations with and without lightning NOx (NO + NO2) production. A priori model resolution and lightning NOx production are both found to have large impact on satellite retrievals by altering the satellite sensitivity to a particular observation by shifting the NO2 vertical distribution interpreted by the radiation model. The retrieved tropospheric NO2 VCs may increase by 25-100% in urban regions and be reduced by 50% in rural regions if the a priori profiles from REAM simulations are used during the retrievals instead of the profiles from TM4 simulations. The a priori profiles with lightning NOx may result in a 25-50% reduction of the retrieved tropospheric NO2 VCs compared to the a priori profiles without lightning. As first priority, a priori vertical NO2 profiles from a chemical transport model with a high resolution, which can better simulate urban-rural NO2 gradients in the boundary layer and make use of observation-based parameterizations of lightning NOx production, should be first implemented to obtain more accurate NO2 retrievals over the United States, where NOx source regions are spatially separated and lightning NOx production is significant. Then as consequence of a priori NO2 profile variabilities resulting from lightning and model resolution dynamics, geostationary satellite, daylight observations would further promote the next step towards producing a more complete NO2 data product provided sufficient resolution of the observations. Both the corrected retrieval algorithm and the proposed next generation geostationary satellite observations would thus improve emission inventories, better validate model simulations, and advantageously optimize regional specific ozone control strategies.

An Observationally Constrained Evaluation of the Oxidative Capacity in the Tropical Western Pacific Troposphere

NASA Technical Reports Server (NTRS)

Nicely, Julie M.; Anderson, Daniel C.; Canty, Timothy P.; Salawitch, Ross J.; Wolfe, Glenn M.; Apel, Eric C.; Arnold, Steve R.; Atlas, Elliot L.; Blake, Nicola J.; Bresch, James F.;

Tropospheric ozone long term trend observed by lidar and ECC ozonesondes at Observatoire de Haute Provence, Southern France.

NASA Astrophysics Data System (ADS)

Ancellet, G.; Gaudel, A.; Godin-Beekmann, S.

2016-12-01

Tropospheric ozone vertical profile measurements have been carried out at OHP (Observatoire de Haute Provence, 44°N, 6.7°E, 690 m) since 1991 using both UV DIAL (DIfferential Absorption Lidar) and ECC (Electrochemical Concentration Cell) ozonesondes. For the first time, ECC and lidar data measured at the same site, have been compared over a 24 year period. The comparison conducted reveals a bias between both measurement types (ECC - lidar) of the order of 0.6 ppbv. The measurements of both instruments have been however combined to decrease the impact of short-term atmospheric variability on the trend estimate. Air mass trajectories have been calculated for all the ozone observations available at OHP including ECMWF potential vorticity (PV) and humidity chnage along the trajectories. The interannual ozone variability shows a negligible trend in the mid troposphere, but a 0.36 ppbv/year significant positive ozone trend in the upper troposphere. The trends will be discussed using the variability of the meteorological parameters. Data clustering using PV and air mass trajectories is useful to identify the role of Stratosphere-Tropopshere Exchanges and long range transport of pollutants in the observed long term trends. In the lower troposphere, the interannual variability shows contrasted trends with an ozone decrease between 1998 and 2008, consistent with the NOx emission decrease, but a new period of ozone increase since 2008 which is not very well understood.

A one-dimensional photochemical model of the troposphere with planetary boundary-layer parameterization

NASA Technical Reports Server (NTRS)

Fishman, J.; Carney, T. A.

1984-01-01

A time-dependent, one-dimensional photochemical model of the troposphere is used to describe the vertical distribution of atmospheric trace constituents for summer-time conditions at midlatitudes in the Northern Hemisphere. The model incorporates a planetary boundary layer (PBL) parametrization and a detailed chemical mechanism that includes the photochemistry of important nonmethane hydrocarbon species formed during the oxidation process. One result of the parametrized PBL is that the concentrations of some trace species in the free troposphere are 20-30 percent higher than when mixing processes are described by a vertical eddy diffusion coefficient which is held constant with respect to height and time. The lifetime of the oxides of nitrogen against photochemical conversion to nitric acid during summertime conditions is on the order of six hours. This lifetime is short enough to deplete most of the NO(x) in the PBL so that other reactive nitrogen species are more abundant than NO(x) throughout the free troposphere.

Comparative Analysis of Seasonal Variation in Tropospheric Nitrogen Dioxide over Pakistan and Saudi Arabia

NASA Astrophysics Data System (ADS)

Fahim Khokhar, Muhammad; Wagner, Thomas; Jamil, Mohsin

2016-07-01

In this study, spatial and temporal distributions of tropospheric NO2 vertical column densities over Pakistan and Saudi Arabia during the time period of 2004-2015 are discussed. Data products from the satellite instrument OMI are used. The results show a large NO2 growth over major cities of both countries, particularly the areas with rapid urbanization. Different seasonal cycles were observed over both countries. Especially, seasonal variation in tropospheric NO2 over Pakistan is largely impacted by the photolysis rate, OH radical and monsoon rains in addition to soil emissions, agriculture fires and other anthropogenic activities. While in the case of Saudi Arabia, the seasonal variation in tropospheric NO2 is completely driven by thermal power generation. Furthermore, different regions of Pakistan exhibited different seasonal trends. In the provinces of Punjab (north-east), Khyber Paktunkhwa (north-west) and Sindh (south-east), NO2 columns are maximum in winter and minimum in summer months while a reversed seasonality was observed in the province of Baluchistan (south-west). We compared the observed Spatio-temporal patterns to existing emission inventories and found that for the most populated provinces the NOx emissions are clearly dominated by anthropogenic sources. In these areas also the strongest positive trends were observed. NOx released from soils and produced by lightning both together contribute about 20% for the provinces of Punjab, Sindh, and Khyber Pakhtunkhwa, while its contribution in Baluchistan is much stronger (~50%). NOx emissions from biomass burning are negligible. This finding can also explain the observed summer maximum in Baluchistan since the highest lightning activity occurs during the Monsoon season. Our comparison also indicates that the inventories of anthropogenic NOx emissions over Pakistan seem to underestimate the true emissions by about a factor of two.

Wildfire and soil emissions of NOx and their consequences for ozone observed at a remote mountaintop site in Central California

NASA Astrophysics Data System (ADS)

Asher, E. C. C.; Caputi, D.; Conley, S. A.; Faloona, I. C.

2016-12-01

Nitric oxide (NOx) emissions contribute to the production of tropospheric ozone and the nutrient supply fueling primary production. Current global estimates indicate that biomass burning, including wildfires, and soil emissions represent 15 - 25 % of the total emissions. Yet estimates suggest that in North America during the summer, natural sources, including biomass burning, soil emissions and lightning, are responsible for nearly half of total emissions. Thus, as domestic air quality standards grow stricter and anthropogenic sources more regulated, constraining natural sources of NOx becomes critical. NOx concentrations in wildfire smoke differ based on the age of the plume, fire intensity and vegetation type. NOx soil emissions depend on soil moisture, soil temperature, soil porosity, and nitrogen storage. We present two years of NOx and ozone (O3) measurements from a remote mountaintop monitoring site located on Chews Ridge in the coastal mountains of Central California, airborne observations, and remotely sensed NO2 tropospheric columns retrieved using the Ozone Monitoring Instrument (OMI). We explore controls on NOx concentrations at Chews Ridge, in Monterey County, such as the age of wildfire smoke plumes and wildfire intensity (i.e. burning vs. smoldering), as well as soil moisture and precipitation, which can lead to pulsed NOx fluxes. Most recently our in situ observations fortuitously captured differing amounts of the active plume of the Soberanes wildfire, which to date has burned >45,000 acres and is expected to continue partially contained through August 2016. Implications of these episodic sources of NOx on the regional ozone budget will be discussed.

Observational constraints for the source strengths, transport and partitioning of reactive nitrogen on regional and global scales

NASA Astrophysics Data System (ADS)

Bertram, Timothy Hugh

Reactive nitrogen (NOy) exerts control over the production of tropospheric ozone (O3) and the destruction of stratospheric O 3, plays an important role in the formation of secondary organic aerosol and represents a critical link between the atmosphere and biosphere. Accurate estimates of the spatial and temporal distribution of nitrogen oxide (NO x) emissions and their subsequent transport and chemical processing are critical to furthering our understanding of these processes. In this dissertation, several new approaches to understanding the role of nitrogen oxides in atmospheric chemistry are developed. Most of the observations and analyses presented are based on aircraft measurements used to describe and understand the distribution of NOx from the surface to the upper troposphere (UT) and to provide an understanding of the accuracy of satellite measurements. First, new experiments to establish the absolute accuracy and long term precision of the standards maintained at the National Institute of Standards and Technology (NIST) are described. These standards serve as the references upon which calibration of the instruments used to make atmospheric measurements of O3, nitric oxide (NO) and nitrogen dioxide (NO2) are based. Gas-phase titration of ozone with nitric oxide was used to show that the O3, NO and NO2 standards are self-consistent to within 1%. Prior experiments had only established these three to be self-consistent to 4%. Following this, the implementation of the Thermal Dissociation - Laser Induced Fluorescence (TD-LIF) Technique for measurements of NO2, total peroxy nitrates (SigmaPNs), total alkyl nitrates (SigmaANs) and nitric acid (HNO3) from an aircraft platform is discussed and the measurements obtained are compared directly to analogous measurements made aboard the same aircraft or different aircraft during in-flight comparisons. Detailed observations of the partitioning of reactive nitrogen in the upper troposphere, during a period of intense convective activity, are used to provide new and unique 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 direct measures of atmospheric rates present a challenge to our thinking about the processes governing UT O3 and its impact on climate. These measurements along with ones from periods without active convection are used to discuss the partitioning of NOy over the remote pacific during spring and over Continental North America during summer. The observations over the remote pacific reveal a strong role for SigmaPNs in the NOy budget and confirm earlier analyses and model predictions showing that the thermal dissociation of SigmaPNs is a significant NOx source to the remote Pacific. In contrast the vertical distribution and partitioning of reactive nitrogen over the North American continent during summer suggests a strong role for lightning initiated NOx production. Comparison to satellite observations during these experiments provides support for the accuracy of the satellite measurements. Finally, the utility of satellite measurements, which were examined in comparison to the aircraft measurements of NO2, to observe the spatial and temporal distribution of NOx emissions from fertilized agricultural soils is shown. These results demonstrate that satellite observations of NO 2 capture the short intense NOx pulses following fertilizer application and subsequent precipitation, and illustrate the strong potential for the use of satellite observations of NO2 in constraining NO x emissions sources.

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

NASA Technical Reports Server (NTRS)

Jeker, Dominique; Pfister, Lenny; Brunner, Dominik; Boccippio, Dennis J.; Pickering, Kenneth E.; Thompson, Anne M.; Wernli, Heini; Selkirk, Rennie B.; Kondo, Yutaka; Koike, Matoke;

Vertical Transport and Sources of Trace Gases in Thunderstorms around the World

NASA Astrophysics Data System (ADS)

Höller, H.; Fehr, T.; Huntrieser, H.; Gatzen, C.; Friedrich, K.; Seltmann, J.; May, P.; Potts, R.; Held, G.; Gomes-Held, A.

2003-04-01

Vertical transport processes in thunderstorms have become an issue of increasing interest in recent years. A better quantitative knowledge of the re-distribution of pollutants from the boundary layer to the upper troposphere is important for regional and global climate studies. The lightning NOx source has been investigated recently by field experiments mainly in mid-latitudes. Growing interest is now in the role of tropical thunderstorms for NOx production. The present paper highlights results from recent measurements and field campaigns and will introduce some future research plans. The LINOX and EULINOX campaign on lightning produced NOx (LNOx) performed in Southern Germany gave indication on the importance of intra-cloud lightning for total LNOx. This result was in agreement with measurements from the STERAO campaign in Colorado. The upcoming TROCCINOX campaign will focus on NOx production in tropical storms. For parameterised representation on lightning and NOx in numerical models dynamical and microphysical properties of thunderstorms are important. This also holds for assessments of vertical transport and trace gas re-distribution. During summer of 2002 the field campaign VERTIKATOR was focussing on orografically induced storms in Southern Germany. Detailed radar and airborne observations of thunderstorms were obtained and will be used for discussing the transport processes. Thunderstorm related field experiments in tropical regions have also been performed recently. During EMERALD II dual Doppler radar, lightning as well as airborne observations were obtained in the Darwin region in Northern Australia. Brazilian storms in the Bauru (Sao Paulo) region may often be accompanied by heavy flooding. Case studies from these regions will be used as a first step of completing the global picture of NOx transports and production.

Modeling of Particulate Emissions

DTIC Science & Technology

2011-12-01

Concern Local Air Quality - A Continuing Concern Ground Level Troposphere Ozone Layer Depletion • H2O Ozone Depletion (ice formation) 5 Modeling... Ozone & Smog Formation Health Effects Local Air Quality 33,000-58,000 ft• NOx •Traffic Growth • CO2* • NOx O3* • NOx Reduces CH4 • H2O Vapor...Particulates • SOx Cloud Formation Global Warming * - Greenhouse Gases Ozone Layer Depletion - Not an Immediate Concern Global Warming - An Emerging

A three-dimensional model of the global ammonia cycle

NASA Astrophysics Data System (ADS)

Dentener, Frank J.; Crutzen, Paul J.

1994-11-01

Using a three-dimensional (3-D) transport model of the troposphere, we calculated the global distributions of ammonia (NH3) and ammonium (NH4(+)), taking into account removal of NH3 on acidic aerosols, in liquid water clouds and by reaction with OH. Our estimated global 10 deg x 10 deg NH3 emission inventory of 45 Tg N-NH3/yr provides a reasonable agreement between calculated wet NH4(+) deposition and measurements and of measured and modeled NH4(+) in aerosols, although in Africa and Asia especially discrepancies exist. NH3 emissions from natural continental ecosystems were calculated applying a canopy compensation point and oceanic NH3 emissions were related to those of DMS (dimethylsulfide). In many regions of the earth, the pH found in rain and cloud water can be attributed to acidity derived from NO, SO2 and DMS emissions and alkalinity from NH3. In the remote lower troposphere, sulfate aerosols are calculated to be almost neutralized to ammonium sulfate (NH4)2SO4, whereas in the middle and upper troposphere, according to our calculations, the aerosol should be more acidic, as a result of the oxidation of DMS and SO2 throughout the troposphere and removal of NH3 on acidic aerosols at lower heights. Although the removal of NH3 by reaction with the OH radical is relatively slow, the intermediate NH2 radical can provide a substantial annual N2O source of 0.9(+0.9/-0.4) Tg, thus contributing by about 5% to estimated global N2O production. The oxidation by OH of NH3 from anthropogenic sources accounts for 10% of the estimated total anthropogenic sources of N2O. This source was not accounted for in previous studies, and is mainly located in the tropics, which have high NH3 and OH concentrations. Biomass burning plumes, containing high NO(x) and NH3 concentrations provide favorable conditions for gas phase N2O production. This source is probably underestimated in this model study, due to the coarse resolution of the 3-D model, and the rather low biomass burning NH3 and NO(x) emissions adopted. The estimate depends heavily on poorly known concentrations of NH3 (and NO(x)) in the tropics, and uncertainties in the rate constants of the reactions NH2 + NO2 yields N2O + H2O (R4), and NH2 + O3 yields NH2O + O2(R7).

Environmental Effects of Space Shuttle Solid Rocket Motor Exhaust Plumes

NASA Technical Reports Server (NTRS)

Hwang, B.; Pergament, H. S.

1976-01-01

The deposition of NOx and HCl in the stratosphere from the space shuttle solid rocket motors (SRM) and exhaust plume is discussed. A detailed comparison between stratospheric deposition rates using the baseline SRM propellant and an alternate propellant, which replaces ammonium perchlorate by ammonium nitrate, shows the total NOx deposition rate to be approximately the same for each propellant. For both propellants the ratio of the deposition rates of NOx to total chlorine-containing species is negligibly small. Rocket exhaust ground cloud transport processes in the troposphere are also examined. A brief critique of the multilayer diffusion models (presently used for predicting pollutant deposition in the troposphere) is presented, and some detailed cloud rise calculations are compared with data for Titan 3C launches. The results show that, when launch time meteorological data are used as input, the model can reasonably predict measured cloud stabilization heights.

Impact of Aircraft Emissions on Reactive Nitrogen over the North Atlantic Flight Corridor Region

NASA Technical Reports Server (NTRS)

Koike, M.; Kondo, Y.; Ikeda, H.; Gregory, G. L.; Anderson, B. E.; Sachse, G. W.; Blake, D.; Liu, S. C.; Singh, H. B.; Thompson, A.

1999-01-01

The impact of aircraft emissions on reactive nitrogen in the upper troposphere (UT) and lowermost stratosphere (LS) was estimated using the NO(y)-O3 correlation obtained during the SASS Ozone and NO(x) Experiment (SONEX) carried out over the US continent and North Atlantic Flight Corridor (NAFC) region in October and November 1997. To evaluate the large scale impact, we made a reference NO(y)-O3 relationship in air masses, upon which aircraft emissions were considered to have little impact. For this purpose, the integrated input of NO(x) from aircraft into an air mass along a 10-d back trajectory (DELTA-NO(y)) was calculated based on the ANCAT/EC2 emission inventory. The excess NO(y) (dNO(y)) was calculated from the observed NO(y) and the reference NO(y)-O3 relationship. As a result, a weak positive correlation was found between the dNO(y) and DELTA-NO(y), and dNO(y) and NO(x)/NO(y) values, while no positive correlation between the dNO(y) and CO values was found, suggesting that dNO(y) values can be used as a measure of the NO(x) input from aircraft emissions. The excess NO(y) values calculated from another NO(y)-O3 reference relationship made using in-situ CN data also agreed with these dNO(y) values, within the uncertainties. At the NAFC region (45 N - 60 N), the median value of dNO(y) in the troposphere increased with altitude above 9 km and reached 70 pptv (20% of NO(y)) at 11 km. The excess NO(x) was estimated to be about half of the dNO(y) values, corresponding to 30% of the observed NO(x) level. Higher dNO(y) values were generally found in air masses where O3 = 75 - 125 ppbv, suggesting a more pronounced effect around the tropopause. The median value of dNO(y) in the stratosphere at the NAFC region at 8.5 - 11.5 km was about 120 pptv. The higher dNO(y) values in the LS were probably due to the accumulated effect of aircraft emissions, given the long residence time of affected air in the LS. Similar dNO(y) values were also obtained in air masses sampled over the US continent.

Impact of aircraft emissions on reactive nitrogen over the North Atlantic Flight Corridor region

NASA Astrophysics Data System (ADS)

Koike, M.; Kondo, Y.; Ikeda, H.; Gregory, G. L.; Anderson, B. E.; Sachse, G. W.; Blake, D. R.; Liu, S. C.; Singh, H. B.; Thompson, A. M.; Kita, K.; Zhao, Y.; Sugita, T.; Shetter, R. E.; Toriyama, N.

2000-02-01

The impact of aircraft emissions on reactive nitrogen in the upper troposphere (UT) and lowermost stratosphere (LS) was estimated using the NOy-O3 correlation obtained during the Subsonic Assessment (SASS) Ozone and Nitrogen Oxide Experiment (SONEX) carried out over the U.S. continent and North Atlantic Flight Corridor (NAFC) region in October and November 1997. To evaluate the large-scale impact, we made a reference NOy-O3 relationship in air masses, upon which aircraft emissions were considered to have little impact. For this purpose, the integrated input of NOx from aircraft into an air mass along a 10-day back trajectory (ΔNOy) was calculated based on the Abatement of Nuisance Caused by Air Traffic/European Commission (ANCAT/EC2) emission inventory. The excess NOy (dNOy) was calculated from the observed NOy and the reference NOy-O3 relationship. As a result, a weak positive correlation was found between the dNOy and ΔNOy, and dNOy and NOx/NOy values, while no positive correlation between the dNOy and CO values was found, suggesting that dNOy values can be used as a measure of the NOx input from aircraft emissions. The excess NOy values calculated from another NOy-O3 reference relationship made using in situ condensation nuclei data also agreed with these dNOy values, within the uncertainties. At the NAFC region (45°N-60°N) the median value of dNOy in the troposphere increased with altitude above 9 km and reached 70 parts per trillion by volume (pptv) (20% of NOy) at 11 km. The excess NOx was estimated to be about half of the dNOy values, corresponding to 30% of the observed NOx level. Higher dNOy values were generally found in air masses where O3 = 75-125 ppbv, suggesting a more pronounced effect around the tropopause. The median value of dNOy in the stratosphere at the NAFC region at 8.5-11.5 km was about 120 pptv. The higher dNOy values in the LS were probably due to the accumulated effect of aircraft emissions, given the long residence time of affected air in the LS. Similar dNOy values were also obtained in air masses sampled over the U.S. continent.

Evaluating a Space-Based Indicator of Surface Ozone-NOx-VOC Sensitivity Over Midlatitude Source Regions and Application to Decadal Trends

EPA Science Inventory

Determining effective strategies for mitigating surface ozone (O3) pollution requires knowledge of the relative ambient concentrations of its precursors, NOx, and VOCs. The space-based tropospheric column ratio of formaldehyde to NO2 (FNR) has been used as an indicator to identif...

Trend analysis of tropospheric NO2 column density over East Asia during 2000-2010: multi-satellite observations and model simulations with the updated REAS emission inventory

NASA Astrophysics Data System (ADS)

Itahashi, S.; Uno, I.; Irie, H.; Kurokawa, J.; Ohara, T.

2013-04-01

Satellite observations of the tropospheric NO2 vertical column density (VCD) are closely correlated to surface NOx emissions and can thus be used to estimate the latter. In this study, the NO2 VCDs simulated by a regional chemical transport model with data from the updated Regional Emission inventory in ASia (REAS) version 2.1 were validated by comparison with multi-satellite observations (GOME, SCIAMACHY, GOME-2, and OMI) between 2000 and 2010. Rapid growth in NO2 VCD driven by expansion of anthropogenic NOx emissions was revealed above the central eastern China region, except during the economic downturn. In contrast, slightly decreasing trends were captured above Japan. The modeled NO2 VCDs using the updated REAS emissions reasonably reproduced the annual trends observed by multi-satellites, suggesting that the NOx emissions growth rate estimated by the updated inventory is robust. On the basis of the close linear relationship of modeled NO2 VCD, observed NO2 VCD, and anthropogenic NOx emissions, the NOx emissions in 2009 and 2010 were estimated. It was estimated that the NOx emissions from anthropogenic sources in China beyond doubled between 2000 and 2010, reflecting the strong growth of anthropogenic emissions in China with the rapid recovery from the economic downturn during late 2008 and mid-2009.

Establishing the Dependence of [HO2]/[OH] on Temperature, Halogen Loading, O3, and NO(x) Based on in Situ Measurements from the NASA ER-2

NASA Technical Reports Server (NTRS)

Lanzendorf, E. J.; Hanisco, T. F.; Wennberg, P. O.; Cohen, R. C.; Stimpfle, R. M.; Anderson, J. G.; Gao, R. S.; Margitan, J. J.; Bui, T. P.

2001-01-01

In situ observations of OH and HO2 from the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA), Stratospheric TRacers of Atmospheric Transport (STRAT), and Polar Ozone Loss in the Arctic Region in Summer (POLARIS) NASA ER-2 field campaigns are used to examine the partitioning of HO(x) in the lower stratosphere (tropopause to approx.21 km) and upper troposphere (approx.10 km to tropopause). These measurements span a latitude range from 70degS to 90degN and a variety of atmospheric conditions as a result of seasonal changes and altitude. The response of the observed [HO2]/[OH] to changes in temperature, [03], [CO], [NO], [CIO], and [BrO] is investigated. The measured ratio is accurately described (approx.+/-10%) by a steady-state model constrained by the measured mixing ratios of O3, CO, NO, CIO, and BrO, where the model is valid for conditions of HO(x) cycling much faster than HO(x) production and loss. The concentration of HO2 depends on [OH], which, to first order, has been observed to be a simple function of the solar zenith angle in the lower stratosphere. The partitioning between OH and HO2 is controlled by the local chemistry between the HO, radicals and O3, CO, NO, CIO, and BrO. The response of [HO(x)] to changes in [NO(x)] and [O3] is demonstrated. Further observations are necessary to illustrate the response of HO(x) to changes in halogen concentrations. A quantitative understanding of [HO2]/[OH] is important, since many of the reactions that control this ratio are directly involved in catalytic removal of O3 in the lower stratosphere and production of O3 in the upper troposphere.

Global financial crisis making a V-shaped fluctuation in NO2 pollution over the Yangtze River Delta

NASA Astrophysics Data System (ADS)

Du, Yin; Xie, Zhiqing

2017-04-01

The Yangtze River Delta (YRD), China's main cultural and economic center, has become one of the most seriously polluted areas in the world with respect to nitrogen oxides (NOx), owing to its rapid industrialization and urbanization, as well as substantial coal consumption. On the basis of nitrogen dioxide (NO2) density data from ozone monitoring instrument (OMI) and ground-based observations, the effects of industrial fluctuations due to the financial crisis on local NO2 pollution were quantitatively assessed. The results were as follows. (1) A distinct V-shaped fluctuation of major industrial products, thermal generating capacity, electricity consumption, and tropospheric NO2 densities was associated with the global financial crisis from May 2007 to December 2009, with the largest anomalies 1.5 times more than standard deviations at the height of the crisis period from November 2008 to February 2009. (2) Among all industrial sectors, thermal power plants were mainly responsible for fluctuations in local NO2 pollution during the crisis period. Thermal generating capacity had its greatest decrease of 12.10% at the height of the crisis compared with that during November 2007-February 2008, leading to local tropospheric NO2 density decreasing by 16.97%. As the crisis appeased, thermal generating capacity increased by 29.63% from November 2009 to February 2010, and tropospheric NO2 densities correspondingly increased by 30.07%. (3) Among all industrial sectors in the YRD, the thermal power sector has the greatest coal consumption of about 65.96%. A decline in thermal power of about 10% can induce a decrease of about 30% in NOx emissions and NO2 densities, meaning that a relative small fluctuation in industrial production can lead to a large decrease in tropospheric NO2 densities over industrially developed areas like the YRD region. Since electricity is mainly obtained from local coal-burning thermal plants without NOx-processing equipment, installing NOx-removal devices for all thermal power plants is an important and feasible way of controlling local NOx pollution at present.

Application of multi-constituent satellite data assimilation for KORUS-AQ

NASA Astrophysics Data System (ADS)

Miyazaki, K.; Sekiya, T.; Fu, D.; Bowman, K. W.; Kulawik, S. S.; Walker, T.; Takigawa, M.; Ogochi, K.; Gaubert, B.; Barré, J.; Emmons, L. K.

2017-12-01

Comprehensive tropospheric maps of multi-constituent fields at 1.1 degree resolution, provided by an assimilation of multiple satellite measurements of O3, CO, NO2, and HNO3 from multiple satellite (OMI, GOME-2, MOPITT, MLS, and AIRS) using an ensemble Kalman filter, are used to study variations in tropospheric composition over east Asia during KORUS-AQ. Assimilated model results for both direct ozone assimilations and assimilations of ozone precursors (NOx and CO) were compared to DC-8 aircraft observations, with significant improvements in model/aircraft comparisons for ozone (the negative model bias was reduced by up to 80 %), CO (by up to 90 %), OH (by up to 40 %), and NOx seen in both approaches. Corrections made to the precursor emissions (i.e., surface NOx and CO emissions), especially over eastern and central China and over South Korea, were important in reducing the negative bias of O3 and CO over South Korea. We obtained additional bias reductions from assimilation of multispectral retrievals of tropospheric ozone profiles from AIRS and OMI, especially for the middle troposphere ozone. Improved agreements with the ground-based measurements at remote sites over South Korea and western Japan suggest that the representation of long-range transport of polluted air is improved by data assimilation, as a result of the optimization of precursor emissions, mainly over China. The higher estimated NOx, by 60-90 % over South Korea and by 20-40 % over eastern China compared to bottom-up inventories, suggests an important underestimation of anthropogenic sources in the emission inventories in these areas. Additional bias reductions were obtained by assimilating the multispectral retrievals, especially for the middle troposphere O3. In the future, assimilating datasets from a new constellation of low Earth orbiting sounders (e.g., IASI, AIRS, CrIS, Sentinel-5p (TROPOMI), and Sentinel-5) and geostationary satellites (Sentinel-4, GEMS, and TEMPO) will provide more detailed knowledge of ozone and its precursors for east Asia and the entire globe. The data assimilation framework will also be used for chemical OSSE studies to evaluate and optimize the current and future observing systems.

The oxidation of isoprene in the troposphere - Mechanism and model calculations

NASA Technical Reports Server (NTRS)

Brewer, D. A.; Ogliaruso, M. A.; Augustsson, T. R.; Levine, J. S.

1984-01-01

Calculations have been performed for 15 deg N and 45 deg N latitude continental conditions using a one-dimensional, steady state photochemical model that incorporates a chemical mechanism describing the oxidation of isoprene by OH and O3 in the troposphere. At the higher latitude, anthropogenic hydrocarbon emission effects on NO(x) vertical profiles, as well as those of HNO3, overshadow isoprene emissions effects; at the lower latitude, reduced anthropogenic emissions and increased isoprene emissions respectively yield 26 and 4 percent increases in NO(x) and HNO3 column contents. It is suggested that a significant quantity of isoprene goes to the formation of longer carbon chain oxygenated organic species.

Tropospheric Ozone Change from 1980 to 2010 Dominated by Equatorward Redistribution of Emissions

NASA Technical Reports Server (NTRS)

Zhang, Yuqiang; Cooper, Owen R.; Gaudel, Audrey; Thompson, Anne M.; Nedelec, Philippe; Ogino, Shin-Ya; West, J. Jason

2016-01-01

Ozone is an important air pollutant at the surface, and the third most important anthropogenic greenhouse gas in the troposphere. Since 1980, anthropogenic emissions of ozone precursors methane, non-methane volatile organic compounds, carbon monoxide and nitrogen oxides (NOx) have shifted from developed to developing regions. Emissions have thereby been redistributed equatorwards, where they are expected to have a stronger effect on the tropospheric ozone burden due to greater convection, reaction rates and NOx sensitivity. Here we use a global chemical transport model to simulate changes in tropospheric ozone concentrations from 1980 to 2010, and to separate the influences of changes in the spatial distribution of global anthropogenic emissions of short-lived pollutants, the magnitude of these emissions, and the global atmospheric methane concentration. We estimate that the increase in ozone burden due to the spatial distribution change slightly exceeds the combined influences of the increased emission magnitude and global methane. Emission increases in Southeast, East and South Asia may be most important for the ozone change, supported by an analysis of statistically significant increases in observed ozone above these regions. The spatial distribution of emissions dominates global tropospheric ozone, suggesting that the future ozone burden will be determined mainly by emissions from low latitudes.

Simulating Changes in Tropospheric Composition, Aerosol Radiative Effects, and Atmospheric Deposition across the Northern Hemisphere: Contrasting Multi-Decadal Trends between Asia and North America

EPA Science Inventory

Significant and contrasting changes in tropospheric composition across the Northern hemisphere have occurred over the past two decades as a result of changing patterns of emissions of primary aerosol and gaseous precursors. During this period, SO2 and NOx emissions across the US...

Simultaneous assimilation of satellite NO2, O3, CO, and HNO3 data for the analysis of the tropospheric chemical composition

NASA Astrophysics Data System (ADS)

Miyazaki, K.; Eskes, H.; Sudo, K.

2012-04-01

Carbon monoxide (CO) and nitrogen oxides (NOx) play an important role in tropospheric chemistry through their influences on the ozone and hydroxyl radical (OH). The simultaneous optimization of various chemical components is expected to improve the emission inversion through the better description of the chemical feedbacks in the NOx- and CO-chemistry. This study aims to reproduce chemical composition distributions in the troposphere by combining information obtained from multiple satellite data sets. The emissions of CO and NOx, together with the 3D concentration fields of all forecasted chemical species in the global CTM CHASER have been simultaneously optimized using the ensemble Kalman filter (EnKF) data assimilation technique, and NO2, O3, CO, and HNO3 data obtained from OMI, TES, MOPITT, and MLS satellite measurements. The performance is evaluated against independent data from ozone sondes, aircraft measurements, GOME-2, and SCIAMACHY satellite data. Observing System Experiments (OSEs) have been carried out. These OSEs quantify the relative importance of each data set on constraining the emissions and concentrations. We confirmed that the simultaneous data assimilation improved the agreement with these independent data sets. The combined analysis of multiple data sets by means of advanced data assimilation system can provide a useful framework for the air quality research.

Upper Tropospheric Ozone Between Latitudes 60S and 60N Derived from Nimbus 7 TOMS/THIR Cloud Slicing

NASA Technical Reports Server (NTRS)

Ziemke, Jerald R.; Chandra, Sushil; Bhartia, P. K.

2002-01-01

This study evaluates the spatial distributions and seasonal cycles in upper tropospheric ozone (pressure range 200-500 hPa) from low to high latitudes (60S to 60N) derived from the satellite retrieval method called "Cloud Slicing." Cloud Slicing is a unique technique for determining ozone profile information in the troposphere by combining co-located measurements of cloud-top, pressure and above-cloud column ozone. For upper tropospheric ozone, co-located measurements of Nimbus 7 Total Ozone Mapping Spectrometer (TOMS) above-cloud column ozone, and Nimbus 7 Temperature Humidity Infrared Radiometer (THIR) cloud-top pressure during 1979-1984 were incorporated. In the tropics, upper tropospheric ozone shows year-round enhancement in the Atlantic region and evidence of a possible semiannual variability. Upper tropospheric ozone outside the tropics shows greatest abundance in winter and spring seasons in both hemispheres with largest seasonal and largest amounts in the NH. These characteristics are similar to lower stratospheric ozone. Comparisons of upper tropospheric column ozone with both stratospheric ozone and a proxy of lower stratospheric air mass (i.e., tropopause pressure) from National Centers for Environmental Prediction (NCEP) suggest that stratosphere-troposphere exchange (STE) may be a significant source for the seasonal variability of upper tropospheric ozone almost everywhere between 60S and 60N except in low latitudes around 10S to 25N where other sources (e.g., tropospheric transport, biomass burning, aerosol effects, lightning, etc.) may have a greater role.

Aerosol indirect effect on tropospheric ozone via lightning

NASA Astrophysics Data System (ADS)

Yuan, T.; Remer, L. A.; Bian, H.; Ziemke, J. R.; Albrecht, R. I.; Pickering, K. E.; Oreopoulos, L.; Goodman, S. J.; Yu, H.; Allen, D. J.

2012-12-01

Tropospheric ozone (O3) is a pollutant and major greenhouse gas and its radiative forcing is still uncertain. The unresolved difference between modeled and observed natural background O3 concentrations is a key source of the uncertainty. Here we demonstrate remarkable sensitivity of lightning activity to aerosol loading with lightning activity increasing more than 30 times per unit of aerosol optical depth over our study area. We provide observational evidence that indicates the observed increase in lightning activity is caused by the influx of aerosols from a volcano. Satellite data analyses suggest O3 is increased as a result of aerosol-induced increase in lightning and lightning produced NOx. Model simulations with prescribed lightning change corroborate the satellite data analysis. This aerosol-O3 connection is achieved via aerosol increasing lightning and thus lightning produced nitrogen oxides. This aerosol-lightning-ozone link provides a potential physical mechanism that may account for a part of the model-observation difference in background O3 concentration. More importantly, O3 production increase from this link is concentrated in the upper troposphere, where O3 is most efficient as a greenhouse gas. Both of these implications suggest a stronger O3 historical radiative forcing. This introduces a new pathway, through which increasing in aerosols from pre-industrial time to present day enhances tropospheric O3 production. Aerosol forcing thus has a warming component via its effect on O3 production. Sensitivity simulations suggest that 4-8% increase of tropospheric ozone, mainly in the tropics, is expected if aerosol-lighting-ozone link is parameterized, depending on the background emission scenario. We note, however, substantial uncertainties remain on the exact magnitude of aerosol effect on tropospheric O3 via lightning. The challenges for obtaining a quantitative global estimate of this effect are also discussed. Our results have significant implications for understanding past and projecting future tropospheric O3 forcing as well as wildfire changes and call for integrated investigations of the coupled aerosol-cloud-chemistry system.

Study Pollution Impacts on Upper-Tropospheric Clouds with Aura, CloudSat, and CALIPSO Data

NASA Technical Reports Server (NTRS)

Wu, Dong

2007-01-01

This viewgraph presentation reviews the impact of pollution on clouds in the Upper Troposphere. Using the data from the Aura Microwave Limb Sounder (MLS), CloudSat, CALIPSO the presentation shows signatures of pollution impacts on clouds in the upper troposphere. The presentation demonstrates the complementary sensitivities of MLS , CloudSat and CALIPSO to upper tropospheric clouds. It also calls for careful analysis required to sort out microphysical changes from dynamical changes.

Analysis of the GOES 6.7 micrometer channel observations during FIRE 2

NASA Technical Reports Server (NTRS)

Soden, B. J.; Ackerman, S. A.; Starr, David

1993-01-01

Clouds form in moist environments. FIRE Phase II Cirrus Implementation Plan (August, 1990) noted the need for mesoscale measurements of upper tropospheric water vapor content. These measurements are needed for initializing and verifying numerical weather prediction models and for describing the environment in which cirrus clouds develop and dissipate. Various instruments where deployed to measure the water vapor amounts of the upper troposphere during FIRE II (e.g. Raman lidar, CLASS sonds and new cryogenic frost hygrometer on-board aircraft). The formation, maintenance and dissipation of cirrus clouds involve the time variation of the water budget of the upper troposphere. The GOES 6.7 mu m radiance observations are sensitive to the upper tropospheric relative humidity, and therefore proved extremely valuable in planning aircraft missions during the field phase of FIRE II. Warm 6.7 mu m equivalent black body temperatures indicate a relatively dry upper troposphere and were associated with regions generally free of cirrus clouds. Regions that were colder, implying more moisture was available may or may not have had cirrus clouds present. Animation of a time sequence of 6.7 mu m images was particularly useful in planning various FIRE missions. The 6.7 mu m observations can also be very valuable in the verification of model simulations and describing the upper tropospheric synoptic conditions. A quantitative analysis of the 6.7 mu m measurement is required to successfully incorporate these satellite observations into describing the upper tropospheric water vapor budget. Recently, Soden and Bretherton (1993) have proposed a method of deriving an upper tropospheric humidity based on observations from the GOES 6.7 mu m observations. The method is summarized in the next section. In their paper they compare their retrieval method to radiance simulations. Observations were also compared to ECMWF model output to assess the model performance. The FIRE experiment provides a unique opportunity to further verify the GOES upper tropospheric relative humidity retrieval scheme by providing (1) aircraft observations to cross-validate the calibration of the GOES 6.7 mu m channel, (2) accurate upper tropospheric water vapor concentrations for verification, and (3) veritical variability of upper tropospheric water vapor.

Measurements of Nitric Acid and Aerosol Species Aboard the NASA DC-8 Aircraft During the SASS OZone and Nitrogen Oxide Experiment (SONEX)

NASA Technical Reports Server (NTRS)

Talbot, Robert W.; Dibb, Jack E.

1999-01-01

The SASS Ozone and Nitrogen Oxides Experiment (SONEX) over the north Atlantic during October/November 1997 offered an excellent opportunity to examine the budget of total reactive nitrogen (NO(y)) in the upper troposphere (8 - 12 km altitude). The median measured NO(y) mixing ratio was 425 parts per trillion by volume (pptv). Two different methods were used to measure HNO3: (1) the mist chamber technique and, (2) chemical ionization mass spectrometry. Two merged data sets using these HNO3 measurements were used to calculate NO(y) by summing the reactive nitrogen species (a combination of measured plus modeled results) and comparing the resultant values to measured NO(y) (gold catalytic reduction method). Both comparisons showed good agreement in the two quantities (slope greater than 0.9 and r(sup 2) greater than 0.9). Thus, the total reactive nitrogen budget in the upper troposphere over the North Atlantic can be explained in a general manner as a simple mixture of NO(x). (NO + NO2), HNO3, and PAN. Median values of NO(x)/NO(y) were approx. = 0.25, HNO3/NO(y) approx. = 0.35 and PAN/NO(y) approx. = 0.17. Particulate NO3 and alkyl nitrates together composed less than 10% of NO(y), while model estimated HNO4 averaged 12%.

Extratropical Influence of Upper Tropospheric Water Vapor on Greenhouse Warming

NASA Technical Reports Server (NTRS)

Hu, H.; Liu, W.

1998-01-01

The purpose of this paper is to re-examine the impact of upper tropospheric water vapor on greenhouse warming in midlatitudes by analyzing the recent observations of the upper tropospheric water vapor from the Microwave Limb Sounder (MLS) on the Upper Atmosphere Research Satellite (UARS), in conjuction with other space-based measurement and model simulation products.

Relationship between VOC and NOx emissions and chemical production of tropospheric ozone in the Aburrá Valley (Colombia).

PubMed

Toro, María Victoria; Cremades, Lázaro V; Calbó, Josep

2006-10-01

Relationship between volatile organic compounds (VOC) and nitrogen oxides (NOx) emissions and the chemical production of tropospheric ozone is studied through mathematical simulation. The study is applied to the Aburrá Valley, in the Colombian Andes, which is a practically unknown area from the point of view of ozone formation. The model used for this application is the European modelling of atmospheric constituents (EUMAC) zooming model (EZM) which consists of a mesoscale prognostic model (MEMO, mesoscale meteorological model) and a chemical reaction model (MUSE, multiscale for the atmospheric dispersion of reactive species), coupled to the chemical mechanism EMEP (European monitoring and evaluation program). The analysis is performed for a real episode that was characterized by high ozone production and that happened during the 23rd and 24th December, 1999 in Medellín (Colombia). From this real scenario, a sensitivity analysis has been carried out in order to assess the influence of VOC and NOx amounts on ozone production and to extract some conclusions for future ozone abatement policies in Andean regions. As far as ozone air quality is concerned, it is shown that in order to keep current levels the emphasis must be put to avoid increasing NOx emissions, or alternatively, to augment VOC emissions in order to have a high VOC/NOx ratio.

Estimating NOx emissions and surface concentrations at high spatial resolution using OMI

NASA Astrophysics Data System (ADS)

Goldberg, D. L.; Lamsal, L. N.; Loughner, C.; Swartz, W. H.; Saide, P. E.; Carmichael, G. R.; Henze, D. K.; Lu, Z.; Streets, D. G.

2017-12-01

In many instances, NOx emissions are not measured at the source. In these cases, remote sensing techniques are extremely useful in quantifying NOx emissions. Using an exponential modified Gaussian (EMG) fitting of oversampled Ozone Monitoring Instrument (OMI) NO2 data, we estimate NOx emissions and lifetimes in regions where these emissions are uncertain. This work also presents a new high-resolution OMI NO2 dataset derived from the NASA retrieval that can be used to estimate surface level concentrations in the eastern United States and South Korea. To better estimate vertical profile shape factors, we use high-resolution model simulations (Community Multi-scale Air Quality (CMAQ) and WRF-Chem) constrained by in situ aircraft observations to re-calculate tropospheric air mass factors and tropospheric NO2 vertical columns during summertime. The correlation between our satellite product and ground NO2 monitors in urban areas has improved dramatically: r2 = 0.60 in new product, r2 = 0.39 in operational product, signifying that this new product is a better indicator of surface concentrations than the operational product. Our work emphasizes the need to use both high-resolution and high-fidelity models in order to re-calculate vertical column data in areas with large spatial heterogeneities in NOx emissions. The methodologies developed in this work can be applied to other world regions and other satellite data sets to produce high-quality region-specific emissions estimates.

Effects of Aircraft Wake Dynamics on Measured and Simulated NO(x) and HO(x) Wake Chemistry. Appendix B

NASA Technical Reports Server (NTRS)

Lewellen, D. C.; Lewellen, W. S.

2001-01-01

High-resolution numerical large-eddy simulations of the near wake of a B757 including simplified NOx and HOx chemistry were performed to explore the effects of dynamics on chemistry in wakes of ages from a few seconds to several minutes. Dilution plays an important basic role in the NOx-O3 chemistry in the wake, while a more interesting interaction between the chemistry and dynamics occurs for the HOx species. These simulation results are compared with published measurements of OH and HO2 within a B757 wake under cruise conditions in the upper troposphere taken during the Subsonic Aircraft Contrail and Cloud Effects Special Study (SUCCESS) mission in May 1996. The simulation provides a much finer grained representation of the chemistry and dynamics of the early wake than is possible from the 1 s data samples taken in situ. The comparison suggests that the previously reported discrepancy of up to a factor of 20 - 50 between the SUCCESS measurements of the [HO2]/[OH] ratio and that predicted by simplified theoretical computations is due to the combined effects of large mixing rates around the wake plume edges and averaging over volumes containing large species fluctuations. The results demonstrate the feasibility of using three-dimensional unsteady large-eddy simulations with coupled chemistry to study such phenomena.

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

NASA Technical Reports Server (NTRS)

Bucsela, Eric; Pickering, Kenneth E.; Huntemann, Tabitha; Cohen, Ronald; Perring, Anne; Gleason, James; Blakeslee, Richard; Navarro, Dylana Vargas; Segura, Ileana Mora; Hernandez, Alexia Pacheco;

Lightning NOx emissions over the USA constrained by TES ozone observations and the GEOS-Chem model

NASA Astrophysics Data System (ADS)

Jourdain, L.; Kulawik, S. S.; Worden, H. M.; Pickering, K. E.; Worden, J.; Thompson, A. M.

2010-01-01

Improved estimates of NOx from lightning sources are required to understand tropospheric NOx and ozone distributions, the oxidising capacity of the troposphere and corresponding feedbacks between chemistry and climate change. In this paper, we report new satellite ozone observations from the Tropospheric Emission Spectrometer (TES) instrument that can be used to test and constrain the parameterization of the lightning source of NOx in global models. Using the National Lightning Detection (NLDN) and the Long Range Lightning Detection Network (LRLDN) data as well as the HYPSLIT transport and dispersion model, we show that TES provides direct observations of ozone enhanced layers downwind of convective events over the USA in July 2006. We find that the GEOS-Chem global chemistry-transport model with a parameterization based on cloud top height, scaled regionally and monthly to OTD/LIS (Optical Transient Detector/Lightning Imaging Sensor) climatology, captures the ozone enhancements seen by TES. We show that the model's ability to reproduce the location of the enhancements is due to the fact that this model reproduces the pattern of the convective events occurrence on a daily basis during the summer of 2006 over the USA, even though it does not well represent the relative distribution of lightning intensities. However, this model with a value of 6 Tg N/yr for the lightning source (i.e.: with a mean production of 260 moles NO/Flash over the USA in summer) underestimates the intensities of the ozone enhancements seen by TES. By imposing a production of 520 moles NO/Flash for lightning occurring in midlatitudes, which better agrees with the values proposed by the most recent studies, we decrease the bias between TES and GEOS-Chem ozone over the USA in July 2006 by 40%. However, our conclusion on the strength of the lightning source of NOx is limited by the fact that the contribution from the stratosphere is underestimated in the GEOS-Chem simulations.

Upper-Tropospheric Synoptic-Scale Waves. Part II: Maintenance and Excitation of Quasi Modes.

NASA Astrophysics Data System (ADS)

Rivest, Chantal; Farrell, Brian F.

1992-11-01

In a preceding paper a simple dynamical model for the maintenance of upper-tropospheric waves was proposed: the upper-level Eady normal modes. In this paper it is shown that these modes have counterparts in basic states with positive tropospheric gradients of potential vorticity, and that these counterparts can be maintained and excited on time scales consistent with observations.In the presence of infinitesimal positive tropospheric gradients of potential vorticity, the upper-level normal-mode solutions no longer exist. That the normal-mode solution disappears when gradients are infinitesimal represents an apparent singularity and challenges the interpretation of upper-level synoptic-scale waves as related to the upper-level Eady normal modes. What happens to the upper-level modal solution in the presence of tropospheric gradients of potential vorticity is examined in a series of initial-value experiments. Our results show that they become slowly decaying quasi modes. Mathematically the quasi modes consist of a superposition of singular modes sharply peaked in the phase speed domain, and their decay proceeds as the modes interfere with one another. We repeat these experiments in basic states with a smooth tropopause in the presence of tropospheric and stratospheric gradients, and similar results are obtained.Following a previous study by Farrell, a class of near-optimal initial conditions for the excitation of upper-level waves is identified. The initial conditions consist of upper-tropospheric disturbances that lean against the shear. They strongly excite upper-level waves not only in the absence of tropospheric potential vorticity gradients, but also in their presence. This result is important mathematically since it suggests that quasi modes are as likely to emerge from favorably configured initial disturbances as true normal modes, although the excitation is followed by a slow decay.

Dynamics and composition of the Asian summer monsoon anticyclone

NASA Astrophysics Data System (ADS)

Gottschaldt, Klaus-Dirk; Schlager, Hans; Baumann, Robert; Sinh Cai, Duy; Eyring, Veronika; Graf, Phoebe; Grewe, Volker; Jöckel, Patrick; Jurkat-Witschas, Tina; Voigt, Christiane; Zahn, Andreas; Ziereis, Helmut

2018-04-01

This study places HALO research aircraft observations in the upper-tropospheric Asian summer monsoon anticyclone (ASMA) into the context of regional, intra-annual variability by hindcasts with the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. The observations were obtained during the Earth System Model Validation (ESMVal) campaign in September 2012. Observed and simulated tracer-tracer relations reflect photochemical O3 production as well as in-mixing from the lower troposphere and the tropopause layer. The simulations demonstrate that tropospheric trace gas profiles in the monsoon season are distinct from those in the rest of the year, and the measurements reflect the main processes acting throughout the monsoon season. Net photochemical O3 production is significantly enhanced in the ASMA, where uplifted precursors meet increased NOx, mainly produced by lightning. An analysis of multiple monsoon seasons in the simulation shows that stratospherically influenced tropopause layer air is regularly entrained at the eastern ASMA flank and then transported in the southern fringe around the interior region. Radial transport barriers of the circulation are effectively overcome by subseasonal dynamical instabilities of the anticyclone, which occur quite frequently and are of paramount importance for the trace gas composition of the ASMA. Both the isentropic entrainment of O3-rich air and the photochemical conversion of uplifted O3-poor air tend to increase O3 in the ASMA outflow.

Toward a more physical representation of precipitation scavenging in global chemistry models: cloud overlap and ice physics and their impact on tropospheric ozone

NASA Astrophysics Data System (ADS)

Neu, J. L.; Prather, M. J.

2011-08-01

Uptake and removal of soluble trace gases and aerosols by precipitation represents a major uncertainty in the processes that control the vertical distribution of atmospheric trace species. Model representations of precipitation scavenging vary greatly in their complexity, and most are divorced from the physics of precipitation formation and transformation. Here, we describe a new large-scale precipitation scavenging algorithm, developed for the UCI chemistry-transport model (UCI-CTM), that represents a step toward a more physical treatment of scavenging through improvements in the formulation of the removal in sub-gridscale cloudy and ambient environments and their overlap within the column as well as ice phase uptake of soluble species. The UCI algorithm doubles the lifetime of HNO3 in the upper troposphere relative to a scheme with commonly made assumptions about cloud overlap and ice uptake, and provides better agreement with HNO3 observations. We find that the process of ice phase scavenging of HNO3 is a critical component of the tropospheric O3 budget, but that differences in the formulation of ice phase removal, while generating large relative differences in HNO3 abundance, have little impact on NOx and O3. The O3 budget is much more sensitive to the lifetime of HNO4, highlighting the need for better understanding of its interactions with ice and for additional observational constraints.

Toward a more physical representation of precipitation scavenging in global chemistry models: cloud overlap and ice physics and their impact on tropospheric ozone

NASA Astrophysics Data System (ADS)

Neu, J. L.; Prather, M. J.

2012-04-01

Uptake and removal of soluble trace gases and aerosols by precipitation represents a major uncertainty in the processes that control the vertical distribution of atmospheric trace species. Model representations of precipitation scavenging vary greatly in their complexity, and most are divorced from the physics of precipitation formation and transformation. Here, we describe a new large-scale precipitation scavenging algorithm, developed for the UCI chemistry-transport model (UCI-CTM), that represents a step toward a more physical treatment of scavenging through improvements in the formulation of the removal in sub-gridscale cloudy and ambient environments and their overlap within the column as well as ice phase uptake of soluble species. The UCI algorithm doubles the lifetime of HNO3 in the upper troposphere relative to a scheme with commonly used fractional cloud cover assumptions and ice uptake determined by Henry's Law and provides better agreement with HNO3 observations. We find that the process of ice phase scavenging of HNO3 is a critical component of the tropospheric O3 budget, but that NOx and O3 mixing ratios are relatively insensitive to large differences in the removal rate. Ozone abundances are much more sensitive to the lifetime of HNO4, highlighting the need for better understanding of its interactions with ice and for additional observational constraints.

Distribution and fate of selected oxygenated organic species in the troposphere and lower stratosphere over the Atlantic

NASA Astrophysics Data System (ADS)

Singh, H.; Chen, Y.; Tabazadeh, A.; Fukui, Y.; Bey, I.; Yantosca, R.; Jacob, D.; Arnold, F.; Wohlfrom, K.; Atlas, E.; Flocke, F.; Blake, D.; Blake, N.; Heikes, B.; Snow, J.; Talbot, R.; Gregory, G.; Sachse, G.; Vay, S.; Kondo, Y.

2000-02-01

A large number of oxygenated organic chemicals (peroxyacyl nitrates, alkyl nitrates, acetone, formaldehyde, methanol, methylhydroperoxide, acetic acid and formic acid) were measured during the 1997 Subsonic Assessment (SASS) Ozone and Nitrogen Oxide Experiment (SONEX) airborne field campaign over the Atlantic. In this paper, we present a first picture of the distribution of these oxygenated organic chemicals (Ox-organic) in the troposphere and the lower stratosphere, and assess their source and sink relationships. In both the troposphere and the lower stratosphere, the total atmospheric abundance of these oxygenated species (ΣOx-organic) nearly equals that of total nonmethane hydrocarbons (ΣNMHC), which have been traditionally measured. A sizable fraction of the reactive nitrogen (10-30%) is present in its oxygenated organic form. The organic reactive nitrogen fraction is dominated by peroxyacetyl nitrate (PAN), with alkyl nitrates and peroxypropionyl nitrate (PPN) accounting for <5% of total NOy. Comparison of observations with the predictions of the Harvard three-dimensional global model suggests that in many key areas (e.g., formaldehyde and peroxides) substantial differences between measurements and theory are present and must be resolved. In the case of CH3OH, there appears to be a large mismatch between atmospheric concentrations and estimated sources, indicating the presence of major unknown removal processes. Instrument intercomparisons as well as disagreements between observations and model predictions are used to identify needed improvements in key areas. The atmospheric chemistry and sources of this group of chemicals is poorly understood even though their fate is intricately linked with upper tropospheric NOx and HOx cycles.

Global Free-tropospheric NO2 Abundances Derived Using a Cloud Slicing Technique from AURA OMI

NASA Technical Reports Server (NTRS)

Choi, S.; Joiner, J.; Choi, Y.; Duncan, B.N.; Vasilkov, A.; Krotkov, N.; Bucsela, E.J.

2014-01-01

We derive free-tropospheric NO2 volume mixing ratios (VMRs) by applying a cloud-slicing technique to data from the Ozone Monitoring Instrument (OMI) on the Aura satellite. In the cloud-slicing approach, the slope of the above-cloud NO2 column versus the cloud scene pressure is proportional to the NO2 VMR. In this work, we use a sample of nearby OMI pixel data from a single orbit for the linear fit. The OMI data include cloud scene pressures from the rotational-Raman algorithm and above-cloud NO2 vertical column density (VCD) (defined as the NO2 column from the cloud scene pressure to the top of the atmosphere) from a differential optical absorption spectroscopy (DOAS) algorithm. We compare OMI-derived NO2 VMRs with in situ aircraft profiles measured during the NASA Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in 2006. The agreement is generally within the estimated uncertainties when appropriate data screening is applied. We then derive a global seasonal climatology of free-tropospheric NO2 VMR in cloudy conditions. Enhanced NO2 in the free troposphere commonly appears near polluted urban locations where NO2 produced in the boundary layer may be transported vertically out of the boundary layer and then horizontally away from the source. Signatures of lightning NO2 are also shown throughout low and middle latitude regions in summer months. A profile analysis of our cloud-slicing data indicates signatures of lightning-generated NO2 in the upper troposphere. Comparison of the climatology with simulations from the global modeling initiative (GMI) for cloudy conditions (cloud optical depth less than10) shows similarities in the spatial patterns of continental pollution outflow. However, there are also some differences in the seasonal variation of free-tropospheric NO2 VMRs near highly populated regions and in areas affected by lightning-generated NOx.

Assessing the quality of humidity measurements from global operational radiosonde sensors

NASA Astrophysics Data System (ADS)

Moradi, Isaac; Soden, Brian; Ferraro, Ralph; Arkin, Phillip; Vömel, Holger

2013-07-01

The quality of humidity measurements from global operational radiosonde sensors in upper, middle, and lower troposphere for the period 2000-2011 were investigated using satellite observations from three microwave water vapor channels operating at 183.31±1, 183.31±3, and 183.31±7 GHz. The radiosonde data were partitioned based on sensor type into 19 classes. The satellite brightness temperatures (Tb) were simulated using radiosonde profiles and a radiative transfer model, then the radiosonde simulated Tb's were compared with the observed Tb's from the satellites. The surface affected Tb's were excluded from the comparison due to the lack of reliable surface emissivity data at the microwave frequencies. Daytime and nighttime data were examined separately to see the possible effect of daytime radiation bias on the sonde data. The error characteristics among different radiosondes vary significantly, which largely reflects the differences in sensor type. These differences are more evident in the mid-upper troposphere than in the lower troposphere, mainly because some of the sensors stop responding to tropospheric humidity somewhere in the upper or even in the middle troposphere. In the upper troposphere, most sensors have a dry bias but Russian sensors and a few other sensors including GZZ2, VZB2, and RS80H have a wet bias. In middle troposphere, Russian sensors still have a wet bias but all other sensors have a dry bias. All sensors, including Russian sensors, have a dry bias in lower troposphere. The systematic and random errors generally decrease from upper to lower troposphere. Sensors from China, India, Russia, and the U.S. have a large random error in upper troposphere, which indicates that these sensors are not suitable for upper tropospheric studies as they fail to respond to humidity changes in the upper and even middle troposphere. Overall, Vaisala sensors perform better than other sensors throughout the troposphere exhibiting the smallest systematic and random errors. Because of the large differences between different radiosonde humidity sensors, it is important for long-term trend studies to only use data measured using a single type of sensor at any given station. If multiple sensor types are used then it is necessary to consider the bias between sensor types and its possible dependence on humidity and temperature.

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

NASA Technical Reports Server (NTRS)

Duncan, Bryan N.; Yoshida, Yasuko; Sillman, Sanford; Retscher, Christian; Pickering, Kenneth E.; Martin, Randall V.; Celarier, Edward A.

2009-01-01

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.

Atmospheric peroxyacetyl nitrate measurements over the Brazilian Amazon Basin during the wet season - Relationships with nitrogen oxides and ozone

NASA Technical Reports Server (NTRS)

Singh, H. B.; Herlth, D.; O'Hara, D.; Salas, L.; Torres, A. L.; Gregory, G. L.; Sachse, G. W.

1990-01-01

An analysis is presented on the distribution and variability of PAN as well as its relationship with measured chemical and meteorological parameters. The chemicals of most interest for which measurements were available are PAN, NO(x), O3, CO, and C2Cl4. PAN was measured by the electron capture gas chromatographic technique, and the technique for calibrations and measurements are detailed. Data show that significant concentrations of PAN (5-125 ppt) are present during the wet season and this PAN is 1-5 times more abundant than NO(x). PAN levels at different atmospheric locations are discussed, and it is noted that PAN shows evidence of a possible latitudinal gradient in the free troposphere, with values falling rapidly from the northern midlatitudes toward the equator. High correlations between O3 and PAN levels suggest that nonmethane hydrocarbons may contribute significantly to high O3 in the free troposphere. Evidence indicates that virtually all of the NO(x) above 4 km could result from PAN decomposition.

Investigating isotopic signatures of atmospheric nitrous acid (HONO)

NASA Astrophysics Data System (ADS)

Chai, J.; Miller, D. J.; Hastings, M. G.

2016-12-01

Nitrous acid (HONO) is an important reactive nitrogen species that can be easily photolyzed to nitrogen oxide and hydroxyl radical in the troposphere. HONO greatly influences atmospheric oxidation capacity, affecting the formation of tropospheric ozone (O3) and secondary aerosol. Recent studies have indicated that in addition to heterogeneous NOx reactions, biomass burning, soil emission and photolysis of nitric acid (HNO3) on surfaces (e.g. aerosol particles and soot) are also important sources of HONO. However, these sources have not yet been well constrained. The stable isotope ratios in nitrate have been successfully used to trace NOx sources and oxidation chemistry in the atmosphere. Can the isotopic signatures of HONO be used to trace NOx oxidation and renoxification pathways? For this purpose, we have built an annular denuder HONO collection system for the stable isotope study of HONO. Preliminary tests show successful collection and recovery of HONO synthesized in our lab. Nitrogen and oxygen isotopic analysis of the recovered HONO also shows consistent isotopic signatures. Results from field applications of this method in near road and on road environments, agricultural settings, and laboratory based biomass burns will be presented.

Tropospheric ozone using an emission tagging technique in the CAM-Chem and WRF-Chem models

NASA Astrophysics Data System (ADS)

Lupascu, A.; Coates, J.; Zhu, S.; Butler, T. M.

2017-12-01

Tropospheric ozone is a short-lived climate forcing pollutant. High concentration of ozone can affect human health (cardiorespiratory and increased mortality due to long-term exposure), and also it damages crops. Attributing ozone concentrations to the contributions from different sources would indicate the effects of locally emitted or transported precursors on ozone levels in specific regions. This information could be used as an important component of the design of emissions reduction strategies by indicating which emission sources could be targeted for effective reductions, thus reducing the burden of ozone pollution. Using a "tagging" approach within the CAM-Chem (global) and WRF-Chem (regional) models, we can quantify the contribution of individual emission of NOx and VOC precursors on air quality. Hence, when precursor emissions of NOx are tagged, we have seen that the largest contributors on ozone levels are the anthropogenic sources, while in the case of precursor emissions of VOCs, the biogenic sources and methane account for more than 50% of ozone levels. Further, we have extended the NOx tagging method in order to investigate continental source region contributions to concentrations of ozone over various receptor regions over the globe, with a zoom over Europe. In general, summertime maximum ozone in most receptor regions is largely attributable to local emissions of anthropogenic NOx and biogenic VOC. During the rest of the year, especially during springtime, ozone in most receptor regions shows stronger influences from anthropogenic emissions of NOx and VOC in remote source regions.

LNOx Estimates Directly from LIS Data

NASA Astrophysics Data System (ADS)

Koshak, W. J.; Vant-hull, B.; McCaul, E.

2014-12-01

Nitrogen oxides (NOx = NO + NO2) are known to indirectly influence climate since they affect the concentration of both atmospheric ozone (O3) and hydroxyl radicals (OH). In addition, lightning NOx (LNOx) is the most important source of NOx in the upper troposphere (particularly in the tropics). It is difficult to estimate LNOx because it is not easy to make measurements near the lightning channel, and the various NOx-producing mechanisms within a lightning flash are not fully understood. A variety of methods have been used to estimate LNOx production [e.g., in-situ observations, combined ground-based VHF lightning mapping and VLF/LF lightning locating observations, indirect retrievals using satellite Ozone Monitoring Instrument (OMI) observations, theoretical considerations, laboratory spark measurements, and rocket triggered lightning measurements]. The present study introduces a new approach for estimating LNOx that employs Lightning Imaging Sensor (LIS) data. LIS optical measurements are used to directly estimate the total energy of a flash; the total flash energy is then converted to LNOx production (in moles) by multiplying by a thermo-chemical yield. Hence, LNOx estimates on a flash-by-flash basis are obtained. A Lightning NOx Indicator (LNI) is computed by summing up the LIS-derived LNOx contributions from a region over a particular analysis period. Larger flash optical areas are consistent with longer channel length and/or more energetic channels, and hence more NOx production. Brighter flashes are consistent with more energetic channels, and hence more NOx production. The location of the flash within the thundercloud and the optical scattering characteristics of the thundercloud are complicating factors. LIS data for the years 2003-2013 were analyzed, and geographical plots of the time-evolution of the LNI over the southern tier states (i.e. upto 38o N) of CONUS were determined. Overall, the LNI trends downward over the 11 yr analysis period. The LNI has been added to the list of indicators presently provided by a sustaining assessment tool developed at the NASA Marshall Space Flight Center (MSFC) for monitoring lightning/climate interactions over the United States, as part of the National Climate Assessment (NCA) program.

Relationship of peroxyacetyl nitrate to active and total odd nitrogen at northern high latitudes - Influence of reservoir species on NO(x) and O3

NASA Technical Reports Server (NTRS)

Singh, H. B.; Herlth, D.; O'Hara, D.; Zahnle, K.; Bradshaw, J. D.; Sandholm, S. T.; Talbot, R.; Crutzen, P. J.; Kanakidou, M. A.

1992-01-01

The partitioning of relative nitrogen in the Arctic and the sub-Arctic troposphere based on measurements conducted during the 1988 Arctic Boundary Layer Expedition (ABLE 3A) is described. The first set of comprehensive odd nitrogen and O3 measurements from the Arctic/sub-Arctic free troposphere shows that a highly aged air mass that has persisted under very cold conditions is present. A large fraction of the odd nitrogen appears to be present in the form of reservoir species such as PAN. Significant quantities of as yet unknown reactive nitrogen species, such as complex alkyl nitrates and pernitrates, are expected to be present. Together with PAN, these nitrate and pernitrate reservoir species could control the entire NO(x) availability of the high-latitude troposphere and in turn influence the O3 photochemistry of the region. The role of PAN in influencing the O3 reservoir is shown to be important and may be responsible for the increasing O3 temporal trend observed at high latitudes.

Observed OH and HO2 concentrations in the upper troposphere inside and outside of Asian monsoon influenced air.

NASA Astrophysics Data System (ADS)

Marno, D. R.; Künstler, C.; Hens, K.; Tatum Ernest, C.; Broch, S.; Fuchs, H.; Martinez, M.; Bourtsoukidis, E.; Williams, J.; Holland, F.; Hofzumahaus, A.; Tomsche, L.; Fischer, H.; Klausner, T.; Schlager, H.; Eirenschmalz, L.; Stratmann, G.; Stock, P.; Ziereis, H.; Roiger, A.; Bohn, B.; Zahn, A.; Wahner, A.; Lelieveld, J.; Harder, H.

2016-12-01

The Asian monsoon convectively transports pollutants like volatile organic compounds (VOCs), NOx, and SO2 from the boundary layer over South Asia into the upper troposphere where they can potentially enter the stratosphere, or be dispersed globally. Therefore, it is crucial to understand the oxidizing capacity of this system regarding the rate of aerosol formation, and conversion of pollutants into compounds that have much shorter atmospheric lifetimes. OH plays a central role in this oxidation process. During the OMO-ASIA campaign in the summer of 2015, OH and HO2 were measured onboard the High Altitude Long-Range (HALO) Research Aircraft. Two laser-induced fluorescence instruments based on the fluorescence assay by gas expansion technique (LIF-FAGE) had been deployed, the AIR-LIF instrument from Forschungszentrum Jülich GmbH and the HORUS instrument from the Max Planck Institute for Chemistry, Mainz. To measure the chemical background of OH potentially produced inside the HORUS instrument from highly oxidized VOCs, atmospheric OH is scavenged by an Inlet Pre-injector (IPI) system. This was the first time an IPI system was implemented within an airborne LIF-FAGE instrument measuring OH and HO2. Throughout this campaign OH and HO2 were measured at 12 to 15km within the Asian monsoon anticyclone. These measurements have been contrasted by probing air outside the anticyclone in air masses influenced by North American emissions, and in very clean air masses originated from the southern hemisphere.

Scale Invariance of High Altitude Aircraft Observations in the Upper Troposphere and Lower Stratosphere at Tropical and Subtropical Latitudes

NASA Technical Reports Server (NTRS)

Mahoney, M.; Hovde, S.; Kelly, K.; Proffitt, M.; Richard, E.; Thompson, T.; Tuck, A.

2000-01-01

Exchange between the upper tropical troposphere and the lower troposphere is considered by examining high altitude aircraft observations of water, ozone, methane, wind and temperature for scale invariance.

Future changes in tropospheric ozone under Representative Concentration Pathways (RCPs)

NASA Astrophysics Data System (ADS)

Kawase, Hiroaki; Nagashima, Tatsuya; Sudo, Kengo; Nozawa, Toru

2011-03-01

We consider future changes in tropospheric ozone based on the Representative Concentration Pathways (RCPs), which are new emission and concentration scenarios for the 5th coupled model intercomparison project. In contrast to the SRES scenarios, all the RCP scenarios assume an emission reduction of NOx by the late 21st Century that has the potential to achieve tropospheric ozone reduction. However, increasing radiative forcing (RF) due to greenhouse gases and changes in CH4 concentration also contribute to differences in the tropospheric ozone distribution among RCP scenarios. In the RCP4.5 and RCP6.0, assuming the stabilization of RF, the increase in tropospheric ozone due to enhanced residual circulation is cancelled out by the ozone reduction due to ozone precursor reductions. In contrast, in the RCP8.5, assuming increasing RF even after 2100, further enhanced residual circulation and significant increase in CH4 cause a dramatic increase in tropospheric ozone.

Non Urban Troposphere Composition Symposium, Hollywood, Fla., November 10-12, 1976, Proceedings

NASA Technical Reports Server (NTRS)

1977-01-01

Papers are presented which originate from a conference on 'The Non-Urban Troposphere Composition', held in 1976. Attention is given to distributions of nitrous oxide in the atmosphere, and to tropospheric and stratospheric compositions which are perturbed by NO(x) emissions from high-altitude aircraft. Ozone is studied in terms of in situ measurements; various meteorological analyses of tropopause folding, ozone measurements in the Boston area, and ozone measurements in rural areas are presented. A one-dimensional model used to study tropospheric photochemistry numerically is presented as are vertical profiles of tropospheric and stratospheric molecular hydrogen. The oxidation of ammonia, methane, and hydrogen sulfide is assessed in nonurban tropospheres along with nonurban measurements of ethane and methane for various atmospheric conditions. With reference to the particle size distribution of chloride in the marine aerosol, organic and inorganic chlorine concentrations are evaluated, and measurements of sea-air CO2 flux by eddy correlation are investigated.

Ozone Pollution

EPA Pesticide Factsheets

Known as tropospheric or ground-level ozone, this gas is harmful to human heath and the environment. Since it forms from emissions of volatile organic compounds (VOCs) and nitrogen oxides (NOx), these pollutants are regulated under air quality standards.

40 CFR 94.304 - Compliance requirements.

Code of Federal Regulations, 2010 CFR

2010-07-01

... specified in this part, except that the applicable FEL replaces the applicable THC+NOX and PM emission... life shall be unlimited. (m) Upper limits. The FELs for THC+NOX and PM for new engines certified for...—Category 1 Upper Limits for Tier 2 Family Emission Limits Subcategory liters/cylinder Model year 1 THC+NOX...

40 CFR 94.304 - Compliance requirements.

Code of Federal Regulations, 2012 CFR

2012-07-01

... specified in this part, except that the applicable FEL replaces the applicable THC+NOX and PM emission... life shall be unlimited. (m) Upper limits. The FELs for THC+NOX and PM for new engines certified for...—Category 1 Upper Limits for Tier 2 Family Emission Limits Subcategory liters/cylinder Model year 1 THC+NOX...

40 CFR 94.304 - Compliance requirements.

Code of Federal Regulations, 2014 CFR

2014-07-01

... specified in this part, except that the applicable FEL replaces the applicable THC+NOX and PM emission... life shall be unlimited. (m) Upper limits. The FELs for THC+NOX and PM for new engines certified for...—Category 1 Upper Limits for Tier 2 Family Emission Limits Subcategory liters/cylinder Model year 1 THC+NOX...

40 CFR 94.304 - Compliance requirements.

Code of Federal Regulations, 2011 CFR

2011-07-01

... specified in this part, except that the applicable FEL replaces the applicable THC+NOX and PM emission... life shall be unlimited. (m) Upper limits. The FELs for THC+NOX and PM for new engines certified for...—Category 1 Upper Limits for Tier 2 Family Emission Limits Subcategory liters/cylinder Model year 1 THC+NOX...

40 CFR 94.304 - Compliance requirements.

Code of Federal Regulations, 2013 CFR

2013-07-01

... specified in this part, except that the applicable FEL replaces the applicable THC+NOX and PM emission... life shall be unlimited. (m) Upper limits. The FELs for THC+NOX and PM for new engines certified for...—Category 1 Upper Limits for Tier 2 Family Emission Limits Subcategory liters/cylinder Model year 1 THC+NOX...

Monitoring tropical cyclone intensity using wind fields derived from short-interval satellite images

NASA Technical Reports Server (NTRS)

Rodgers, E. B.; Gentry, R. C.

1981-01-01

Rapid scan visible images from the Visible Infrared Spin Scan Radiometer sensor on board SMS-2 and GOES-1 were used to derive high resolution upper and lower tropospheric environmental wind fields around three western Atlantic tropical cyclones (1975-78). These wind fields were used to derive upper and lower tropospheric areal mean relative vorticity and their differences, the net relative angular momentum balance and upper tropospheric mass outflow. These kinematic parameters were shown by studies using composite rawinsonde data to be strongly related to tropical cyclone formation and intensity changes. Also, the role of forced synoptic scale subsidence in tropical cyclone formation was examined. The studies showed that satellite-derived lower and upper tropospheric wind fields can be used to monitor and possibly predict tropical cyclone formation and intensity changes. These kinematic analyses showed that future changes in tropical cyclone intensity are mainly related to the "spin-up" of the storms by the net horizontal transport of relative angular momentum caused by convergence of cyclonic vorticity in the lower troposphere and to a lesser extent the divergence of anticyclone vorticity in the upper troposphere.

Origins of tropospheric ozone interannual variation over Réunion: A model investigation

NASA Astrophysics Data System (ADS)

Liu, Junhua; Rodriguez, Jose M.; Thompson, Anne M.; Logan, Jennifer A.; Douglass, Anne R.; Olsen, Mark A.; Steenrod, Stephen D.; Posny, Françoise

2016-01-01

Observations from long-term ozonesonde measurements show robust variations and trends in the evolution of ozone in the middle and upper troposphere over Réunion Island (21.1°S, 55.5°E) in June-August. Here we examine possible causes of the observed ozone variation at Réunion Island using hindcast simulations by the stratosphere-troposphere Global Modeling Initiative chemical transport model for 1992-2014, driven by assimilated Modern-Era Retrospective Analysis for Research and Applications meteorological fields. Réunion Island is at the edge of the subtropical jet, a region of strong stratospheric-tropospheric exchange. Our analysis implies that the large interannual variation (IAV) of upper tropospheric ozone over Réunion is driven by the large IAV of the stratospheric influence. The IAV of the large-scale, quasi-horizontal wind patterns also contributes to the IAV of ozone in the upper troposphere. Comparison to a simulation with constant emissions indicates that increasing emissions do not lead to the maximum trend in the middle and upper troposphere over Réunion during austral winter implied by the sonde data. The effects of increasing emission over southern Africa are limited to the lower troposphere near the surface in August-September.

Origins of Tropospheric Ozone Interannual Variation (IAV) over Reunion: A Model Investigation

NASA Technical Reports Server (NTRS)

Liu, Junhua; Rodriguez, Jose M.; Thompson, Anne M.; Logan, Jennifer A.; Douglass, Anne R.; Olsen, Mark A.; Steenrod, Stephen D.; Posny, Francoise

2016-01-01

Observations from long-term ozonesonde measurements show robust variations and trends in the evolution of ozone in the middle and upper troposphere over Reunion Island (21.1 degrees South Latitude, 55.5 degrees East Longitude) in June-August. Here we examine possible causes of the observed ozone variation at Reunion Island using hindcast simulations by the stratosphere-troposphere Global Modeling Initiative chemical transport model for 1992-2014, driven by assimilated Modern-Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Reunion Island is at the edge of the subtropical jet, a region of strong stratospheric-tropospheric exchange. Our analysis implies that the large interannual variation (IAV) of upper tropospheric ozone over Reunion is driven by the large IAV of the stratospheric influence. The IAV of the large-scale, quasi-horizontal wind patterns also contributes to the IAV of ozone in the upper troposphere. Comparison to a simulation with constant emissions indicates that increasing emissions do not lead to the maximum trend in the middle and upper troposphere over Reunion during austral winter implied by the sonde data. The effects of increasing emission over southern Africa are limited tothe lower troposphere near the surface in August-September.

Effect of the 1997 El Niño on the distribution of upper tropospheric cirrus

NASA Astrophysics Data System (ADS)

Massie, Steven; Lowe, Paul; Tie, Xuexi; Hervig, Mark; Thomas, Gary; Russell, James

2000-09-01

Geographical distributions of Halogen Occultation Experiment (HALOE) aerosol extinction data for 1993-1998 are analyzed in the troposphere and stratosphere at pressures between 121 and 46 hPa. The El Niño conditions of 1997 increased upper tropospheric cirrus over the mid-Pacific and decreased cirrus over Indonesia. Longitudinal centroids of cirrus in the Pacific and over Indonesia shifted eastward by 25° in the troposphere in 1997. Longitudinal centroids of aerosol in the lower stratosphere do not exhibit longitudinal shifts in 1997, indicating that the effects of El Niño upon equatorial particle distributions are confined to the troposphere. The correlation of the longitudinal centroids of outgoing longwave radiation and HALOE extinction confirms the spatial relationship between deep convective clouds and upper tropospheric cirrus. The number of cirrus events observed each year in 1993-1998 in the upper troposphere are quite similar for the region from the Indian Ocean to the mid-Pacific (30°S to 30°N, 50° to 240°E).

Quantifying the causes of differences in tropospheric OH within global models

NASA Astrophysics Data System (ADS)

Nicely, Julie M.; Salawitch, Ross J.; Canty, Timothy; Anderson, Daniel C.; Arnold, Steve R.; Chipperfield, Martyn P.; Emmons, Louisa K.; Flemming, Johannes; Huijnen, Vincent; Kinnison, Douglas E.; Lamarque, Jean-François; Mao, Jingqiu; Monks, Sarah A.; Steenrod, Stephen D.; Tilmes, Simone; Turquety, Solene

2017-02-01

The hydroxyl radical (OH) is the primary daytime oxidant in the troposphere and provides the main loss mechanism for many pollutants and greenhouse gases, including methane (CH4). Global mean tropospheric OH differs by as much as 80% among various global models, for reasons that are not well understood. We use neural networks (NNs), trained using archived output from eight chemical transport models (CTMs) that participated in the Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport Model Intercomparison Project (POLMIP), to quantify the factors responsible for differences in tropospheric OH and resulting CH4 lifetime (τCH4) between these models. Annual average τCH4, for loss by OH only, ranges from 8.0 to 11.6 years for the eight POLMIP CTMs. The factors driving these differences were quantified by inputting 3-D chemical fields from one CTM into the trained NN of another CTM. Across all CTMs, the largest mean differences in τCH4 (ΔτCH4) result from variations in chemical mechanisms (ΔτCH4 = 0.46 years), the photolysis frequency (J) of O3 → O(1D) (0.31 years), local O3 (0.30 years), and CO (0.23 years). The ΔτCH4 due to CTM differences in NOx (NO + NO2) is relatively low (0.17 years), although large regional variation in OH between the CTMs is attributed to NOx. Differences in isoprene and J(NO2) have negligible overall effect on globally averaged tropospheric OH, although the extent of OH variations due to each factor depends on the model being examined. This study demonstrates that NNs can serve as a useful tool for quantifying why tropospheric OH varies between global models, provided that essential chemical fields are archived.

A Decadal (2004-2014) Analysis of Global-to-Regional Tropospheric Ozone Column Trends Using GFDL-AM3 Model Simulations and OMI Observations

NASA Astrophysics Data System (ADS)

Huang, G.; Liu, X.; Lin, M.; Ziemke, J. R.; Chance, K.; Zoogman, P.; Sun, K.

2017-12-01

Tropospheric ozone is a greenhouse gas, biological irritant, and significant source of highly reactive hydroxyl radicals, which remove many hazardous trace gases from the atmosphere. The decadal trend of tropospheric ozone columns (TOCs) can be influenced by many factors including anthropogenic and natural emissions of ozone precursors, large-scale atmospheric circulation patterns, and stratosphere-to-troposphere exchange. Since 2000, anthropogenic emissions of NOx have tended to shift from North America and Europe to Asia. This rapid shift has been implicated in raising background tropospheric ozone burden. However, large meteorologically-driven ozone variability complicates the unambiguous attribution of TOC trends calculated over short periods. In this study, we examine global-to-regional TOC trends during 2004-2014 using two independent satellite retrievals from OMI SAO (Smithsonian Astrophysical Observatory) and OMI/MLS, and interpret the results with a suite of GFDL-AM3 chemistry-climate model hindcasts designed to isolate the response of ozone to anthropogenic emissions, wildfires, and meteorology. Generally, OMI SAO, OMI/MLS and GFDL-AM3 BASE simulations agree on regional hot spots of TOC trends. On the regional scale, we find strong positive TOC trends during 2004-2014 in Mid-East (0.3-0.6 DU yr-1), South Asia (0.3-0.5 DU yr-1), Southeast Asia, East Asia ( 0.1-0.6 DU yr-1) and Central Africa ( 0.6 DU yr-1). Our initial analysis indicates that meteorological variability and anthropogenic emission trends play equally important roles in the positive TOC trends in East Asia and on a global scale during 2004-2014. We are working to investigate the potential influences from lightening NOx emissions, forest fires, and the stratosphere-to-troposphere exchange.

Weekly cycle of NO2 by GOME measurements: A signature of anthropogenic sources

NASA Astrophysics Data System (ADS)

Beirle, S.; Platt, U.; Wenig, M.; Wagner, T.

2003-07-01

Nitrogen oxides (NO+NO2=NOx) are important trace gases in the troposphere with impact on human health, atmospheric chemistry and climate. Besides natural sources (lightning, soil emissions) and biomass burning, fossil fuel combustion is estimated to be responsible for about 50% of the total production of NOx. Since human activity in industrialized countries largely follows an artificial seven-day cycle, fossil fuel combustion is expected to be reduced during weekends. This "weekend effect" is well known from local, ground based measurements, but has never been analysed on a global scale before. The Global Ozone Monitoring Experiment (GOME) on board the ESA-satellite ERS-2 allows measurements of NO2 column densities. Applying sophisticated algorithms, vertical column densities (VCD) of tropospheric NO2 can be determined. We demonstrate the statistical analysis of weekly cycles of tropospheric NO2 VCDs for different regions of the world. In the cycles of the industrialized regions and cities in the US, Europe and Japan a clear Sunday minimum of tropospheric NO2 VCD can be seen. Sunday NO2 VCDs are about 25-50% lower than working day levels. Metropolitan areas with other religious and cultural backgrounds (Jerusalem, Mecca) show different weekly patterns corresponding to different days of rest. In China, no weekly pattern can be found. The presence of a weekly cycle in the measured tropospheric NO2 VCD allows the identification of anthropogenic sources. In addition, the fraction of emissions subjected to a weekly cycle (mainly transport, power generation) with respect to a constant background (all kind of natural sources, biomass burning, heavy industry) can be estimated. Furthermore, we estimated the lifetime of tropospheric NO2 by analysing the mean weekly cycle over Germany in detail, obtaining a value of about 12 h.

Weekly cycle of NO2 by GOME measurements: a signature of anthropogenic sources

NASA Astrophysics Data System (ADS)

Beirle, S.; Platt, U.; Wenig, M.; Wagner, T.

2003-12-01

Nitrogen oxides (NO+NO2=NOx and reservoir species) are important trace gases in the troposphere with impact on human health, atmospheric chemistry and climate. Besides natural sources (lightning, soil emissions) and biomass burning, fossil fuel combustion is estimated to be responsible for about 50% of the total production of NOx. Since human activity in industrialized countries largely follows a seven-day cycle, fossil fuel combustion is expected to be reduced during weekends. This "weekend effect" is well known from local, ground based measurements, but has never been analysed on a global scale before. The Global Ozone Monitoring Experiment (GOME) on board the ESA-satellite ERS-2 allows measurements of NO2 column densities. By estimating and subtracting the stratospheric column, and considering radiative transfer, vertical column densities (VCD) of tropospheric NO2 can be determined (e.g. Leue et al., 2001). We demonstrate the statistical analysis of weekly cycles of tropospheric NO2 VCDs for different regions of the world. In the cycles of the industrialized regions and cities in the US, Europe and Japan a clear Sunday minimum of tropospheric NO2 VCD can be seen. Sunday NO2 VCDs are about 25-50% lower than working day levels. Metropolitan areas with other religious and cultural backgrounds (Jerusalem, Mecca) show different weekly patterns corresponding to different days of rest. In China, no weekly pattern can be found. The presence of a weekly cycle in the measured tropospheric NO2 VCD may help to identify the different anthropogenic source categories. Furthermore, we estimated the lifetime of tropospheric NO2 by analysing the mean weekly cycle exemplarily over Germany, obtaining a value of about 6 h in summer and 18-24 h in winter.

Partitioning the LIS/OTD Lightning Climatological Dataset into Separate Ground and Cloud Flash Distributions

NASA Technical Reports Server (NTRS)

Koshak, W. J.; Solarkiewicz, R. J.

2009-01-01

Presently, it is not well understood how to best model nitrogen oxides (NOx) emissions from lightning because lightning is highly variable. Peak current, channel length, channel altitude, stroke multiplicity, and the number of flashes that occur in a particular region (i.e., flash density) all influence the amount of lightning NOx produced. Moreover, these 5 variables are not the same for ground and cloud flashes; e.g., cloud flashes normally have lower peak currents, higher altitudes, and higher flash densities than ground flashes [see (Koshak, 2009) for additional details]. Because the existing satellite observations of lightning (Fig. 1) from the Lightning Imaging Sensor/Optical Transient Detector (LIS/OTD) do not distinguish between ground and cloud fashes, which produce different amounts of NOx, it is very difficult to accurately account for the regional/global production of lightning NOx. Hence, the ability to partition the LIS/OTD lightning climatology into separate ground and cloud flash distributions would substantially benefit the atmospheric chemistry modeling community. NOx indirectly influences climate because it controls the concentration of ozone and hydroxyl radicals in the atmosphere. The importance of lightning-produced NOx is empasized throughout the scientific literature (see for example, Huntrieser et al. 1998). In fact, lightning is the most important NOx source in the upper troposphere with a global production rate estimated to vary between 2 and 20 Tg (N)yr(sup -1) (Lee et al., 1997), with more recent estimates of about 6 Tg(N)yr(sup -1) (Martin et al., 2007). In order to make accurate predictions, global chemistry/climate models (as well as regional air quality modells) must more accurately account for the effects of lightning NOx. In particular, the NASA Goddard Institute for Space Studies (GISS) Model E (Schmidt et al., 2005) and the GEOS-CHEM global chemical transport model (Bey et al., 2001) would each benefit from a partitioning of the LIS/OTD lightning climatology. In this study, we introduce a new technique for retrieving the ground flash fraction in a set of N lightning observed from space and that occur within a specific latitude/longitude bin. The method is briefly described and applied to CONUS lightning that have already been partitioned into ground and cloud flashes using independent ground-based observations, in order to assess the accuracy of the retrieval method. The retrieval errors are encouragingly small.

Removal of NOx and NOy in biomass burning plumes in the boundary layer over northern Australia

NASA Astrophysics Data System (ADS)

Takegawa, N.; Kondo, Y.; Koike, M.; Ko, M.; Kita, K.; Blake, D. R.; Nishi, N.; Hu, W.; Liley, J. B.; Kawakami, S.; Shirai, T.; Miyazaki, Y.; Ikeda, H.; Russel-Smith, J.; Ogawa, T.

2003-05-01

The Biomass Burning and Lightning Experiment Phase B (BIBLE-B) aircraft measurement campaign was conducted over the western Pacific and Australia in August and September 1999. In situ aircraft measurements of carbon monoxide (CO), nitric oxide (NO), total reactive nitrogen (NOy), ozone (O3), nonmethane hydrocarbons (NMHCs), and other species were made during BIBLE-B. Meteorological analysis shows that the trace gases emitted from biomass burning in northern Australia were mostly confined within the planetary boundary layer (below ˜3 km) by strong subsidence in the free troposphere. Removal processes of NOx (equal to measured NO + calculated NO2) and NOy in biomass burning plumes in the boundary layer are examined on the basis of correlation analysis. The photochemical lifetime of NOx in biomass burning plumes during the daytime is estimated to be 0.1 to 0.3 days using the correlations of NOx with short-lived NMHCs and hydroxyl radical (OH) concentration calculated from a constrained photochemical model. Correlation of NOy with CO shows that ˜60% of the NOy molecules originating from biomass burning were removed in the boundary layer within 2-3 days. This result is consistent with dry deposition of nitric acid (HNO3) in the plumes. It is likely that only a small fraction of NOy emitted from biomass burning was exported from the boundary layer to the free troposphere during the BIBLE-B period.

"Cloud Slicing" : A New Technique to Derive Tropospheric Ozone Profile Information from Satellite Measurements

NASA Technical Reports Server (NTRS)

Ziemke, J. R.; Chandra, S.; Bhartia, P. K.; Einaudi, Franco (Technical Monitor)

2000-01-01

A new technique denoted cloud slicing has been developed for estimating tropospheric ozone profile information. All previous methods using satellite data were only capable of estimating the total column of ozone in the troposphere. Cloud slicing takes advantage of the opaque property of water vapor clouds to ultraviolet wavelength radiation. Measurements of above-cloud column ozone from the Nimbus 7 total ozone mapping spectrometer (TOMS) instrument are combined together with Nimbus 7 temperature humidity and infrared radiometer (THIR) cloud-top pressure data to derive ozone column amounts in the upper troposphere. In this study tropical TOMS and THIR data for the period 1979-1984 are analyzed. By combining total tropospheric column ozone (denoted TCO) measurements from the convective cloud differential (CCD) method with 100-400 hPa upper tropospheric column ozone amounts from cloud slicing, it is possible to estimate 400-1000 hPa lower tropospheric column ozone and evaluate its spatial and temporal variability. Results for both the upper and lower tropical troposphere show a year-round zonal wavenumber 1 pattern in column ozone with largest amounts in the Atlantic region (up to approx. 15 DU in the 100-400 hPa pressure band and approx. 25-30 DU in the 400-1000 hPa pressure band). Upper tropospheric ozone derived from cloud slicing shows maximum column amounts in the Atlantic region in the June-August and September-November seasons which is similar to the seasonal variability of CCD derived TCO in the region. For the lower troposphere, largest column amounts occur in the September-November season over Brazil in South America and also southern Africa. Localized increases in the tropics in lower tropospheric ozone are found over the northern region of South America around August and off the west coast of equatorial Africa in the March-May season. Time series analysis for several regions in South America and Africa show an anomalous increase in ozone in the lower troposphere around the month of March which is not observed in the upper troposphere. The eastern Pacific indicates weak seasonal variability of upper, lower, and total tropospheric ozone compared to the western Pacific which shows largest TCO amounts in both hemispheres around spring months. Ozone variability in the western Pacific is expected to have greater variability caused by strong convection, pollution and biomass burning, land/sea contrast and monsoon developments.

Enhancement in the upper tropospheric humidity associated with aerosol loading over tropical Pacific

NASA Astrophysics Data System (ADS)

Kottayil, Ajil; Satheesan, K.

2015-12-01

Many modeling studies have indicated that aerosol interactions with clouds increase the upper tropospheric humidity (UTH), but observational evidences are sparse. Using satellite datasets of upper tropospheric humidity and aerosols, this study shows that aerosols increase the upper tropospheric humidity over the tropical North West Pacific (NWP) and North East Pacific (NEP). The observations show an increase in the UTH by 2.8%RH over NEP for an increment of 0.12 in aerosol optical depth (AOD) and 2%RH increase in UTH over NWP for an increment of 0.19 in AOD. The study also quantifies the change in longwave cloud radiative forcing (LWCRF) as a consequence of the increase in UTH due to aerosols. The LWCRF increases by 3.38 W m-2 over NEP and by 4.46 W m-2 over NWP. The result that aerosols increase the upper tropospheric humidity is significant since the latter plays a crucial role in regulating the Earth's radiation budget and water vapor feedback.

Elevated Ozone in the Troposphere over the Atlantic and Pacific Oceans in the Northern Hemisphere

NASA Technical Reports Server (NTRS)

Chandra, S.; Ziemke, J. R.; Tie, Xuexi

2003-01-01

Tropospheric column ozone (TCO) is derived from differential measurements of total column ozone from Nimus-7 and Earth Probe TOMS, and stratospheric column ozone from the Microwave Limb Sounder instrument on the Upper Atmospheric Research Satellite. It is shown that TCO during summer months over the Atlantic and Pacific Oceans at northern mid-latitudes is about the same (50-60 Dobson Units) as over the continents of North America, Europe and Asia, where surface emissions of nitrogen oxides from industrial sources, biomass and biofuel burning and biogenic emissions are significantly larger. This nearly uniform zonal variation in TCO is modulated by surface topography of the Rocky and Himalayan mountains and Tibetan Plateau where TCO is reduced by 20-30 Dobson Units. The zonal characteristics of TCO derived from satellite measurements are well simulated by a global chemical transport model called MOZART-2 (Model of Ozone and Related Chemical Tracers, version 2). The model results are analyzed to delineate the relative importance of various processes contributing to observed zonal characteristics of TCO, and they are shown that the surface emission of NOx contributes about 50% of the TCO at northern mid-latitudes, especially over the continents of North America, Europe and Asia. The result of TCO derived from TOMS and the analysis from MOZART-2 indicate that TCO is a very useful tool to study tropospheric O3 pollution resulting from surface emissions of pollutants.

Physical Mechanisms Controlling Upper Tropospheric Water Vapor as Revealed by MLS Data from UARS

NASA Technical Reports Server (NTRS)

Newell, Reginald E.; Douglass, Anne (Technical Monitor)

2002-01-01

The third year and final report on the physical mechanisms controlling upper tropospheric water vapor revealed by the Microwave Limb Sounder (MLS) on the Upper Atmosphere Research Satellite (UARS) is presented.

The influence of boreal biomass burning emissions on the distribution of tropospheric ozone over North America and the North Atlantic during 2010

NASA Astrophysics Data System (ADS)

Parrington, M.; Palmer, P. I.; Henze, D. K.; Tarasick, D. W.; Hyer, E. J.; Owen, R. C.; Helmig, D.; Clerbaux, C.; Bowman, K. W.; Deeter, M. N.; Barratt, E. M.; Coheur, P.-F.; Hurtmans, D.; Jiang, Z.; George, M.; Worden, J. R.

2012-02-01

We have analysed the sensitivity of the tropospheric ozone distribution over North America and the North Atlantic to boreal biomass burning emissions during the summer of 2010 using the GEOS-Chem 3-D global tropospheric chemical transport model and observations from in situ and satellite instruments. We show that the model ozone distribution is consistent with observations from the Pico Mountain Observatory in the Azores, ozonesondes across Canada, and the Tropospheric Emission Spectrometer (TES) and Infrared Atmospheric Sounding Instrument (IASI) satellite instruments. Mean biases between the model and observed ozone mixing ratio in the free troposphere were less than 10 ppbv. We used the adjoint of GEOS-Chem to show the model ozone distribution in the free troposphere over Maritime Canada is largely sensitive to NOx emissions from biomass burning sources in Central Canada, lightning sources in the central US, and anthropogenic sources in the eastern US and south-eastern Canada. We also used the adjoint of GEOS-Chem to evaluate the Fire Locating And Monitoring of Burning Emissions (FLAMBE) inventory through assimilation of CO observations from the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument. The CO inversion showed that, on average, the FLAMBE emissions needed to be reduced to 89% of their original values, with scaling factors ranging from 12% to 102%, to fit the MOPITT observations in the boreal regions. Applying the CO scaling factors to all species emitted from boreal biomass burning sources led to a decrease of the model tropospheric distributions of CO, PAN, and NOx by as much as -20 ppbv, -50 pptv, and -20 pptv respectively. The modification of the biomass burning emission estimates reduced the model ozone distribution by approximately -3 ppbv (-8%) and on average improved the agreement of the model ozone distribution compared to the observations throughout the free troposphere, reducing the mean model bias from 5.5 to 4.0 ppbv for the Pico Mountain Observatory, 3.0 to 0.9 ppbv for ozonesondes, 2.0 to 0.9 ppbv for TES, and 2.8 to 1.4 ppbv for IASI.

An airborne compatible photofragmentation two-photon laser-induced fluorescence instrument for measuring background tropospheric levels of NO, NO(x), and NO2

NASA Technical Reports Server (NTRS)

Sandholm, S. T.; Bradshaw, J. D.; Dorris, K. S.; Rodgers, M. O.; Davis, D. D.

1990-01-01

The operating principle, design, and performance of a two-photon LIF (TP-LIF) sensor for simultaneous measurements of NO, NO(x) (NO + NO2), and NO2 are described. In this instrument, NO is first measured by direct spectroscopic TP-LIF detection; NO2 is converted to NO by photofragmentation using an XeF excimer laser operating at 353 nm; and the resulting NO is then detected quantitatively by TP-LIF. The detection limits of the instrument are found to be 3.5 parts per trillion by volume (pptv) of NO and 10 pptv for NO2, with integration times of 2 and 6 min, respectively. The in-flight performance of the instrument was evaluated during the NASA Global Tropospheric Experiment Chemical Instrumentation Test and Evaluation 2 program in summer 1986, as reported by Gregory et al. (1990).

Space based inverse modeling of seasonal variations of anthropogenic and natural emissions of nitrogen oxides over China and effects of uncertainties in model meteorology and chemistry

NASA Astrophysics Data System (ADS)

Lin, J.

2011-12-01

Nitrogen oxides (NOx ≡ NO + NO2) are important atmospheric constituents affecting the tropospheric chemistry, surface air quality and climatic forcing. They are emitted both from anthropogenic and from natural (soil, lightning, biomass burning, etc.) sources, which can be estimated inversely from satellite remote sensing of the vertical column densities (VCDs) of nitrogen dioxide (NO2) in the troposphere. Based on VCDs of NO2 retrieved from OMI, a novel approach is developed in this study to separate anthropogenic emissions of NOx from natural sources over East China for 2006. It exploits the fact that anthropogenic and natural emissions vary with seasons with distinctive patterns. The global chemical transport model (CTM) GEOS-Chem is used to establish the relationship between VCDs of NO2 and emissions of NOx for individual sources. Derived soil emissions are compared to results from a newly developed bottom-up approach. Effects of uncertainties in model meteorology and chemistry over China, an important source of errors in the emission inversion, are evaluated systematically for the first time. Meteorological measurements from space and the ground are used to analyze errors in meteorological parameters driving the CTM.

Data archive for NO(y) from observations and construction and testing of airborne instrument for simultaneous measurement of NO, NO2, NO(y), and O3

NASA Technical Reports Server (NTRS)

Carroll, Mary Anne; Emmons, Louisa

1995-01-01

The compilation and archiving of NO(x) and NO(y) measurements began in mid-March 1994. Since the submission of the first report, data summaries have been obtained for the TROPOZ 2, STRATOZ 3, OCTA and TOR/Schauinsland campaigns, and the full data sets will become a part of this archive in the near future. Climatologies of NO(x) and NO(y) have been developed from these and previously archived data sets, including the available GTE campaigns (ABLE-2A, B, -3A, B, CITE-2, -3, TRACE-A, PEM WEST-A) and AASE 1 and 2. The data have been grouped by season and altitude (boundary layer and 3 km ranges in the free troposphere). Maps showing median values of midday NO, NO(x) and NO(y) have been produced for each season for the boundary layer and 3 km ranges of the free troposphere. The statistics of the data (median, mean, and standard deviation, central 67% and 90%) have also been determined, and are shown in representative figures included in this report.

Origins of tropospheric ozone interannual variation (IAV) over Réunion: A model investigation.

PubMed

Liu, Junhua; Rodriguez, Jose M; Thompson, Anne M; Logan, Jennifer A; Douglass, Anne R; Olsen, Mark A; Steenrod, Stephen D; Posny, Francoise

2016-01-16

Observations from long-term ozonesonde measurements show robust variations and trends in the evolution of ozone in the middle and upper troposphere over Réunion Island (21.1°S, 55.5°E) in June-August. Here we examine possible causes of the observed ozone variation at Réunion Island using hindcast simulations by the stratosphere-troposphere Global Modeling Initiative chemical transport model (GMI-CTM) for 1992-2014, driven by assimilated Modern-Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Réunion Island is at the edge of the subtropical jet, a region of strong stratospheric-tropospheric exchange (STE). Our analysis implies that the large interannual variation (IAV) of upper tropospheric ozone over Réunion is driven by the large IAV of the stratospheric influence. The IAV of the large-scale, quasi-horizontal wind patterns also contributes to the IAV of ozone in the upper troposphere. Comparison to a simulation with constant emissions indicates that increasing emissions do not lead to the maximum trend in the middle and upper troposphere over Réunion during austral winter implied by the sonde data. The effects of increasing emission over southern Africa are limited to the lower troposphere near the surface in August - September.

Origins of tropospheric ozone interannual variation (IAV) over Réunion: A model investigation

PubMed Central

Liu, Junhua; Rodriguez, Jose M.; Thompson, Anne M.; Logan, Jennifer A.; Douglass, Anne R.; Olsen, Mark A.; Steenrod, Stephen D.; Posny, Francoise

2018-01-01

Observations from long-term ozonesonde measurements show robust variations and trends in the evolution of ozone in the middle and upper troposphere over Réunion Island (21.1°S, 55.5°E) in June-August. Here we examine possible causes of the observed ozone variation at Réunion Island using hindcast simulations by the stratosphere-troposphere Global Modeling Initiative chemical transport model (GMI-CTM) for 1992–2014, driven by assimilated Modern-Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Réunion Island is at the edge of the subtropical jet, a region of strong stratospheric-tropospheric exchange (STE). Our analysis implies that the large interannual variation (IAV) of upper tropospheric ozone over Réunion is driven by the large IAV of the stratospheric influence. The IAV of the large-scale, quasi-horizontal wind patterns also contributes to the IAV of ozone in the upper troposphere. Comparison to a simulation with constant emissions indicates that increasing emissions do not lead to the maximum trend in the middle and upper troposphere over Réunion during austral winter implied by the sonde data. The effects of increasing emission over southern Africa are limited to the lower troposphere near the surface in August – September. PMID:29657911

Exploring the Production of NOx by Lightning and Its Impact on Tropospheric Ozone

NASA Technical Reports Server (NTRS)

Gillani, Noor; Koshak, William; Biazar, Arastoo; Doty, Kevin; Mahon, Robert; Newchurch, Michael; Byun, Daewon; Emmons, Louisa

2006-01-01

Our quantitative understanding of free tropospheric (FT) chemistry is quite poor. State-of-the-art regional air quality models (e.g., US EPA's CMAQ) perform very poorly in simulating FT chemistry, with Uniform ozone around 70 ppb throughout the FT in summer, while ozonesonde data show much higher levels of ozone and much spatial-temporal structure. Such models completely neglect lightning-NOx (LNOx) emissions (the most significant source of NOx in the FT), and also contain large uncertainties in the specifications of intercontinental transport, stratosphere-troposphere exchange (STE) and PBLFT exchange (PFTE). Global air chemistry models include LNOx, but in very crude fashion, with the frequency and distribution of lightning being based on modeled cloud parameters (hence large uncertainty), lightning energetics being assumed to be constant for all flashes (literature value, while in reality there is at least a two-orders of magnitude variability from flash-to-flash), and the production of NOx in the surrounding heated air, per Joule of heating, being assumed to be constant also (literature value, while in fact it is a non-linear function of the dissipated heat and local air density, p). This situation is commonly blamed on paucity of pertinent observational data, but for the USA, there is now a wealth of surface- and satellite-based data of lightning available to permit much improved observation-based estimation of LNOx emissions. In the FT, such NOx has a long residence time, and also the ozone production efficiency from NOx there is considerably higher than in the PBL. It is, therefore, of critical importance in FT chemistry. This paper will describe the approach and data products of an ongoing NSSTC project aimed at a much-improved quantification of not only LNOx production on the scale of continental USA based on local and regional lightning observations, but also of intercontinental transport, STE and PFTE, all in upgraded simulations of tropospheric transport and chemistry. In our approach for LNOx, (a) we utilize continuous observed lightning information from the NLDN ground network and from satellite imagers (OTD and LIS) to quantify lightning frequency and distribution at the spatial-temporal scales of models such as CMAQ; (b) we develop new methodologies to quantify flash-specific lightning energy dissipation as heat (epsilon) using data from the research-grade lightning measurement facility at NASA-KSC, and to parameterize epsilon based on regional lightning monitoring data (ground- and satellite-based); and, (c) we develop a new parameterization of NOx production as a function of epsilon and rho. Based on such observation-based information, we are working to develop a gridded, episodic LNOx emissions inventory for the USA for use in models like CMAQ. We are also developing approaches for global(MOZART)- regional(CMAQ) chemistry coupling to improve intercontinental transport and STE. Finally, we are developing new methodologies for assimilation of satellite-observed (GOES) clouds into meteorological modeling (MM5), to improve PFTE and to optimize co-location of cloud convection and observed lightning. We will incorporate these improvements in CMAQ simulations over the USA to better understand FT processes and chemistry, and its impact on ground-level ozone.

Demonstration of long-term increases in tropospheric O3 levels: causes and potential impacts.

PubMed

Susaya, Janice; Kim, Ki-Hyun; Shon, Zang-Ho; Brown, Richard J C

2013-09-01

Ground-level ozone (O3) is a well-known atmospheric pollutant with its adverse impacts on the environment and human health. Here, the tropospheric O3 concentrations monitored in seven major cities in Korea at monthly intervals over a 22-year period (1989-2010) are presented, and their long-term variability examined. The analysis of annual mean values of O3 (in nmolmol(-1), or ppb) showed a noticeable increase of 118±69% in all seven cities over the two decades (p<0.01). Changes in O3 levels are closely associated with both environmental (e.g., NOx (NO+NO2), SO2, CO, and total suspended particles (TSPs) (p<0.01), temperature, and sunshine hours) and common anthropogenic variables (e.g., population density and number of vehicles). Evidence collected in this study suggests that the atmospheric conditions in most major cities of Korea should be volatile organic compounds (VOCs) sensitive or NOx saturated with respect to O3 formation. As such, establishment of a proper management strategy seems a sensible approach to control tropospheric ozone concentrations in densely populated cities. Copyright © 2013 Elsevier Ltd. All rights reserved.

Rapid increases in tropospheric ozone production and export from China: A view from AURA and TM5

NASA Astrophysics Data System (ADS)

Verstraeten, W. W.; Neu, J. L.; Williams, J. E.; Bowman, K. W.; Worden, J. R.; Boersma, K. F.

2015-12-01

Eastern Asia has the fastest growing anthropogenic emissions in the world, possibly affecting both the pollution in the local troposphere as well as in the trans-Pacific region. Local measurements over Asia show that tropospheric ozone (O3) has increased by 1 to 3% per year since the start of the millennium. This increase is often invoked to explain positive tropospheric O3 trends observed in western US, but to date there is no unambiguous evidence showing that enhanced Asian pollution is responsible for these trends. In this research we use observations of tropospheric O3 from TES (Tropospheric Emission Spectrometer, onboard AURA), tropospheric NO2 measurements from OMI (Ozone Monitoring Instrument, onboard AURA) and lower stratospheric observations of O3 from MLS (Microwave Limb Sounder, onboard AURA) in combination with the TM5 CTM. Satellite-based studies focusing on tropospheric O3 and NO2 have the potential to close the gap left by previous studies on air quality since spaceborne data provide large-scale observational evidence that both O3 precursor concentrations and tropospheric O3 levels are rapidly changing over source receptor areas. We show the increased ability of TM5 to reproduce the 2005-2010 observed rapid rise in free tropospheric O3 of 7% over China from TES, once OMI NO2 measurements were implemented in TM5 to update NOX emissions. MLS observations on lower stratospheric O3 have the potential to improve the stratosphere-troposphere exchange (STE) estimate in TM5 which is mainly driven by ECMWF meteorological fields. Constraining the TM5 modelled trend of the STE contribution to the 3-9 km partial O3 column using MLS observations of stratospheric O3 lead to a better explanation of the sources of the free tropospheric O3 trends over China. Based on the OMI inferred TM5 updates in NOX emissions, the impact of Asian O3 and its precursors on the free troposphere (3-9 km) over the western US could be quantified. Large import from China offsets the local efforts to improve air quality in the 3-9 km partial column over the western US with more than 40%. The issue of export and long-range transport of pollution from other countries indicates that global efforts may be required to address both the global as well as the regional air quality and climate change.

Global Free Tropospheric NO2 Abundances Derived Using a Cloud Slicing Technique Applied to Satellite Observations from the Aura Ozone Monitoring Instrument (OMI)

NASA Technical Reports Server (NTRS)

Choi, S.; Joiner, J.; Choi, Y.; Duncan, B. N.; Bucsela, E.

2014-01-01

We derive free-tropospheric NO2 volume mixing ratios (VMRs) and stratospheric column amounts of NO2 by applying a cloud slicing technique to data from the Ozone Monitoring Instrument (OMI) on the Aura satellite. In the cloud-slicing approach, the slope of the above-cloud NO2 column versus the cloud scene pressure is proportional to the NO2 VMR. In this work, we use a sample of nearby OMI pixel data from a single orbit for the linear fit. The OMI data include cloud scene pressures from the rotational-Raman algorithm and above-cloud NO2 vertical column density (VCD) (defined as the NO2 column from the cloud scene pressure to the top-of-the-atmosphere) from a differential optical absorption spectroscopy (DOAS) algorithm. Estimates of stratospheric column NO2 are obtained by extrapolating the linear fits to the tropopause. We compare OMI-derived NO2 VMRs with in situ aircraft profiles measured during the NASA Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in 2006. The agreement is generally within the estimated uncertainties when appropriate data screening is applied. We then derive a global seasonal climatology of free-tropospheric NO2 VMR in cloudy conditions. Enhanced NO2 in the free troposphere commonly appears near polluted urban locations where NO2 produced in the boundary layer may be transported vertically out of the boundary layer and then horizontally away from the source. Signatures of lightning NO2 are also shown throughout low and middle latitude regions in summer months. A profile analysis of our cloud slicing data indicates signatures of uplifted and transported anthropogenic NO2 in the middle troposphere as well as lightning-generated NO2 in the upper troposphere. Comparison of the climatology with simulations from the Global Modeling Initiative (GMI) for cloudy conditions (cloud optical thicknesses > 10) shows similarities in the spatial patterns of continental pollution outflow. However, there are also some differences in the seasonal variation of free-tropospheric NO2 VMRs near highly populated regions and in areas affected by lightning-generated NOx. Stratospheric column NO2 obtained from cloud slicing agrees well with other independently-generated estimates, providing further confidence in the free-tropospheric results.

Interannual variability in tropical tropospheric ozone and OH: The role of lightning

NASA Astrophysics Data System (ADS)

Murray, Lee T.; Logan, Jennifer A.; Jacob, Daniel J.

2013-10-01

Nitrogen oxide radicals (NOx) produced by lightning are natural precursors for the production of the dominant tropospheric oxidants, OH and ozone. Observations of the interannual variability (IAV) of tropical ozone and of global mean OH (from the methyl chloroform proxy) offer a window for understanding the sensitivity of ozone and OH to environmental factors. We present the results of simulations for 1998-2006 using the GEOS-Chem chemical transport model (CTM) with IAV in tropical lightning constrained by satellite observations from the Lightning Imaging Sensor. We find that this imposed IAV in lightning NOx improves the ability of the model to reproduce observed IAV in tropical ozone and OH. Lightning is far more important than biomass burning in driving the IAV of tropical ozone, even though the IAV of NOx emissions from fires is greater than that from lightning. Our results indicate that the IAV in tropospheric OH is highly sensitive to lightning relative to other emissions and suggest that lightning contributes an important fraction of the observed IAV in OH inferred from the methyl chloroform proxy. Lightning affects OH through the HO2+ NO reaction, an effect compounded by positive feedback from the resulting increase in ozone production and in CO loss. We can account in the model for the observed increase in OH in 1998-2004 and for its IAV, but the model fails to explain the OH decrease in 2004-2006. We find that stratospheric ozone plays little role in driving IAV in OH during 1998-2006, in contrast to previous studies that examined earlier periods.

Tropospheric Ozone Source Attribution in Southern California during Summer 2014 Based on Lidar Measurements and Model Simulations

NASA Technical Reports Server (NTRS)

Granados Munoz, Maria Jose; Johnson, Matthew S.; Leblanc, Thierry

2016-01-01

In the past decades, significant efforts have been made to increase tropospheric ozone long-term monitoring. A large number of ground-based, airborne and space-borne instruments are currently providing valuable data to contribute to better understand tropospheric ozone budget and variability. Nonetheless, most of these instruments provide in-situ surface and column-integrated data, whereas vertically resolved measurements are still scarce. Besides ozonesondes and aircraft, lidar measurements have proven to be valuable tropospheric ozone profilers. Using the measurements from the tropospheric ozone differential absorption lidar (DIAL) located at the JPL Table Mountain Facility, California, and the GEOS-Chem and GEOS-5 model outputs, the impact of the North American monsoon on tropospheric ozone during summer 2014 is investigated. The influence of the Monsoon lightning-induced NOx will be evaluated against other sources (e.g. local anthropogenic emissions and the stratosphere) using also complementary data such as backward-trajectories analysis, coincident water vapor lidar measurements, and surface ozone in-situ measurements.

Monthly mean large-scale analyses of upper-tropospheric humidity and wind field divergence derived from three geostationary satellites

NASA Technical Reports Server (NTRS)

Schmetz, Johannes; Menzel, W. Paul; Velden, Christopher; Wu, Xiangqian; Vandeberg, Leo; Nieman, Steve; Hayden, Christopher; Holmlund, Kenneth; Geijo, Carlos

1995-01-01

This paper describes the results from a collaborative study between the European Space Operations Center, the European Organization for the Exploitation of Meteorological Satellites, the National Oceanic and Atmospheric Administration, and the Cooperative Institute for Meteorological Satellite Studies investigating the relationship between satellite-derived monthly mean fields of wind and humidity in the upper troposphere for March 1994. Three geostationary meteorological satellites GOES-7, Meteosat-3, and Meteosat-5 are used to cover an area from roughly 160 deg W to 50 deg E. The wind fields are derived from tracking features in successive images of upper-tropospheric water vapor (WV) as depicted in the 6.5-micron absorption band. The upper-tropospheric relative humidity (UTH) is inferred from measured water vapor radiances with a physical retrieval scheme based on radiative forward calculations. Quantitative information on large-scale circulation patterns in the upper-troposphere is possible with the dense spatial coverage of the WV wind vectors. The monthly mean wind field is used to estimate the large-scale divergence; values range between about-5 x 10(exp -6) and 5 x 10(exp 6)/s when averaged over a scale length of about 1000-2000 km. The spatial patterns of the UTH field and the divergence of the wind field closely resemble one another, suggesting that UTH patterns are principally determined by the large-scale circulation. Since the upper-tropospheric humidity absorbs upwelling radiation from lower-tropospheric levels and therefore contributes significantly to the atmospheric greenhouse effect, this work implies that studies on the climate relevance of water vapor should include three-dimensional modeling of the atmospheric dynamics. The fields of UTH and WV winds are useful parameters for a climate-monitoring system based on satellite data. The results from this 1-month analysis suggest the desirability of further GOES and Meteosat studies to characterize the changes in the upper-tropospheric moisture sources and sinks over the past decade.

The influence of boreal biomass burning emissions on the distribution of tropospheric ozone over North America and the North Atlantic during 2010

NASA Astrophysics Data System (ADS)

Parrington, M.; Palmer, P. I.; Henze, D. K.; Tarasick, D. W.; Hyer, E. J.; Owen, R. C.; Helmig, D.; Clerbaux, C.; Bowman, K. W.; Deeter, M. N.; Barratt, E. M.; Coheur, P.-F.; Hurtmans, D.; George, M.; Worden, J. R.

2011-09-01

We analyse the tropospheric ozone distribution over North America and the North Atlantic to boreal biomass burning emissions during the summer of 2010 using the GEOS-Chem 3-D global tropospheric chemical transport model, and observations from in situ and satellite instruments. In comparison to observations from the PICO-NARE observatory in the Azores, ozonesondes across Canada, and the Tropospheric Emission Spectrometer (TES) and Infrared Atmospheric Sounding Instrument (IASI) satellite instruments, the model ozone distribution is shown to be in reasonable agreement with mean biases less than 10 ppbv. We use the adjoint of GEOS-Chem to show the model ozone distribution in the free troposphere over Maritime Canada is largely sensitive to NOx emissions from biomass burning sources in Central Canada, lightning sources in the central US, and anthropogenic sources in eastern US and south-eastern Canada. We also use the adjoint of GEOS-Chem to evaluate the Fire Locating And Monitoring of Burning Emissions (FLAMBE) inventory through assimilation of CO observations from the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument. The CO inversion showed that, on average the FLAMBE emissions needed to be reduced to 89 % of their original values, with scaling factors ranging from 12 % to 102 %, to fit the MOPITT observations in the boreal regions. Applying the CO scaling factors to all species emitted from boreal biomass burning sources led to a decrease of the model tropospheric distributions of CO, PAN, and NOx by as much as -20 ppbv, -50 ppbv, and -20 ppbv respectively. The impact of optimizing the biomass burning emissions was to reduce the model ozone distribution by approximately -3 ppbv (-8 %) and on average improved the agreement of the model ozone distribution compared to the observations throughout the free troposphere reducing the mean model bias from 5.5 to 4.0 ppbv for the PICO-NARE observatory, 3.0 to 0.9 ppbv for ozonesondes, 2.0 to 0.9 ppbv for TES, and 2.8 to 1.4 ppbv for IASI.

Lower tropospheric ozone over India and its linkage to the South Asian monsoon

NASA Astrophysics Data System (ADS)

Lu, Xiao; Zhang, Lin; Liu, Xiong; Gao, Meng; Zhao, Yuanhong; Shao, Jingyuan

2018-03-01

Lower tropospheric (surface to 600 hPa) ozone over India poses serious risks to both human health and crops, and potentially affects global ozone distribution through frequent deep convection in tropical regions. Our current understanding of the processes controlling seasonal and long-term variations in lower tropospheric ozone over this region is rather limited due to spatially and temporally sparse observations. Here we present an integrated process analysis of the seasonal cycle, interannual variability, and long-term trends of lower tropospheric ozone over India and its linkage to the South Asian monsoon using the Ozone Monitoring Instrument (OMI) satellite observations for years 2006-2014 interpreted with a global chemical transport model (GEOS-Chem) simulation for 1990-2010. OMI observed lower tropospheric ozone over India averaged for 2006-2010, showing the highest concentrations (54.1 ppbv) in the pre-summer monsoon season (May) and the lowest concentrations (40.5 ppbv) in the summer monsoon season (August). Process analyses in GEOS-Chem show that hot and dry meteorological conditions and active biomass burning together contribute to 5.8 Tg more ozone being produced in the lower troposphere in India in May than January. The onset of the summer monsoon brings ozone-unfavorable meteorological conditions and strong upward transport, which all lead to large decreases in the lower tropospheric ozone burden. Interannually, we find that both OMI and GEOS-Chem indicate strong positive correlations (r = 0.55-0.58) between ozone and surface temperature in pre-summer monsoon seasons, with larger correlations found in high NOx emission regions reflecting NOx-limited production conditions. Summer monsoon seasonal mean ozone levels are strongly controlled by monsoon strengths. Lower ozone concentrations are found in stronger monsoon seasons mainly due to less ozone net chemical production. Furthermore, model simulations over 1990-2010 estimate a mean annual trend of 0.19 ± 0.07 (p value < 0.01) ppbv yr-1 in Indian lower tropospheric ozone over this period, which are mainly driven by increases in anthropogenic emissions with a small contribution (about 7 %) from global methane concentration increases.

Hydrogen Radicals, Nitrogen Radicals, and the Production of O3 in the Upper Troposphere

NASA Technical Reports Server (NTRS)

Wennberg, P. O.; Hanisco, T. F.; Jaegle, L.; Jacob, D. J.; Hintsa, E. J.; Lanzendorf, E. J.; Anderson, J. G.; Gao, R.-S.; Keim, E. R.; Donnelly, S. G.;

Hydrogen Radicals, Nitrogen Radicals, and the Production of O3 in the Upper Troposphere

NASA Technical Reports Server (NTRS)

Wennberg, P. O.; Hanisco, T. F.; Jaegle, L.; Jacob, D. J.; Hintsa, E. J.; Lanzendorf, E. J.; Anderson, J. G.; Gao, R.-S.; Keim, E. R.; Donnelly, S. G.;

Cloud and radiative heating profiles associated with the boreal summer intraseasonal oscillation

NASA Astrophysics Data System (ADS)

Kim, Jinwon; Waliser, Duane E.; Cesana, Gregory V.; Jiang, Xianan; L'Ecuyer, Tristan; Neena, J. M.

2018-03-01

The cloud water content (CW) and radiative heating rate (QR) structures related to northward propagating boreal summer intraseasonal oscillations (BSISOs) are analyzed using data from A-train satellites in conjunction with the ERA-Interim reanalysis. It is found that the northward movement of CW- and QR anomalies are closely synchronized with the northward movement of BSISO precipitation maxima. Commensurate with the northward propagating BSISO precipitation maxima, the CW anomalies exhibit positive ice (liquid) CW maxima in the upper (middle/low) troposphere with a prominent tilting structure in which the low-tropospheric (upper-tropospheric) liquid (ice) CW maximum leads (lags) the BSISO precipitation maximum. The BSISO-related shortwave heating (QSW) heats (cools) the upper (low) troposphere; the longwave heating (QLW) cools (heats) the upper (middle/low) troposphere. The resulting net radiative heating (QRN), being dominated by QLW, cools (heats) the atmosphere most prominently above the 200 hPa level (below the 600 hPa level). Enhanced clouds in the upper and middle troposphere appears to play a critical role in increasing low-level QLW and QRN. The vertically-integrated QSW, QLW and QRN are positive in the region of enhanced CW with the maximum QRN near the latitude of the BSISO precipitation maximum. The bottom-heavy radiative heating anomaly resulting from the cloud-radiation interaction may act to strengthen convection.

Adaptation of an In Situ Ground-Based Tropospheric OH/HO2 Instrument for Aircraft Use

NASA Technical Reports Server (NTRS)

Brune, William H.

1997-01-01

In-situ HO(x) (OH and HO2) measurements are an essential part of understanding the photochemistry of aircraft exhaust in the atmosphere. HO(x) affects the partitioning of nitrogen species in the NO(y) family. Its reactions are important sources and sinks for tropospheric ozone, thus providing a link between the NO(x) in aircraft exhaust and tropospheric ozone. OH mixing ratios are enhanced in aircraft wakes due to the photolysis of the HONO that is made close to the engine. Measurements of HO(x) in aircraft wakes, along with NO(x) measurements, thus provides a constraint on chemical models of the engine combustion and exhaust. The development of the Airborne Tropospheric Hydrogen Oxides Sensor (ATHOS) is reported. We designed, developed, and successfully flew this instrument. It was part of the instrument complement on board the NASA DC-8 during SUCCESS, which took place in Kansas in April and May, 1996. ATHOS has a limit-of-detection for OH (S/N = 2) of 10(exp 5) OH molecules cm(exp -3) in less than 150 seconds. While this sensitivity is about 2-3 times less than the initial projections in the proposal, it is more than adequate for good measurements of OH and HO2 from the planetary boundary layer to the stratosphere. Our participation in SUCCESS was to be engineering test flights for ATHOS; however, the high-quality measurements we obtained are being used to study HO(x) photochemistry in contrails, clouds, and the clear air.

Understanding tropical upper tropospheric warming: The role of SSTs, convective parameterizations, and observational uncertainties

NASA Astrophysics Data System (ADS)

Po-Chedley, S.; Thorsen, T. J.; Fu, Q.

2015-12-01

Recent research has compared CMIP5 general circulation model (GCM) simulations with satellite observations of warming in the tropical upper troposphere relative to the lower-middle troposphere. Although the pattern of SST warming is important, this research demonstrated that models overestimate increases in static stability between the mid- to upper- tropical troposphere, even when they are forced with historical sea surface temperatures. This discrepancy between satellite-borne microwave sounding unit measurements (MSU) and GCMs is important because it has implications for the strength of the lapse rate and water vapor feedback. The apparent model-observational difference for changes in static stability in the tropical upper troposphere represents an important problem, but it is not clear whether the difference is a result of common biases in GCMs, biases in observational datasets, or both. In this work, we will use GCM simulations to examine the importance of the spatial pattern of SST warming and different convective parameterizations in determining the lapse rate changes in tropical troposphere. We will also consider uncertainties in MSU satellite observations, including changes in the diurnal sampling of temperature and instrument calibration biases when comparing GCMs with the observed record.

SOA YIELDS AND ORGANIC PRODUCT DISTRIBUTION FROM NATURAL HYDROCARBON/NOX IRRADIATIONS

EPA Science Inventory

Secondary organic aerosol (SOA) typically comprises one-quarter to one-third of the ambient aerosol mass in summertime urban atmospheres. In tropospheric environments, the main precursors of SOA come from aromatic and natural hydrocarbons. Recent work by various investigators...

Quantifying the Causes of Differences in Tropospheric OH Within Global Models

NASA Technical Reports Server (NTRS)

Nicely, Julie M.; Salawitch, Ross J.; Canty, Timothy; Anderson, Daniel C.; Arnold, Steve R.; Chipperfield, Martyn P.; Emmons, Louisa K.; Flemming, Johannes; Huijnen, Vincent; Kinnison, Douglas E.;

Chemistry-Transport Modeling of the Satellite Observed Distribution of Tropical Tropospheric Ozone

NASA Technical Reports Server (NTRS)

Peters, Wouter; Krol, Maarten; Dentener, Frank; Thompson, Anne M.; Leloeveld, Jos; Bhartia, P. K. (Technical Monitor)

2002-01-01

We have compared the 14-year record of satellite derived tropical tropospheric ozone columns (TTOC) from the NIMBUS-7 Total Ozone Mapping Spectrometer (TOMS) to TTOC calculated by a chemistry-transport model (CTM). An objective measure of error, based on the zonal distribution of TTOC in the tropics, is applied to perform this comparison systematically. In addition, the sensitivity of the model to several key processes in the tropics is quantified to select directions for future improvements. The comparisons indicate a widespread, systematic (20%) discrepancy over the tropical Atlantic Ocean, which maximizes during austral Spring. Although independent evidence from ozonesondes shows that some of the disagreement is due to satellite over-estimate of TTOC, the Atlantic mismatch is largely due to a misrepresentation of seasonally recurring processes in the model. Only minor differences between the model and observations over the Pacific occur, mostly due to interannual variability not captured by the model. Although chemical processes determine the TTOC extent, dynamical processes dominate the TTOC distribution, as the use of actual meteorology pertaining to the year of observations always leads to a better agreement with TTOC observations than using a random year or a climatology. The modeled TTOC is remarkably insensitive to many model parameters due to efficient feedbacks in the ozone budget. Nevertheless, the simulations would profit from an improved biomass burning calendar, as well as from an increase in NOX abundances in free tropospheric biomass burning plumes. The model showed the largest response to lightning NOX emissions, but systematic improvements could not be found. The use of multi-year satellite derived tropospheric data to systematically test and improve a CTM is a promising new addition to existing methods of model validation, and is a first step to integrating tropospheric satellite observations into global ozone modeling studies. Conversely,the CTM may suggest improvements to evolving satellite retrievals for tropospheric ozone.

Regional modeling of tropospheric NO2 vertical column density over East Asia during the period 2000-2010: comparison with multisatellite observations

NASA Astrophysics Data System (ADS)

Itahashi, S.; Uno, I.; Irie, H.; Kurokawa, J.-I.; Ohara, T.

2014-04-01

Satellite observations of the tropospheric NO2 vertical column density (VCD) are closely correlated to, and thus can be used to estimate, surface NOx emissions. In this study, the NO2 VCD simulated by a regional chemical transport model with emissions data from the updated Regional Emission inventory in ASia (REAS) version 2.1 were validated through comparison with multisatellite observations during the period 2000-2010. Rapid growth in NO2 VCD (~11% year-1) driven by the expansion of anthropogenic NOx emissions was identified above the central eastern China (CEC) region, except for the period during the economic downturn. In contrast, slightly decreasing trends (~2% year-1) were identified above Japan accompanied by a decline in anthropogenic emissions. To systematically compare the modeled NO2 VCD, we estimated sampling bias and the effect of applying the averaging kernel information, with particular focus on the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) data. Using the updated REAS, the modeled NO2 VCD reasonably reproduced annual trends observed by multisatellites, suggesting that the rate of increase of NOx emissions estimated by the updated REAS inventory would be robust. Province-scale revision of emissions above CEC is needed to further refine emission inventories. Based on the close linear relationship between modeled and observed NO2 VCD and anthropogenic NOx emissions, NOx emissions in 2009 and 2010, which were not covered by the updated REAS inventory, were estimated. NOx emissions from anthropogenic sources in China in 2009 and 2010 were determined to be 26.4 and 28.5 Tg year-1, respectively, indicating that NOx emissions increased more than twofold between 2000 and 2010. This increase reflected the strong growth of anthropogenic emissions in China following the rapid recovery from the economic downturn from late 2008 until mid-2009. Our method consists of simple estimations from satellite observations and provides results that are consistent with the most recent inventory of emissions data for China.

Hydrogen Radicals, Nitrogen Radicals, and the Production of O3 in the Upper Troposphere

NASA Technical Reports Server (NTRS)

Wennberg, P. O.; Hanisco, T. F.; Jaegle, L.; Jacob, D. J.; Hintsa, E. J.; Lanzendorf, E. J.; Anderson, J. G.; Gao, R.-S.; Keim, E. R.; Donnelly, S. G.;

The Distribution of Lightning Channel Lengths in Northern Alabama Thunderstorms

NASA Technical Reports Server (NTRS)

Peterson, H. S.; Koshak, W. J.

2010-01-01

Lightning is well known to be a major source of tropospheric NOx, and in most cases is the dominant natural source (Huntreiser et al 1998, Jourdain and Hauglustaine 2001). Production of NOx by a segment of a lightning channel is a function of channel segment energy density and channel segment altitude. A first estimate of NOx production by a lightning flash can be found by multiplying production per segment [typically 104 J/m; Hill (1979)] by the total length of the flash s channel. The purpose of this study is to determine average channel length for lightning flashes near NALMA in 2008, and to compare average channel length of ground flashes to the average channel length of cloud flashes.

Lidar investigations of ozone in the upper troposphere - lower stratosphere: technique and results of measurements

NASA Astrophysics Data System (ADS)

Romanovskii, Oleg A.; Nevzorov, Alexey A.; Nevzorov, Alexey V.; Kharchenko, Olga V.

2018-04-01

The main aim of the research is to develop the technique for laser remote ozone sensing in the upper troposphere - lower stratosphere by differential absorption method for temperature and aerosol correction and analysis of measurement results. The authors have determined wavelengths, promising to measure ozone profiles in the upper troposphere - lower stratosphere. We present the results of DIAL measurements of the vertical ozone distribution at the Siberian lidar station in Tomsk. The recovered ozone profiles were compared with IASI satellite data and Kruger model.

Characterization of ozone in the lower troposphere during the 2016 G20 conference in Hangzhou.

PubMed

Su, Wenjing; Liu, Cheng; Hu, Qihou; Fan, Guangqiang; Xie, Zhouqing; Huang, Xin; Zhang, Tianshu; Chen, Zhenyi; Dong, Yunsheng; Ji, Xiangguang; Liu, Haoran; Wang, Zhuang; Liu, Jianguo

2017-12-12

Recently, atmospheric ozone pollution has demonstrated an aggravating tendency in China. To date, most research about atmospheric ozone has been confined near the surface, and an understanding of the vertical ozone structure is limited. During the 2016 G20 conference, strict emission control measures were implemented in Hangzhou, a megacity in the Yangtze River Delta, and its surrounding regions. Here, we monitored the vertical profiles of ozone concentration and aerosol extinction coefficients in the lower troposphere using an ozone lidar, in addition to the vertical column densities (VCDs) of ozone and its precursors in the troposphere through satellite-based remote sensing. The ozone concentrations reached a peak near the top of the boundary layer. During the control period, the aerosol extinction coefficients in the lower lidar layer decreased significantly; however, the ozone concentration fluctuated frequently with two pollution episodes and one clean episode. The sensitivity of ozone production was mostly within VOC-limited or transition regimes, but entered a NOx-limited regime due to a substantial decline of NOx during the clean episode. Temporary measures took no immediate effect on ozone pollution in the boundary layer; instead, meteorological conditions like air mass sources and solar radiation intensities dominated the variations in the ozone concentration.

Analysis of alternative pathways for reducing nitrogen oxide emissions.

PubMed

Loughlin, Daniel H; Kaufman, Katherine R; Lenox, Carol S; Hubbell, Bryan J

2015-09-01

Strategies for reducing tropospheric ozone (O3) typically include modifying combustion processes to reduce the formation of nitrogen oxides (NOx) and applying control devices that remove NOx from the exhaust gases of power plants, industrial sources and vehicles. For portions of the U.S., these traditional controls may not be sufficient to achieve the National Ambient Air Quality Standard for ozone. We apply the MARKet ALlocation (MARKAL) energy system model in a sensitivity analysis to explore whether additional NOx reductions can be achieved through extensive electrification of passenger vehicles, adoption of energy efficiency and conservation measures within buildings, and deployment of wind and solar power in the electric sector. Nationally and for each region of the country, we estimate the NOx implications of these measures. Energy efficiency and renewable electricity are shown to reduce NOx beyond traditional controls. Wide-spread light duty vehicle electrification produces varied results, with NOx increasing in some regions and decreasing in others. However, combining vehicle electrification with renewable electricity reduces NOx in all regions. State governments are charged with developing plans that demonstrate how air quality standards will be met and maintained. The results presented here provide an indication of the national and regional NOx reductions available beyond traditional controls via extensive adoption of energy efficiency, renewable electricity, and vehicle electrification.

Relationship between changes in the upper and lower tropospheric water vapor: A revisit

NASA Astrophysics Data System (ADS)

Yang, M.; Sun, D. Z.; Zhang, G. J.

2017-12-01

Upper tropospheric water vapor response to enhanced greenhouse gas forcing is as important as the lower tropospheric water vapor response in determining climate sensitivity. Early studies using older versions of climate models have suggested that the upper- and lower-troposphere water vapor changes are more strongly coupled in the climate models than in the observations. Here we reexamine this issue using a state-of-the-art climate model—the NCAR community model CAM5. Specifically, we have calculated the correlations between interannual variations of specific humidity in all levels of the troposphere with that at the surface in CAM5 and in the observations (as represented by the updated ERA-Interim and NCEP reanalysis). It is found that the previously noted biases in how strongly upper tropospheric water vapor and lower troposphere water vapor are linked still exist in CAM5—the change in the tropical averaged upper tropospheric water vapor is more strongly correlated with the change in the surface. However, this bias disappears in the averaged correlation obtained by averaging the point-by-point correlations over the tropics. The spatial pattern of the point-by-point correlations reveals that the better agreement between the model and the observations is related to the opposite model biases in different regions: the correlation is weaker in the model in the western Pacific, but stronger in the central and eastern Pacific. Further analysis of precipitation fields suggests that the weaker (stronger) coupling between tropospheric water vapor and surface moisture over western (central-eastern) Pacific in model is related to weaker (stronger) simulated convective activities in these regions. More specifically, during El Nino, the model has excessive deep convection in the central Pacific, but too littler deep convection in western Pacific. Implications of the results are discussed in the context of climate change as well as in the context of how to improve the model in this regard.

Concentrations of ethane (C2H6) in the lower stratosphere and upper troposphere and acetylene (C2H2) in the upper troposphere deduced from Atmospheric Trace Molecule Spectroscopy/Spacelab 3 spectra

NASA Technical Reports Server (NTRS)

Rinsland, C. P.; Russell, J. M., III; Zander, R.; Farmer, C. B.; Norton, R. H.

1987-01-01

This paper reports the results of the spectroscopic analysis of C2H6 and C2H2 absorption spectra obtained by the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument flown on the Shuttle as part of the Spacelab 3 mission. The spectra were recorded during sunset occultations occurring between 25 deg N and 31 deg N latitudes, yielding volume-mixing ratio profiles of C2H6 in the lower stratosphere and the upper troposphere, and an upper tropospheric profile of C2H2. These results compare well with previous in situ and remote sounding data obtained at similar latitudes and with model calculations. The results demonstrate the feasibility of the ATMOS instrument to sound the lower atmosphere from space.

HALOE Algorithm Improvements for Upper Tropospheric Sounding

NASA Technical Reports Server (NTRS)

Thompson, Robert Earl; McHugh, Martin J.; Gordley, Larry L.; Hervig, Mark E.; Russell, James M., III; Douglass, Anne (Technical Monitor)

2001-01-01

This report details the ongoing efforts by GATS, Inc., in conjunction with Hampton University and University of Wyoming, in NASA's Mission to Planet Earth Upper Atmospheric Research Satellite (UARS) Science Investigator Program entitled 'HALOE Algorithm Improvements for Upper Tropospheric Sounding.' The goal of this effort is to develop and implement major inversion and processing improvements that will extend Halogen Occultation Experiment (HALOE) measurements further into the troposphere. In particular, O3, H2O, and CH4 retrievals may be extended into the middle troposphere, and NO, HCl and possibly HF into the upper troposphere. Key areas of research being carried out to accomplish this include: pointing/tracking analysis; cloud identification and modeling; simultaneous multichannel retrieval capability; forward model improvements; high vertical-resolution gas filter channel retrievals; a refined temperature retrieval; robust error analyses; long-term trend reliability studies; and data validation. The current (first year) effort concentrates on the pointer/tracker correction algorithms, cloud filtering and validation, and multichannel retrieval development. However, these areas are all highly coupled, so progress in one area benefits from and sometimes depends on work in others.

A NASA Lightning Parameterization for CMAQ

NASA Technical Reports Server (NTRS)

Koshak, William; Khan, Maudood; Biazar, Arastoo; Newchurch, Mike; McNider, Richard

2009-01-01

Many state and local air quality agencies use the U.S. Environmental Protection Agency (EPA) Community Multiscale Air Quality (CMAQ) modeling system to determine compliance with the National Ambient Air Quality Standards (NAAQS). Because emission reduction scenarios are tested using CMAQ with an aim of determining the most efficient and cost effective strategies for attaining the NAAQS, it is very important that trace gas concentrations derived by CMAQ are accurate. Overestimating concentrations can literally translate into billions of dollars lost by commercial and government industries forced to comply with the standards. Costly health, environmental and socioeconomic problems can result from concentration underestimates. Unfortunately, lightning modeling for CMAQ is highly oversimplified. This leads to very poor estimates of lightning-produced nitrogen oxides "NOx" (= NO + NO2) which directly reduces the accuracy of the concentrations of important CMAQ trace gases linked to NOx concentrations such as ozone and methane. Today it is known that lightning is the most important NOx source in the upper troposphere with a global production rate estimated to vary between 2-20 Tg(N)/yr. In addition, NOx indirectly influences our climate since it controls the concentration of ozone and hydroxyl radicals (OH) in the atmosphere. Ozone is an important greenhouse gas and OH controls the oxidation of various greenhouse gases. We describe a robust NASA lightning model, called the Lightning Nitrogen Oxides Model (LNOM) that combines state-of-the-art lightning measurements, empirical results from field studies, and beneficial laboratory results to arrive at a realistic representation of lightning NOx production for CMAQ. NASA satellite lightning data is used in conjunction with ground-based lightning detection systems to assure that the best representation of lightning frequency, geographic location, channel length, channel altitude, strength (i.e., channel peak current), and number of strokes per flash are accounted for. LNOM combines all of these factors in a straightforward approach that is easily implemented into CMAQ. We anticipate that future applications of LNOM will produce significant and important changes in CMAQ trace gas concentrations for various regions and times. We also anticipate that these changes will have a direct impact on decision makers responsible for NAAQS attainment.

Quasi-biweekly oscillations of the South Asian monsoon and its co-evolution in the upper and lower troposphere

NASA Astrophysics Data System (ADS)

Ortega, Sebastián; Webster, Peter J.; Toma, Violeta; Chang, Hai-Ru

2017-11-01

The Upper Tropospheric Quasi-Biweekly Oscillation (UQBW) of the South Asian monsoon is studied using the potential vorticity field on the 370 K isentrope. The UQBW is shown to be a common occurrence in the upper troposphere during the monsoon, and its typical evolution is described. We suggest that the UQBW is a phenomenon of both the middle and tropical latitudes, owing its existence to the presence of the planetary-scale upper-tropospheric monsoon anticyclone. The UQBW is first identified as Rossby waves originating in the northern flank of the monsoon anticyclone. These Rossby waves break when reaching the Pacific Ocean, and their associated cyclonic PV anomalies move southward to the east of Asia and then westward across the Indian Ocean and Africa advected by the monsoon anticyclone. A strong correlation, or co-evolution, between the UQBW and quasi-biweekly oscillations in the lower troposphere (QBW) is also found. In particular, analysis of vertically-integrated horizontal moisture transport, 850 hPa geopotential, and outgoing long-wave radiation show that the UQBW is usually observed at the same time as, and co-evolves with, the lower tropospheric QBW over South Asia. We discuss the nature of the UQBW, and its possible physical link with the QBW.

Observation of NO(x) Enhancement and Ozone Depletion in the Northern and Southern hemispheres after the October-November 2003 Solar Proton Events

NASA Technical Reports Server (NTRS)

Lopez-Puertas, M.; Funke, B.; Gil-Lopez, S.; vonClarmann, T.; Stiller, G. P.; Hoepfner, M.; Kellmann, S.; Fischer, H.; Jackman, C. H.

2005-01-01

The large solar storms in October-November 2003 produced enormous solar proton events (SPEs) where high energetic particles reached the Earth and penetrated into the middle atmosphere in the polar regions. At this time, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) was observing the atmosphere in the 6-68 km altitude range. MIPAS observations of NO(x) (NO+NO2) and O3 of the period from 25 October to 14 November 2003 are the first global measurements of NO(x) species, covering both the summer (daylight) and winter (dark) polar regions during an SPE. Very large values of NO(x) in the upper stratosphere of 180 ppbv (parts per billion by volume) have been measured, and a large asymmetry in Northern and Southern polar cap NO(x) enhancements was found. Arctic mean polar cap (>60 deg) NO(x) enhancements of 20 to 70 ppbv between 40 to 60 km lasted for at least two weeks, while the Antarctic mean NO(x) enhancement was between 10 and 35 ppbv and was halved after two weeks. Ozone shows depletion signatures associated with both HO(x) (H+OH+HO2) and NO(x) enhancements but at different time scales. Arctic lower mesospheric (upper stratospheric) ozone is reduced by 50-70% (30-40%) for about two weeks The large solar storms in October-November 2003 produced after the SPEs. A smaller ozone depletion signal was observed in the Antarctic atmosphere. After the locally produced Arctic middle and upper stratospheric as well as mesospheric NO(x) enhancement, large amounts of NO(x) were observed until the end of December. These are explained by downward transport processes.

RESEARCH AREA -- MOBILE SOURCE EMISSIONS (EMISSIONS CHARACTERIZATION AND PREVENTION BRANCH, APPCD, NRMRL)

EPA Science Inventory

The objective of this program is to characterize mobile source emissions which are one of the largest sources of tropospheric ozone precursor emissions (CO, NOx, and volotile organic compounds) in the U.S. The research objective of the Emissions Characterization and Prevention Br...

Influence of isoprene chemical mechanism on modelled changes in tropospheric ozone due to climate and land use over the 21st century

NASA Astrophysics Data System (ADS)

Squire, O. J.; Archibald, A. T.; Griffiths, P. T.; Jenkin, M. E.; Pyle, J. A.

2014-09-01

Isoprene is a precursor to tropospheric ozone, a key pollutant and greenhouse gas. Anthropogenic activity over the coming century is likely to cause large changes in atmospheric CO2 levels, climate and land use, all of which will alter the global vegetation distribution leading to changes in isoprene emissions. Previous studies have used global chemistry-climate models to assess how possible changes in climate and land use could affect isoprene emissions and hence tropospheric ozone. The chemistry of isoprene oxidation, which can alter the concentration of ozone, is highly complex, therefore it must be parameterised in these models. In this work we compare the effect of four different reduced isoprene chemical mechanisms, all currently used in Earth-system models, on tropospheric ozone. Using a box model we compare ozone in these reduced schemes to that in a more explicit scheme (the MCM) over a range of NOx and isoprene emissions, through the use of O3 isopleths. We find that there is some variability, especially at high isoprene emissions, caused by differences in isoprene-derived NOx reservoir species. A global model is then used to examine how the different reduced schemes respond to potential future changes in climate, isoprene emissions, anthropogenic emissions and land use change. We find that, particularly in isoprene rich regions, the response of the schemes varies considerably. The wide ranging response is due to differences in the types of peroxy radicals produced by isoprene oxidation, and their relative rates of reaction towards NO, leading to ozone formation, or HO2, leading to termination. Also important is the yield of isoprene-nitrates and peroxyacyl nitrate precursors from isoprene oxidation. Those schemes that produce less of these NOx reservoir species, tend to produce more ozone locally and less away from the source region. Additionally, by combining the emissions and O3 data from all of the global model integrations, we are able to construct isopleth plots comparable to those from the box model analysis. We find that the global and box model isopleths show good qualitative agreement, suggesting that comparing chemical mechanisms with a box model in this framework is a useful tool for assessing mechanistic performance in complex global models. We conclude that as the choice of reduced isoprene mechanism may alter both the magnitude and sign of the ozone response, how isoprene chemistry is parameterised in perturbation experiments such as these is a crucially important consideration. More measurements are needed to validate these reduced mechanisms especially in high-VOC, low-NOx environments.

The potential impact on atmospheric ozone and temperature of increasing trace gas concentrations

NASA Technical Reports Server (NTRS)

Brasseur, G.; Derudder, A.

1987-01-01

The response of the atmosphere to emissions of chlorofluorocarbons (CFCs) and other chlorocarbons, and to increasing concentrations of other radiatively active trace gases such as CO2, CH4, and N2O is calculated by a coupled chemical-radiative transport one-dimensional model. It is shown that significant reductions in the ozone concentration and in the temperature are expected in the upper stratosphere as a result of increasing concentrations of active chlorine produced by photodecomposition of the CFCs. The ozone content is expected to increase in the troposphere, as a consequence of increasing concentrations of methane and nitrogen oxides. Due to enhanced greenhouse effects, the Earth's surface should warm up by several degrees. The amplitude and even the sign of future changes in the ozone column are difficult to predict as they are strongly scenario-dependent. An early detection system to prevent noticeable ozone changes as a result of increasing concentrations of source gases should thus be based on a continuous monitoring of the ozone amount in the upper stratosphere rather than on measurements of the ozone column only. Measurements of NOx, Clx, and HOx are also required for unambiguous trend detection and interpretation.

Characterization of tropospheric ozone based on lidar measurement in Hangzhou, East China during the G20 Leaders' Summit

NASA Astrophysics Data System (ADS)

Su, Wenjing; Liu, Cheng; Fan, Guangqiang; Hu, Qihou; Huang, Xin; Dong, Yunsheng; Zhang, Tianshu; Liu, Jianguo

2017-04-01

Owing to the G20 (Group of Twenty Finance Ministers and Central Bank Governors) Leaders' Summit (Sep.5th-6th, 2016), a series of strict air quality control measures were implemented in Hangzhou and its surrounding regions from Aug.26th to Sep.6th. A differential absorption lidar was employed to monitor tropospheric ozone in urban Hangzhou during a campaign from Aug. 24th to Sep. 10th, and the satellite-based NO2 VCDs and HCHO VCDs in the troposphere were also retrieved using the Ozone Monitoring Instrument (OMI). During our campaign, six O3 pollution events, which were determined according to the National Ambient Air Quality Standard of China (GB-3095-2012), and two stages with rapid reduction of O3 concentration on Aug. 26th and Sep.4-6th were observed. The temporal variation tendency of O3 concentrations was well reproduced by the Weather Research and Forecasting model coupled with chemistry (WRF-Chem). Typical cases with the abrupt rise and decline of O3 concentrations were analyzed using Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) back trajectory, satellite NO2 and HCHO product and the prediction by WRF-Chem model. The transport from northern cities have an important impact on pollutants observed in Hangzhou, and the chemical sensitivity of O3 production, which were approximately evaluated using the ratio of HCHO VCDs to NO2 VCDs in the troposphere, was turned from a mixed VOC-NOx-limited regime into a NOX-limited regime in Hangzhou due to the strict emission control measures.

Stratospheric Aerosol and Gas Experiment (SAGE) II and III Aerosol Extinction Measurements in the Arctic Middle and Upper Troposphere

NASA Technical Reports Server (NTRS)

Treffeisen, R. E.; Thomason, L. W.; Strom, J.; Herber, A. B.; Burton, S. P.; Yamanouchi, T.

2006-01-01

In recent years, substantial effort has been expended toward understanding the impact of tropospheric aerosols on Arctic climate and chemistry. A significant part of this effort has been the collection and documentation of extensive aerosol physical and optical property data sets. However, the data sets present significant interpretive challenges because of the diverse nature of these measurements. Among the longest continuous records is that by the spaceborne Stratospheric Aerosol and Gas Experiment (SAGE) II. Although SAGE tropospheric measurements are restricted to the middle and upper troposphere, they may be able to provide significant insight into the nature and variability of tropospheric aerosol, particularly when combined with ground and airborne observations. This paper demonstrates the capacity of aerosol products from SAGE II and its follow-on experiment SAGE III to describe the temporal and vertical variations of Arctic aerosol characteristics. We find that the measurements from both instruments are consistent enough to be combined. Using this combined data set, we detect a clear annual cycle in the aerosol extinction for the middle and upper Arctic troposphere.

Use of On-Line Tracers as a Diagnostic Tool in General Circulation Model Development. 2; Transport Between the Troposphere and Stratosphere

NASA Technical Reports Server (NTRS)

Rind, David H.; Lerner, Jean; Shah, Kathy; Suozzo, Robert

1999-01-01

A key component of climate/chemistry modeling is how to handle the influx into (and egress from) the troposphere. This is especially important when considering tropospheric ozone, and its precursors (e.g., NO(x) from aircraft). A study has been conducted with various GISS models to determine the minimum requirements necessary for producing realistic troposphere-stratosphere exchange. Four on-line tracers are employed: CFC-11 and SF6 for mixing from the troposphere into the stratosphere, Rn222 for vertical mixing within the troposphere, and 14C for mixing from the stratosphere into the troposphere. Four standard models are tested, with varying vertical resolution, gravity wave drag and location of the model top, and additional subsidiary models are employed to examine specific features. The results show that proper vertical transport between the troposphere and stratosphere in the GISS models requires lifting the top of the model considerably out of the stratosphere, and including gravity wave drag in the lower stratosphere. Increased vertical resolution without these aspects does not improve troposphere-stratosphere exchange. The transport appears to be driven largely by the residual circulation within the stratosphere; associated E-P flux convergences require both realistic upward propagating energy from the troposphere, and realistic pass-through possibilities. A 23 layer version with a top at the mesopause and incorporating gravity wave drag appears to have reasonable stratospheric-tropospheric exchange, in terms of both the resulting tracer distributions and atmospheric mass fluxes.

Stratospheric aerosols from the Sarychev volcano eruption in the 2009 Arctic summer

NASA Astrophysics Data System (ADS)

Jégou, F.; Berthet, G.; Brogniez, C.; Renard, J.-B.; François, P.; Haywood, J. M.; Jones, A.; Bourgeois, Q.; Lurton, T.; Auriol, F.; Godin-Beekmann, S.; Guimbaud, C.; Krysztofiak, G.; Gaubicher, B.; Chartier, M.; Clarisse, L.; Clerbaux, C.; Balois, J. Y.; Verwaerde, C.

2013-02-01

Aerosols from the Sarychev volcano eruption (Kuril Islands, northeast of Japan) were observed in the Arctic lower stratosphere a few days after the strongest SO2 injection which occurred on 15 and 16 June 2009. From the observations provided by the Infrared Atmospheric Sounding Interferometer (IASI) an estimated 0.9 Tg of sulphur dioxide was injected into the Upper Troposphere and Lower Stratosphere (UTLS). The resultant stratospheric sulphate aerosols were detected by the Optical Spectrograph and Infrared Imaging System (OSIRIS) limb sounder and by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instruments. By the first week of July the aerosol plume had spread out over the entire Arctic region. The Sarychev-induced stratospheric aerosol over the Kiruna region (north of Sweden) was measured by the Stratospheric and Tropospheric Aerosol Counter (STAC) during eight balloon flights planned in August and September 2009. During this balloon campaign the Micro RADIomètre BALlon (MicroRADIBAL) and the Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NOx (SALOMON) remote-sensing instruments also observed these aerosols. Aerosol concentrations returned to near-background levels by spring 2010. The effective radius, the Surface Area Density (SAD), the aerosol extinction, and the total sulphur mass from STAC in situ measurements are enhanced with mean values in the range 0.15-0.21 μm, 5.5-14.7 μm2 cm-3, 5.5-29.5×10-4 km-1, and 4.9-12.6×10-10 kg [S] kg-1 [air], respectively, between 14 km and 18 km. The observed and modelled e-folding time of sulphate aerosols from the Sarychev eruption is around 70-80 days, a value much shorter than the 12-14 months calculated for aerosols from the 1991 eruption of Mt. Pinatubo. The OSIRIS stratospheric Aerosol Optical Depth (AOD) at 750 nm is enhanced by a factor of 6 with a value of 0.02 in late July compared to 0.0035 before the eruption. The HadGEM2 and MIMOSA model outputs indicate that aerosol layers in polar region up to 14-15 km are largely modulated by stratosphere-troposphere exchange processes. The spatial extension of the Sarychev plume is well represented in the HadGEM2 model with lower altitudes of the plume being controlled by upper tropospheric troughs which displace the plume downward and upper altitudes around 18-20 km in agreement with lidar observations. A good consistency is found between the HadGEM2 sulphur mass density and the value inferred from the STAC observations with a maximum located about 1 km above the tropopause ranging from 1 to 2×10-9 kg [S] kg-1 [air], which is one order of magnitude higher than the background level.

Upper-Tropospheric Winds Derived from Geostationary Satellite Water Vapor Observations

NASA Technical Reports Server (NTRS)

Velden, Christopher S.; Hayden, Christopher M.; Nieman, Steven J.; Menzel, W. Paul; Wanzong, Steven; Goerss, James S.

1997-01-01

The coverage and quality of remotely sensed upper-tropospheric moisture parameters have improved considerably with the deployment of a new generation of operational geostationary meteorological satellites: GOES-8/9 and GMS-5. The GOES-8/9 water vapor imaging capabilities have increased as a result of improved radiometric sensitivity and higher spatial resolution. The addition of a water vapor sensing channel on the latest GMS permits nearly global viewing of upper-tropospheric water vapor (when joined with GOES and Meteosat) and enhances the commonality of geostationary meteorological satellite observing capabilities. Upper-tropospheric motions derived from sequential water vapor imagery provided by these satellites can be objectively extracted by automated techniques. Wind fields can be deduced in both cloudy and cloud-free environments. In addition to the spatially coherent nature of these vector fields, the GOES-8/9 multispectral water vapor sensing capabilities allow for determination of wind fields over multiple tropospheric layers in cloud-free environments. This article provides an update on the latest efforts to extract water vapor motion displacements over meteorological scales ranging from subsynoptic to global. The potential applications of these data to impact operations, numerical assimilation and prediction, and research studies are discussed.

Investigation of shortcomings in simulated aerosol vertical profiles

NASA Astrophysics Data System (ADS)

Park, S.; Allen, R.

2017-12-01

The vertical distribution of aerosols is one important factor for aerosol radiative forcing. Previous studies show that climate models poorly reproduce the aerosol vertical profile, with too much aerosol aloft in the upper troposphere. This bias may be related to several factors, including excessive convective mass flux and wet removal. In this study, we evaluate the aerosol vertical profile from several Coupled Model Intercomparison Project 5 (CMIP5) models, as well as the Community Atmosphere Model 5 (CAM5), relative to the Cloud-Aerosol Lidar Infrared Pathfinder Satellite Observation (CALIPSO). The results show that all models significantly underestimate extinction coefficient in the lower troposphere, while overestimating extinction coefficient in the upper troposphere. In addition, the majority of models indicate a land-ocean dependence in the relationship between aerosol extinction coefficient in the upper troposphere and convective mass flux. Over the continents, more convective mass flux is related to more aerosol aloft; over the ocean, more convective mass flux is associated with less aerosol in upper troposphere. Sensitivity experiments are conducted to investigate the role that convection and wet deposition have in contributing to the deficient simulation of the vertical aerosol profile, including the land-ocean dependence.

Reanalysis comparisons of upper tropospheric-lower stratospheric jets and multiple tropopauses

NASA Astrophysics Data System (ADS)

Manney, Gloria L.; Hegglin, Michaela I.; Lawrence, Zachary D.; Wargan, Krzysztof; Millán, Luis F.; Schwartz, Michael J.; Santee, Michelle L.; Lambert, Alyn; Pawson, Steven; Knosp, Brian W.; Fuller, Ryan A.; Daffer, William H.

2017-09-01

The representation of upper tropospheric-lower stratospheric (UTLS) jet and tropopause characteristics is compared in five modern high-resolution reanalyses for 1980 through 2014. Climatologies of upper tropospheric jet, subvortex jet (the lowermost part of the stratospheric vortex), and multiple tropopause frequency distributions in MERRA (Modern-Era Retrospective analysis for Research and Applications), ERA-I (ERA-Interim; the European Centre for Medium-Range Weather Forecasts, ECMWF, interim reanalysis), JRA-55 (the Japanese 55-year Reanalysis), and CFSR (the Climate Forecast System Reanalysis) are compared with those in MERRA-2. Differences between alternate products from individual reanalysis systems are assessed; in particular, a comparison of CFSR data on model and pressure levels highlights the importance of vertical grid spacing. Most of the differences in distributions of UTLS jets and multiple tropopauses are consistent with the differences in assimilation model grids and resolution - for example, ERA-I (with coarsest native horizontal resolution) typically shows a significant low bias in upper tropospheric jets with respect to MERRA-2, and JRA-55 (the Japanese 55-year Reanalysis) a more modest one, while CFSR (with finest native horizontal resolution) shows a high bias with respect to MERRA-2 in both upper tropospheric jets and multiple tropopauses. Vertical temperature structure and grid spacing are especially important for multiple tropopause characterizations. Substantial differences between MERRA and MERRA-2 are seen in mid- to high-latitude Southern Hemisphere (SH) winter upper tropospheric jets and multiple tropopauses as well as in the upper tropospheric jets associated with tropical circulations during the solstice seasons; some of the largest differences from the other reanalyses are seen in the same times and places. Very good qualitative agreement among the reanalyses is seen between the large-scale climatological features in UTLS jet and multiple tropopause distributions. Quantitative differences may, however, have important consequences for transport and variability studies. Our results highlight the importance of considering reanalyses differences in UTLS studies, especially in relation to resolution and model grids; this is particularly critical when using high-resolution reanalyses as an observational reference for evaluating global chemistry-climate models.

Hydrogen Radicals, Nitrogen Radicals, and the Production of Ozone in the Middle and Upper Troposphere

NASA Technical Reports Server (NTRS)

Bui, T. P.

1997-01-01

The concentrations of hydrogen radicals, OH and HO2, in the middle and upper troposphere were measured simultaneously with those of NO, O3,CO, H20, CH4, non-methane hydrocarbons, and with the ultraviolet and visible radiation field.

Understanding the Laminar Distribution of Tropospheric Ozone from Ground-Based, Airborne, Spaceborne, and Modeling Perspectives

NASA Technical Reports Server (NTRS)

Newchurch, Mike; Johnson, Matthew S.; Huang, Guanyu; Kuang, Shi; Wang, Lihua; Chance, Kelly; Liu, Xiong

2016-01-01

Laminar ozone structure is a ubiquitous feature of tropospheric-ozone distributions resulting from dynamic and chemical atmospheric processes. Understanding the characteristics of these ozone laminae and the mechanisms responsible for producing them is important to outline the transport pathways of trace gases and to quantify the impact of different sources on tropospheric background ozone. In this study, we present a new method to detect ozone laminae to understand their climatological characteristics of occurrence frequency in terms of thickness and altitude. We employ both ground-based and airborne ozone lidar measurements and other synergistic observations and modeling to investigate the sources and mechanisms such as biomass burning transport, stratospheric intrusion, lightning-generated NOx, and nocturnal low-level jets that are responsible for depleted or enhanced tropospheric ozone layers. Spaceborne (e.g., OMI (Ozone Monitoring Instrument), TROPOMI (Tropospheric Monitoring Instrument), TEMPO (Tropospheric Emissions: Monitoring of Pollution)) measurements of these laminae will observe greater horizontal extent and lower vertical resolution than balloon-borne or lidar measurements will quantify. Using integrated ground-based, airborne, and spaceborne observations in a modeling framework affords insight into how to gain knowledge of both the vertical and horizontal evolution of these ubiquitous ozone laminae.

Modeled Full-Flight Aircraft Emissions Impacts on Air Quality and Their Sensitivity to Grid Resolution

EPA Science Inventory

Aviation is a unique anthropogenic source with four-dimensional varying emissions, peaking at cruise altitudes (9–12 km). Aircraft emission budgets in the upper troposphere lower stratosphere region and their potential impacts on upper troposphere and surface air quality ar...

Internal gravity waves in the upper atmosphere, generated by tropospheric jet streams

NASA Technical Reports Server (NTRS)

Chunchuzov, Y. P.; Torgashin, Y. M.

1979-01-01

A mechanism of internal gravity wave generation by jet streams in the troposphere is considered. Evaluations of the energy and pulse of internal gravity waves emitted into the upper atmosphere are given. The obtained values of flows can influence the thermal and dynamic regime of these layers.

Summertime partitioning and budget of NO(y) compounds in the troposphere over Alaska and Canada: ABLE 3B

NASA Technical Reports Server (NTRS)

Sandholm, S.; Olson, J.; Bradshaw, J.; Talbot, R.; Singh, H.; Gregory, G.; Blake, D.; Anderson, B.; Sachse, G.; Barrick, J.

1994-01-01

As part of NASA's Arctic Boundary Layer Expedition 3A and 3B field measurement programs, measurements of NO(x), HNO3, PAN, PPN, and NO(y) were made in the middle to lower troposphere over Alaska and Canada during the summers of 1988 and 1990. These measurements are used to assess the degree of closure within the reactive odd nitrogen (N(x)O(y)) budget through the comparison of the values of NO(y) measured with a catalytic convertor to the sum of individually measured NO(y) (i) compounds (i.e., sigmaNO(y)(i) = NO(x) + HNO3 + PAN + PPN). Significant differences were observed between the various study regions. In the lower 6 km of the troposphere over Alaska and the Hudson Bay lowlands of Canada a significant fraction of the NO(y) budget (30 to 60%) could not be accounted for by the measured sigmaNO(y)i. This deficit in the NO(y) budget is about 100 to 200 parts per trillion by volume (pptv) in the lower troposphere (0.15 to 3 km) and about 200 to 400 pptv in the middle free troposphere (3 to 6.2 km). Conversely, the NO(y) budget in the northern Labrador and Quebec regions of Canada is almost totally accounted for within the combined measurement uncertainties of NO(y) and the various NO(y)(i) compounds. A substantial portion of the NO(y) budget's 'missing compounds' appears to be coupled to the photochemical and/or dynamical parameters influencing the tropospheric oxidative potential over these regions. A combination of factors are suggested as the causes for the variability observed in the NO(y) budget. In addition, the apparent stability of compounds represented by the NO(y) budget deficit in the lower-altitude range questions the ability of these compounds to participate as reversible reservoirs for 'active' odd nitrogen and suggest that some portion of the NO(y) budget may consist of relatively unreactive nitrogen-containing compounds.

Space-Based Diagnosis of Surface Ozone Sensitivity to Anthropogenic Emissions

NASA Technical Reports Server (NTRS)

Martin, Randall V.; Fiore, Arlene M.; VanDonkelaar, Aaron

2004-01-01

We present a novel capability in satellite remote sensing with implications for air pollution control strategy. We show that the ratio of formaldehyde columns to tropospheric nitrogen dioxide columns is an indicator of the relative sensitivity of surface ozone to emissions of nitrogen oxides (NO(x) = NO + NO2) and volatile organic compounds (VOCs). The diagnosis from these space-based observations is highly consistent with current understanding of surface ozone chemistry based on in situ observations. The satellite-derived ratios indicate that surface ozone is more sensitive to emissions of NO(x) than of VOCs throughout most continental regions of the Northern Hemisphere during summer. Exceptions include Los Angeles and industrial areas of Germany. A seasonal transition occurs in the fall when surface ozone becomes less sensitive to NOx and more sensitive to VOCs.

A satellite view of the sources and interannual variability of free tropospheric PAN over the eastern Pacific Ocean during summer and its timeline for trend detection

NASA Astrophysics Data System (ADS)

Zhu, L.; Fischer, E. V.; Payne, V.; Walker, T. W.; Worden, J. R.; Jiang, Z.; Kulawik, S. S.

2016-12-01

Peroxyacetyl nitrate (PAN) is the most important reservoir for nitrogen oxide radicals (NOx = NO + NO2) in the troposphere and plays a significant role in the redistribution of NOx to remote regions. There is strong evidence that PAN decomposition in specific plumes of Asian origin subsiding over the eastern Pacific Ocean can lead to significant ozone (O3) enhancements in the troposphere. Thus quantifying the spatial and temporal variability of PAN over the eastern Pacific Ocean is an important part of understanding the O3 budget upwind of the North American airshed. Here we present observations of PAN from the Tropospheric Emission Spectrometer (TES) over the eastern Pacific for July 2006-2010. We focus our analysis on July because prior work based on in situ observations has primarily addressed the transpacific transport of PAN in spring. Plumes containing elevated PAN are present almost every day in the month of July, and we show that elevated PAN observed in July has multiple sources, including fires in Siberia, anthropogenic and lightning sources in eastern China, and re-circulated pollution from the continental U.S. We provide examples of each type of source using both HYPLIT trajectories and a GEOS-Chem adjoint sensitivity analysis. Based on the variability observed in the TES PAN retrievals over this region, we predict it would be faster to detect a trend of a given magnitude in PAN using satellite observations over the eastern Pacific Ocean region rather than surface in situ observations at one site, and that a trend of a given magnitude would be more quickly detected in summer than spring.

Photochemical ozone production in tropical squall line convection during NASA Global Tropospheric Experiment/Amazon Boundary Layer Experiment 2A

NASA Technical Reports Server (NTRS)

Pickering, Kenneth E.; Thompson, Anne M.; Tao, Wei-Kuo; Simpson, Joanne; Scala, John R.

1991-01-01

The role of convection was examined in trace gas transport and ozone production in a tropical dry season squall line sampled on August 3, 1985, during NASA Global Tropospheric Experiment/Amazon Boundary Layer Experiment 2A (NASA GTE/ABLE 2A) in Amazonia, Brazil. Two types of analyses were performed. Transient effects within the cloud are examined with a combination of two-dimensional cloud and one-dimensional photochemical modeling. Tracer analyses using the cloud model wind fields yield a series of cross sections of NO(x), CO, and O3 distribution during the lifetime of the cloud; these fields are used in the photochemical model to compute the net rate of O3 production. At noon, when the cloud was mature, the instantaneous ozone production potential in the cloud is between 50 and 60 percent less than in no-cloud conditions due to reduced photolysis and cloud scavenging of radicals. Analysis of cloud inflows and outflows is used to differentiate between air that is undisturbed and air that has been modified by the storm. These profiles are used in the photochemical model to examine the aftereffects of convective redistribution in the 24-hour period following the storm. Total tropospheric column O3 production changed little due to convection because so little NO(x) was available in the lower troposphere. However, the integrated O3 production potential in the 5- to 13-km layer changed from net destruction to net production as a result of the convection. The conditions of the August 3, 1985, event may be typical of the early part of the dry season in Amazonia, when only minimal amounts of pollution from biomass burning have been transported into the region.

Methane from the Tropospheric Emission Spectrometer (TES)

NASA Technical Reports Server (NTRS)

Payne, Vivienne; Worden, John; Kulawik, Susan; Frankenberg, Christian; Bowman, Kevin; Wecht, Kevin

2012-01-01

TES V5 CH4 captures latitudinal gradients, regional variability and interannual variation in the free troposphere. V5 joint retrievals offer improved sensitivity to lower troposphere. Time series extends from 2004 to present. V5 reprocessing in progress. Upper tropospheric bias. Mitigated by N2O correction. Appears largely spatially uniform, so can be corrected. How to relate free-tropospheric values to surface emissions.

Upper-Level Waves of Synoptic Scale at Midlatitudes

NASA Astrophysics Data System (ADS)

Rivest, Chantal

1990-01-01

Upper-level waves of synoptic scale are important dynamical entities at midlatitudes. They often induce surface cyclogenesis (cf. Peterssen and Smebye, 1971), and their life duration is typically longer than time scales for disruption by the ambient shear (Sanders, 1988). The objectives of the present thesis are to explain the maintenance and genesis of upper-level synoptic-scale waves in the midlatitude flow. We develop an analytical model of waves on generalized Eady basic states that have uniform tropospheric and stratospheric potential vorticity, but allow for the decay of density with height. The Eady basic state represents the limiting case of infinite stratospheric stability and constant density. We find that the Eady normal mode characteristics hold in the presence of realistic tropopause and stratosphere. In particular, the basic states studied support at the synoptic scale upper-level normal modes. These modes provide simple models for the dynamics of upper-level synoptic-scale waves, as waves supported by the large latitudinal gradients of potential vorticity at the tropopause. In the presence of infinitesimal positive tropospheric gradients of potential vorticity, the upper-level normal mode solutions no longer exist, as was demonstrated in Green (1960). Disappearance of the normal mode solution when a parameter changes slightly represents a dilemma that we seek to understand. We examine what happens to the upper-level normal modes in the presence of tropospheric gradients of potential vorticity in a series of initial -value experiments. Our results show that the normal modes become slowly decaying quasi-modes. Mathematically the quasi-modes consist of a superposition of singular modes sharply peaked in the phase speed domain, and their decay proceeds as the modes interfere with one another. We repeat these experiments in basic states with a smooth tropopause in the presence of tropospheric and stratospheric gradients, and similar results are obtained. Basic states with positive tropospheric and stratospheric gradients of potential vorticity are found to support upper-level synoptic-scale waves for time scales consistent with observations. Following Farrell (1989), we then identify a class of near optimal initial conditions for the excitation of upper-level waves. The initial conditions consist of upper -tropospheric disturbances that lean against the shear. They strongly excite upper-level waves not only in the absence of tropospheric potential vorticity gradients, but also in their presence. This result demonstrates that quasi -modes are as likely to emerge from favorably configured initial conditions as real normal modes, although their excitation is followed by a slow decay. (Copies available exclusively from MIT Libraries, Rm. 14-0551, Cambridge, MA 02139-4307. Ph. 617-253-5668; Fax 617-253-1690.).

Airborne measurements of NO, NO2, and NO(sub y) as related to NASA's TRACE-A field program

NASA Technical Reports Server (NTRS)

Bradshaw, John; Sandholm, Scott

1995-01-01

The Georgia Tech group's effort on NASA's GTE program and TRACE-A field mission primarily involved analysis and interpretation of the measurement data base obtained during the TRACE-A field campaign. These investigations focused on the distribution of ozone and ozone precursors over the south Atlantic and nearby continental regions of Africa and South Africa. The Transport and Atmospheric Chemistry near the Equator-Atlantic (TRACE-A) Mission was designed with the goal of investigating tropospheric trace gas distributions, sources, and photochemical state over the southern Atlantic. Major scientific issues related to N(x)O(y) tropospheric chemistry addressed in this program included: (1) what controls the tropospheric ozone budget over the southern Atlantic? (2) What are the spatial distributions of CO, CO2, NO, NO2, NO(sub y), O3, NMHC, H2O3, etc. over the southern Atlantic? (3) How does long range transport of long-lived NO(y) compounds affect the more reactive NO(x) budget in southern Atlantic troposphere?

Space-Time Variations in Water Vapor as Observed by the UARS Microwave Limb Sounder

NASA Technical Reports Server (NTRS)

Elson, Lee S.; Read, William G.; Waters, Joe W.; Mote, Philip W.; Kinnersley, Jonathan S.; Harwood, Robert S.

1996-01-01

Water vapor in the upper troposphere has a significant impact on the climate system. Difficulties in making accurate global measurements have led to uncertainty in understanding water vapor's coupling to the hydrologic cycle in the lower troposphere and its role in radiative energy balance. The Microwave Limb Sounder (MLS) on the Upper Atmosphere Research Satellite is able to retrieve water vapor concentration in the upper troposphere with good sensitivity and nearly global coverage. An analysis of these preliminary retrievals based on 3 years of observations shows the water vapor distribution to be similar to that measured by other techniques and to model results. The primary MLS water vapor measurements were made in the stratosphere, where this species acts as a conserved tracer under certain conditions. As is the case for the upper troposphere, most of the stratospheric discussion focuses on the time evolution of the zonal mean and zonally varying water vapor. Stratospheric results span a 19-month period and tropospheric results a 36-month period, both beginning in October of 1991. Comparisons with stratospheric model calculations show general agreement, with some differences in the amplitude and phase of long-term variations. At certain times and places, the evolution of water vapor distributions in the lower stratosphere suggests the presence of meridional transport.

Ground-based remote sensing of HDO/H2O ratio profiles: introduction and validation of an innovative retrieval approach

NASA Astrophysics Data System (ADS)

Schneider, M.; Hase, F.; Blumenstock, T.

2006-10-01

We propose an innovative approach for analysing ground-based FTIR spectra which allows us to detect variabilities of lower and middle/upper tropospheric HDO/H2O ratios. We show that the proposed method is superior to common approaches. We estimate that lower tropospheric HDO/H2O ratios can be detected with a noise to signal ratio of 15% and middle/upper tropospheric ratios with a noise to signal ratio of 50%. The method requires the inversion to be performed on a logarithmic scale and to introduce an inter-species constraint. While common methods calculate the isotope ratio posterior to an independent, optimal estimation of the HDO and H2O profile, the proposed approach is an optimal estimator for the ratio itself. We apply the innovative approach to spectra measured continuously during 15 months and present, for the first time, an annual cycle of tropospheric HDO/H2O ratio profiles as detected by ground-based measurements. Outliers in the detected middle/upper tropospheric ratios are interpreted by backward trajectories.

Ground-based remote sensing of HDO/H2O ratio profiles: introduction and validation of an innovative retrieval approach

NASA Astrophysics Data System (ADS)

Schneider, M.; Hase, F.; Blumenstock, T.

2006-06-01

We propose an innovative approach for analysing ground-based FTIR spectra which allows us to detect variabilities of lower and middle/upper tropospheric HDO/H2O ratios. We show that the proposed method is superior to common approaches. We estimate that lower tropospheric HDO/H2O ratios can be detected with a noise to signal ratio of 15% and middle/upper tropospheric ratios with a noise to signal ratio of 50%. The method requires the inversion to be performed on a logarithmic scale and to introduce an inter-species constraint. While common methods calculate the isotope ratio posterior to an independent, optimal estimation of the HDO and H2O profile, the proposed approach is an optimal estimator for the ratio itself. We apply the innovative approach to spectra measured continuously during 15 months and present, for the first time, an annual cycle of tropospheric HDO/H2O ratio profiles as detected by ground-based measurements. Outliers in the detected middle/upper tropospheric ratios are interpreted by backward trajectories.

HALOE Algorithm Improvements for Upper Tropospheric Sounding

NASA Technical Reports Server (NTRS)

McHugh, Martin J.; Gordley, Larry L.; Russell, James M., III; Hervig, Mark E.

1999-01-01

This report details the ongoing efforts by GATS, Inc., in conjunction with Hampton University and University of Wyoming, in NASA's Mission to Planet Earth UARS Science Investigator Program entitled "HALOE Algorithm Improvements for Upper Tropospheric Soundings." The goal of this effort is to develop and implement major inversion and processing improvements that will extend HALOE measurements further into the troposphere. In particular, O3, H2O, and CH4 retrievals may be extended into the middle troposphere, and NO, HCl and possibly HF into the upper troposphere. Key areas of research being carried out to accomplish this include: pointing/tracking analysis; cloud identification and modeling; simultaneous multichannel retrieval capability; forward model improvements; high vertical-resolution gas filter channel retrievals; a refined temperature retrieval; robust error analyses; long-term trend reliability studies; and data validation. The current (first-year) effort concentrates on the pointer/tracker correction algorithms, cloud filtering and validation, and multi-channel retrieval development. However, these areas are all highly coupled, so progress in one area benefits from and sometimes depends on work in others.

Sensitivities of NOx transformation and the effects on surface ozone and nitrate

NASA Astrophysics Data System (ADS)

Lei, H.; Wang, J. X. L.

2013-08-01

As precursors for tropospheric ozone and nitrate aerosols, Nitrogen oxides (NOx) in present atmosphere and its transformation in responding to emission and climate perturbations are studied by CAM-Chem model and air quality measurements including National Emission Inventory (NEI), Clean Air Status and Trends Network (CASTNET) and Environmental Protection Agency Air Quality System (EPA AQS). It is found that not only the surface ozone formation but also the nitrate formation is associated with the relative emissions of NOx and volatile organic compounds (VOC). Due to the availability of VOC and associated NOx titration, ozone productions in industrial regions increase in warmer conditions and slightly decrease against NOx emission increase, which is converse to the response in farming region. The decrease or small increase in ozone concentrations over industrial regions result in the responded nitrate increasing rate staying above the increasing rate of NOx emissions. It is indicated that ozone concentration change is more directly affected by changes in climate and precursor emissions, while nitrate concentration change is also affected by local ozone production types and their seasonal transfer. The sensitivity to temperature perturbations shows that warmer climate accelerates the decomposition of odd nitrogen (NOy) during the night. As a result, the transformation rate of NOx to nitrate decreases. Examinations on the historical emission and air quality records on typical pollution areas further confirm the conclusion drawn from modeling experiments.

Satellite-based emission constraint for nitrogen oxides: Capability and uncertainty

NASA Astrophysics Data System (ADS)

Lin, J.; McElroy, M. B.; Boersma, F.; Nielsen, C.; Zhao, Y.; Lei, Y.; Liu, Y.; Zhang, Q.; Liu, Z.; Liu, H.; Mao, J.; Zhuang, G.; Roozendael, M.; Martin, R.; Wang, P.; Spurr, R. J.; Sneep, M.; Stammes, P.; Clemer, K.; Irie, H.

2013-12-01

Vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) retrieved from satellite remote sensing have been employed widely to constrain emissions of nitrogen oxides (NOx). A major strength of satellite-based emission constraint is analysis of emission trends and variability, while a crucial limitation is errors both in satellite NO2 data and in model simulations relating NOx emissions to NO2 columns. Through a series of studies, we have explored these aspects over China. We separate anthropogenic from natural sources of NOx by exploiting their different seasonality. We infer trends of NOx emissions in recent years and effects of a variety of socioeconomic events at different spatiotemporal scales including the general economic growth, global financial crisis, Chinese New Year, and Beijing Olympics. We further investigate the impact of growing NOx emissions on particulate matter (PM) pollution in China. As part of recent developments, we identify and correct errors in both satellite NO2 retrieval and model simulation that ultimately affect NOx emission constraint. We improve the treatments of aerosol optical effects, clouds and surface reflectance in the NO2 retrieval process, using as reference ground-based MAX-DOAS measurements to evaluate the improved retrieval results. We analyze the sensitivity of simulated NO2 to errors in the model representation of major meteorological and chemical processes with a subsequent correction of model bias. Future studies will implement these improvements to re-constrain NOx emissions.

Evidence of Convective Redistribution of Carbon Monoxide in Aura Tropospheric Emission Sounder (TES) and Microwave Limb Sounder (MLS) Observations

NASA Technical Reports Server (NTRS)

Manyin, Michael; Douglass, Anne; Schoeberl, Mark

2010-01-01

Vertical convective transport is a key element of the tropospheric circulation. Convection lofts air from the boundary layer into the free troposphere, allowing surface emissions to travel much further, and altering the rate of chemical processes such as ozone production. This study uses satellite observations to focus on the convective transport of CO from the boundary layer to the mid and upper troposphere. Our hypothesis is that strong convection associated with high rain rate regions leads to a correlation between mid level and upper level CO amounts. We first test this hypothesis using the Global Modeling Initiative (GMI) chemistry and transport model. We find the correlation is robust and increases as the precipitation rate (the strength of convection) increases. We next examine three years of CO profiles from the Tropospheric Emission Sounder (TES) and Microwave Limb Sounder (MLS) instruments aboard EOS Aura. Rain rates are taken from the Tropical Rainfall Measuring Mission (TRMM) 3B-42 multi-satellite product. Again we find a correlation between mid-level and upper tropospheric CO, which increases with rain rate. Our result shows the critical importance of tropical convection in coupling vertical levels of the troposphere in the transport of trace gases. The effect is seen most clearly in strong convective regions such as the Inter-tropical Convergence Zone.

Climatology of water vapor in the upper troposphere and lower stratosphere determined from Sage 2 observations

NASA Technical Reports Server (NTRS)

Chiou, Er-Woon; McCormick, M. P.

1994-01-01

The purpose of this paper is to present a vertically-resolved global climatology of water vapor in the upper troposphere and lower stratosphere based on multi-year SAGE 2 observations. Seasonally averaged zonal mean profiles are illustrated in terms of both mixing ration and relative humidity.

Evaluation of Simulated Photochemical Partitioning of Oxidized Nitrogen in the Upper Troposphere

EPA Science Inventory

Regional and global chemical transport models underpredict NO_x (NO +NO₂) in the upper troposphere where it is a precursor to the greenhouse gas ozone. The NO_x bias has been shown in model evaluations using aircraft data (Singh et al., 2007) and to...

The China Clipper - Fast advective transport of radon-rich air from the Asian boundary layer to the upper troposphere near California

NASA Technical Reports Server (NTRS)

Kritz, Mark A.; Le Roulley, Jean-Claude; Danielsen, Edwin F.

1990-01-01

A series of upper tropospheric radon concentration measurements made over the eastern Pacific and west coast of the U.S. during the summers of 1983 and 1984 has revealed the occurrence of unexpectedly high radon concentrations for 9 of the 61 measurements. A frequency distribution plot of the set of 61 observations shows a distinct bimodal distribution, with approximately 2/5 of the observations falling close to 1 pCi/SCM, and 3/5 falling in a high concentration mode centered at about 11 pCi/SCM. Trajectory and synoptic analyses for two of the flights on which such high radon concentrations were observed indicate that this radon-rich air originated in the Asian boundary layer, ascended in cumulus updrafts, and was carried eastward in the fast moving air on the anticyclonic side of the upper tropospheric jet. The results suggest that the combination of rapid vertical transport from the surface boundary layer to the upper troposphere, followed by rapid horizontal transport eastward represents an efficient mode of long-transport for other, chemically reactive atmospheric trace constituents.

The China Clipper - Fast advective transport of radon-rich air from the Asian boundary layer to the upper troposphere near California

NASA Astrophysics Data System (ADS)

Kritz, Mark A.; Le Roulley, Jean-Claude; Danielsen, Edwin F.

1990-02-01

A series of upper tropospheric radon concentration measurements made over the eastern Pacific and west coast of the U.S. during the summers of 1983 and 1984 has revealed the occurrence of unexpectedly high radon concentrations for 9 of the 61 measurements. A frequency distribution plot of the set of 61 observations shows a distinct bimodal distribution, with approximately 2/5 of the observations falling close to 1 pCi/SCM, and 3/5 falling in a high concentration mode centered at about 11 pCi/SCM. Trajectory and synoptic analyses for two of the flights on which such high radon concentrations were observed indicate that this radon-rich air originated in the Asian boundary layer, ascended in cumulus updrafts, and was carried eastward in the fast moving air on the anticyclonic side of the upper tropospheric jet. The results suggest that the combination of rapid vertical transport from the surface boundary layer to the upper troposphere, followed by rapid horizontal transport eastward represents an efficient mode of long-transport for other, chemically reactive atmospheric trace constituents.

Trace gas transport out of the Indian Summer Monsoon

NASA Astrophysics Data System (ADS)

Tomsche, Laura; Pozzer, Andrea; Zimmermann, Peter; Parchatka, Uwe; Fischer, Horst

2016-04-01

The trace gas transport out of the Indian summer monsoon was investigated during the aircraft campaign OMO (Oxidation Mechanism Observations) with the German research aircraft HALO (High Altitude and Long Range Research Aircraft) in July/August 2015. HALO was based at Paphos/Cyprus and also on Gan/Maledives. Flights took place over the Mediterranean Sea, the Arabian Peninsula and the Arabian Sea. In this work the focus is on the distribution of carbon monoxide (CO) and methane (CH4) in the upper troposphere. They were measured with the laser absorption spectrometer TRISTAR on board of HALO. During the Indian summer monsoon strong convection takes place over India and the Bay of Bengal. In this area the population is high accompanied by many emission sources e.g. wetlands and cultivation of rice. Consequently the boundary layer is polluted containing high concentrations of trace gases like methane and carbon monoxide. Due to vertical transport these polluted air masses are lifted to the upper troposphere. Here they circulate with the so called Asian monsoon anticyclone. In the upper troposphere polluted air masses lead to a change in the chemical composition thus influence the chemical processes. Furthermore the anticyclone spreads the polluted air masses over a larger area. Thus the outflow of the anticyclone in the upper troposphere leads to higher concentrations of trace gases over the Arabian Sea, the Arabian Peninsula and also over the eastern part of North Africa and the eastern part of the Mediterranean Sea. During OMO higher concentrations of methane and carbon monoxide were detected at altitudes between 11km and 15km. The highest measured concentrations of carbon monoxide and methane were observed over Oman. The CO concentration in the outflow of the monsoon exceeds background levels by 10-15ppb. However the enhancement in the concentration is not obviously connected to the monsoon due to the natural variability in the troposphere. The enhancement in the methane concentration (30-40ppb) is more obviously connected to the monsoon because it is much higher than the natural variability. Consequently methane is a very good tracer for the monsoon influenced air masses. Beside flights into the outflow of the Indian summer monsoon, there were also measurements of background concentrations in the upper troposphere in air not influenced by the monsoon. Profiles have shown that the high concentrations of trace gases are only observed in the upper troposphere. The high concentrations in the upper troposphere cannot be explained by vertical transport form local ground sources.

Three-dimensional circulation structures leading to heavy summer rainfall over central North China

NASA Astrophysics Data System (ADS)

Sun, Wei; Yu, Rucong; Li, Jian; Yuan, Weihua

2016-04-01

Using daily and hourly rain gauge records and Japanese 25 year reanalysis data over 30 years, this work reveals two major circulation structures leading to heavy summer rainfall events in central North China (CNC), and further analyzes the effects of the circulations on these rainfall events. One circulation structure has an extensive upper tropospheric warm anomaly (UTWA) covering North China (NC). By strengthening the upper anticyclonic anomaly and lower southerly flows around NC, the UTWA plays a positive role in forming upper level divergence and lower level moisture convergence. As a result, the warm anomalous circulation has a solid relationship with large-scale, long-duration rainfall events with a diurnal peak around midnight to early morning. The other circulation structure has an upper tropospheric cold anomaly (UTCA) located in the upper stream of NC. Contributed to by the UTCA, a cold trough appears in the upper stream of NC and an unstable configuration with upper (lower) cold (warm) anomalies forms around CNC. Consequently, CNC is covered by strong instability and high convective energy, and the cold anomalous circulation is closely connected with local, short-duration rainfall events concentrated from late afternoon to early nighttime. The close connections between circulation structures and typical rainfall events are confirmed by two independent converse analysis processes: from circulations to rainfall characteristics, and from typical rainfall events to circulations. The results presented in this work indicate that the upper tropospheric temperature has significant influences on heavy rainfall, and thus more attention should be paid to the upper tropospheric temperature in future analyses.

Atmospheric chemistry and transport modeling in the outer solar system

NASA Astrophysics Data System (ADS)

Lee, Yuan-Tai (Anthony)

2001-11-01

This thesis consists of 1-D and 2-D photochemical- dynamical modeling in the upper atmospheres of outer planets. For 1-D modeling, a unified hydrocarbon photochemical model has been studied in Jupiter, Saturn, Uranus, Neptune, and Titan, by comparing with the Voyager observations, and the recent measurements of methyl radicals by ISO in Saturn and Neptune. The CH3 observation implies a kinetically sensitive test to the measured and estimated hydrocarbon rate constants at low temperatures. We identify the key reactions that control the concentrations of CH3 in the model, such as the three-body recombination reaction, CH3 + CH3 + M --> C 2H6 + M, and the recycling reaction H + CH3 + M --> CH4 + M. The results show reasonable agreement with ISO values. In Chapter 4, the detection of PH3 in the lower stratosphere and upper troposphere of Jupiter has provided a photochemical- dynamical coupling model to derive the eddy diffusion coefficient in the upper troposphere of Jupiter. Using a two-layers photochemical model with updated photodissociation cross-sections and chemical rate constants for NH3 and PH 3, we find that the upper tropospheric eddy diffusion coefficient <10 5 cm2 sec-1, and the deeper tropospheric value >106 cm2 sec-1, are required to match the derived PH3 vertical profile by the observation. The best-fit functional form derivation of eddy diffusion coefficient in the upper troposphere of Jupiter above 400 mbar is K = 2.0 × 104 (n/2.2 × 1019)-0.5 cm 2 sec-1. On the other hand, Chapter 5 demonstrates a dynamical-only 2-D model of C2H6 providing a complete test for the current 2-D transport models in Jovian lower stratosphere and upper troposphere (270 to 0.1 mbar pressure levels). Different combinations of residual advection, horizontal eddy dispersion, and vertical eddy mixing are examined at different latitudes.

Physical Mechanisms for the Maintenance of GCM-Simulated Madden-Julian Oscillation over the Indian Ocean and Pacific

DOE Office of Scientific and Technical Information (OSTI.GOV)

Deng, Liping; Wu, Xiaoqing

2011-05-05

The kinetic energy budget is conducted to analyze the physical processes responsible for the improved Madden-Julian Oscillation (MJO) simulated by the Iowa State University general circulation models (ISUGCM). The modified deep convection scheme that includes the revised convection closure, convection trigger condition and convective momentum transport (CMT) enhances the equatorial (10oS-10oN) MJO-related perturbation kinetic energy (PKE) in the upper troposphere and leads to more robust and coherent eastward propagating MJO signal. In the MJO source region-the Indian Ocean (45oE-120oE), the upper-tropospheric MJO PKE is maintained by the vertical convergence of wave energy flux and the barotropic conversion through the horizontalmore » shear of mean flow. In the convectively active region-the western Pacific (120oE-180o), the upper-tropospheric MJO PKE is supported by the convergence of horizontal and vertical wave energy fluxes. Over the central-eastern Pacific (180o-120oW), where convection is suppressed, the upper-tropospheric MJO PKE is mainly due to the horizontal convergence of wave energy flux. The deep convection trigger condition produces stronger convective heating which enhances the perturbation available potential energy (PAPE) production and the upward wave energy fluxes, and leads to the increased MJO PKE over the Indian Ocean and western Pacific. The trigger condition also enhances the MJO PKE over the central-eastern Pacific through the increased convergence of meridional wave energy flux from the subtropical latitudes of both hemispheres. The revised convection closure affects the response of mean zonal wind shear to the convective heating over the Indian Ocean and leads to the enhanced upper-tropospheric MJO PKE through the barotropic conversion. The stronger eastward wave energy flux due to the increase of convective heating over the Indian Ocean and western Pacific by the revised closure is favorable to the eastward propagation of MJO and the convergence of horizontal wave energy flux over the central-eastern Pacific. The convection-induced momentum tendency tends to decelerate the upper-tropospheric wind which results in a negative work to the PKE budget in the upper troposphere. However, the convection momentum tendency accelerates the westerly wind below 800 hPa over the western Pacific, which is partially responsible for the improved MJO simulation.« less

Aerosols increase upper tropospheric humidity over the North Western Pacific

NASA Astrophysics Data System (ADS)

Riuttanen, Laura; Bister, Marja; John, Viju; Sundström, Anu-Maija; Dal Maso, Miikka; Räisänen, Jouni; de Leeuw, Gerrit; Kulmala, Markku

2014-05-01

Water vapour in the upper troposphere is highly important for the global radiative transfer. The source of upper tropospheric humidity is deep convection, and aerosol effects on them have got attention only recently. E.g., aerosol effects on deep convective clouds have been missing in general circulation models (Quaas et al., 2009). In deep convection, aerosol effect on cloud microphysics may lead to more ice precipitation and less warm rain (Khain et al., 2005), and thus more water vapour in upper troposphere (Bister & Kulmala, 2011). China outflow region over the Pacific Ocean was chosen as a region for a more detailed study, with latitudes 25-45 N and three longitude slots: 120-149 E, 150-179 E and 150-179 W. In this study, we used satellite measurements of aerosol optical depth (AOD) and upper tropospheric humidity (UTH). AOD was obtained from the MODIS instrument onboard Terra satellite, that crosses the equator southward at 10:30 AM local solar time (Remer et al., 2005). UTH was obtained from a microwave humidity sounder (MHS) onboard MetOp-A satellite, with passing time at 9:30 PM local solar time. It measures relative humidity of a layer extending approximately from 500 to 200 hPa. We binned the AOD and UTH data according to daily rainfall product 3B42 from Tropical Rainfall Measuring Mission (TRMM) satellite. Binning the data according to the amount of precipitation gives us a new way to account for the possible aerosol invigoration effect on convection and to alleviate the contamination and causality problems in aerosol indirect effect studies. In this study, we show for the first time, based on satellite data, that there is a connection between upper tropospheric humidity and aerosols. Anthropogenic aerosols from China increase upper tropospheric humidity, which causes a significant positive local radiative forcing in libRadtran radiative transfer model (Mayer & Kylling, 2005). References: Bister, M. & Kulmala, M. (2011). Atmos. Chem. Phys., 11, 4577-4586. Khain, A., Rosenfeld, D. & Pokrovsky, A. (2005). Q. J. R. Meteorol. Soc., 131, 2639-2663. Mayer, B. & Kylling, A. (2005). Atmos. Chem. Phys., 5, 1855-1877. Remer, L. A. et al. (2005). J. Atmos. Sci., 62, 947-973. Quaas, J. et al. (2009). Atmos. Chem. Phys., 9, 8697-8717.

On the Tropospheric Measurements of Ozone by the Stratospheric Aerosol and Gas Experiment II (SAGE II, version 6.1) in the Tropics

NASA Technical Reports Server (NTRS)

Kar, J.; Trepte, C. R.; Thomason, L. W.; Zawodny, J. M.; Cunnold, D. M.; Wang, H. J.

2002-01-01

Tropospheric measurements of ozone from SAGE II (version 6.1) in the tropics have been analyzed using 12 years of data (1985-1990, 1994-1999). The seasonally averaged vertical profiles of the ozone mixing ratio in the upper troposphere have been presented for the first time from satellite measurements. These profiles show qualitative similarities with corresponding seasonal mean ozonesonde profiles at northern and southern tropical stations and are about 40-50% less than the sonde values. Despite this systematic offset, the measurements appear to be consistent with a zonal wave one pattern in the upper tropospheric column ozone and with the recently predicted summertime ozone enhancement over the Middle East. These results thus affirm the usefulness of the occultation method in studying tropospheric ozone.

Subtropical subsidence and surface deposition of oxidized mercury produced in the free troposphere

NASA Astrophysics Data System (ADS)

Shah, Viral; Jaeglé, Lyatt

2017-07-01

Oxidized mercury (Hg(II)) is chemically produced in the atmosphere by oxidation of elemental mercury and is directly emitted by anthropogenic activities. We use the GEOS-Chem global chemical transport model with gaseous oxidation driven by Br atoms to quantify how surface deposition of Hg(II) is influenced by Hg(II) production at different atmospheric heights. We tag Hg(II) chemically produced in the lower (surface-750 hPa), middle (750-400 hPa), and upper troposphere (400 hPa-tropopause), in the stratosphere, as well as directly emitted Hg(II). We evaluate our 2-year simulation (2013-2014) against observations of Hg(II) wet deposition as well as surface and free-tropospheric observations of Hg(II), finding reasonable agreement. We find that Hg(II) produced in the upper and middle troposphere constitutes 91 % of the tropospheric mass of Hg(II) and 91 % of the annual Hg(II) wet deposition flux. This large global influence from the upper and middle troposphere is the result of strong chemical production coupled with a long lifetime of Hg(II) in these regions. Annually, 77-84 % of surface-level Hg(II) over the western US, South America, South Africa, and Australia is produced in the upper and middle troposphere, whereas 26-66 % of surface Hg(II) over the eastern US, Europe, and East Asia, and South Asia is directly emitted. The influence of directly emitted Hg(II) near emission sources is likely higher but cannot be quantified by our coarse-resolution global model (2° latitude × 2.5° longitude). Over the oceans, 72 % of surface Hg(II) is produced in the lower troposphere because of higher Br concentrations in the marine boundary layer. The global contribution of the upper and middle troposphere to the Hg(II) dry deposition flux is 52 %. It is lower compared to the contribution to wet deposition because dry deposition of Hg(II) produced aloft requires its entrainment into the boundary layer, while rain can scavenge Hg(II) from higher altitudes more readily. We find that 55 % of the spatial variation of Hg wet deposition flux observed at the Mercury Deposition Network sites is explained by the combined variation of precipitation and Hg(II) produced in the upper and middle troposphere. Our simulation points to a large role of the dry subtropical subsidence regions. Hg(II) present in these regions accounts for 74 % of Hg(II) at 500 hPa over the continental US and more than 60 % of the surface Hg(II) over high-altitude areas of the western US. Globally, it accounts for 78 % of the tropospheric Hg(II) mass and 61 % of the total Hg(II) deposition. During the Nitrogen, Oxidants, Mercury, and Aerosol Distributions, Sources, and Sinks (NOMADSS) aircraft campaign, the contribution of Hg(II) from the dry subtropical regions was found to be 75 % when measured Hg(II) exceeded 250 pg m-3. Hg(II) produced in the upper and middle troposphere subsides in the anticyclones, where the dry conditions inhibit the loss of Hg(II). Our results highlight the importance the subtropical anticyclones as the primary conduits for the production and export of Hg(II) to the global atmosphere.

Spatial and Temporal Variability of Surface Energy Fluxes During Autumn Ice Advance: Observations and Model Validation

NASA Astrophysics Data System (ADS)

Persson, O. P. G.; Blomquist, B.; Grachev, A. A.; Guest, P. S.; Stammerjohn, S. E.; Solomon, A.; Cox, C. J.; Capotondi, A.; Fairall, C. W.; Intrieri, J. M.

2016-12-01

From Oct 4 to Nov 5, 2015, the Office of Naval Research - sponsored Sea State cruise in the Beaufort Sea with the new National Science Foundation R/V Sikuliaq obtained extensive in-situ and remote sensing observations of the lower troposphere, the advancing sea ice, wave state, and upper ocean conditions. In addition, a coupled atmosphere, sea ice, upper-ocean model, based on the RASM model, was run at NOAA/PSD in a hindcast mode for this same time period, providing a 10-day simulation of the atmosphere/ice/ocean evolution. Surface energy fluxes quantitatively represent the air-ice, air-ocean, and ice-ocean interaction processes, determining the cooling (warming) rate of the upper ocean and the growth (melting) rate of sea ice. These fluxes also impact the stratification of the lower troposphere and the upper ocean. In this presentation, both direct and indirect measurements of the energy fluxes during Sea State will be used to explore the spatial and temporal variability of these fluxes and the impacts of this variability on the upper ocean, ice, and lower atmosphere during the autumn ice advance. Analyses have suggested that these fluxes are impacted by atmospheric synoptic evolution, proximity to existing ice, ice-relative wind direction, ice thickness and snow depth. In turn, these fluxes impact upper-ocean heat loss and timing of ice formation, as well as stability in the lower troposphere and upper ocean, and hence heat transport to the free troposphere and ocean mixed-layer. Therefore, the atmospheric structure over the advancing first-year ice differs from that over the nearby open water. Finally, these observational analyses will be used to provide a preliminary validation of the spatial and temporal variability of the surface energy fluxes and the associated lower-tropospheric and upper-ocean structures in the simulations.

The chemistry-climate model ECHAM6.3-HAM2.3-MOZ1.0

NASA Astrophysics Data System (ADS)

Schultz, Martin G.; Stadtler, Scarlet; Schröder, Sabine; Taraborrelli, Domenico; Franco, Bruno; Krefting, Jonathan; Henrot, Alexandra; Ferrachat, Sylvaine; Lohmann, Ulrike; Neubauer, David; Siegenthaler-Le Drian, Colombe; Wahl, Sebastian; Kokkola, Harri; Kühn, Thomas; Rast, Sebastian; Schmidt, Hauke; Stier, Philip; Kinnison, Doug; Tyndall, Geoffrey S.; Orlando, John J.; Wespes, Catherine

2018-05-01

The chemistry-climate model ECHAM-HAMMOZ contains a detailed representation of tropospheric and stratospheric reactive chemistry and state-of-the-art parameterizations of aerosols using either a modal scheme (M7) or a bin scheme (SALSA). This article describes and evaluates the model version ECHAM6.3-HAM2.3-MOZ1.0 with a focus on the tropospheric gas-phase chemistry. A 10-year model simulation was performed to test the stability of the model and provide data for its evaluation. The comparison to observations concentrates on the year 2008 and includes total column observations of ozone and CO from IASI and OMI, Aura MLS observations of temperature, HNO3, ClO, and O3 for the evaluation of polar stratospheric processes, an ozonesonde climatology, surface ozone observations from the TOAR database, and surface CO data from the Global Atmosphere Watch network. Global budgets of ozone, OH, NOx, aerosols, clouds, and radiation are analyzed and compared to the literature. ECHAM-HAMMOZ performs well in many aspects. However, in the base simulation, lightning NOx emissions are very low, and the impact of the heterogeneous reaction of HNO3 on dust and sea salt aerosol is too strong. Sensitivity simulations with increased lightning NOx or modified heterogeneous chemistry deteriorate the comparison with observations and yield excessively large ozone budget terms and too much OH. We hypothesize that this is an impact of potential issues with tropical convection in the ECHAM model.

Long-range transport of Asian pollution to the northeast Pacific: Seasonal variations and transport pathways of carbon monoxide

NASA Astrophysics Data System (ADS)

Liang, Qing; Jaeglé, Lyatt; Jaffe, Daniel A.; Weiss-Penzias, Peter; Heckman, Anna; Snow, Julie A.

2004-12-01

Continuous CO measurements were obtained at Cheeka Peak Observatory (CPO, 48.3°N, 124.6°W, 480 m), a coastal site in Washington state, between 9 March 2001 and 31 May 2002. We analyze these observations as well as CO observations at ground sites throughout the North Pacific using the GEOS-CHEM global tropospheric chemistry model to examine the seasonal variations of Asian long-range transport. The model reproduces the observed CO levels, their seasonal cycle and day-to-day variability, with a 5-20 ppbv negative bias in winter/spring and 5-10 ppbv positive bias during summer. Asian influence on CO levels in the North Pacific troposphere maximizes during spring and minimizes during summer, ranging from 91 ppbv (44% of total CO) to 52 ppbv (39%) along the Asian Pacific Rim and from 44 ppbv (30%) to 24 ppbv (23%) at CPO. Maximum export of Asian pollution to the western Pacific occurs at 20°-50°N during spring throughout the tropospheric column, shifting to 30°-60°N during summer, mostly in the upper troposphere. The model captures five particularly strong transpacific transport events reaching CPO (four in spring, one in winter) resulting in 20-40 ppbv increases in observed CO levels. Episodic long-range transport of pollutants from Asia to the NE Pacific occurs throughout the year every 10, 15, and 30 days in the upper, middle, and lower troposphere, respectively. Lifting ahead of cold fronts followed by transport in midlatitude westerlies accounts for 78% of long-range transport events reaching the NE Pacific middle and upper troposphere. During summer, convective injection into the upper troposphere competes with frontal mechanisms in this export. Most events reaching the NE Pacific lower troposphere below 2 km altitude result from boundary layer outflow behind cold fronts (for spring) or ahead of cold fronts (for other seasons) followed by low-level transpacific transport.

Harold S. Johnston (1920-2012)

NASA Astrophysics Data System (ADS)

Wuebbles, Donald

2013-02-01

One of the most exceptional atmospheric chemists of the twentieth century, Harold "Hal" S. Johnston died on 20 October 2012 at the age of 92. Hal's pioneering work on atmospheric kinetics, both in laboratory and theoretical studies, greatly advanced understanding of the processes affecting ozone in the troposphere and stratosphere, especially related to the chemistry and impacts resulting from nitrogen oxides (NOx ).

Sensitivities of NOx transformation and the effects on surface ozone and nitrate

NASA Astrophysics Data System (ADS)

Lei, H.; Wang, J. X. L.

2014-02-01

As precursors to tropospheric ozone and nitrate, nitrogen oxide (NOx) in the present atmosphere and its transformation in response to emission and climate perturbations are studied by using the CAM-Chem model and air quality measurements from the National Emissions Inventory (NEI), Clean Air Status and Trends Network (CASTNET), and Environmental Protection Agency Air Quality System (EPA AQS). It is found that NOx transformations in present atmospheric conditions show different sensitivities over industrial and non-industrial regions. As a result, the surface ozone and nitrate formations can be divided into several regimes associated with the dominant emission types and relative levels of NOx and volatile organic compounds (VOC). Ozone production in industrial regions (the main NOx emission source areas) increases in warmer conditions and slightly decreases following an increase in NOx emissions due to NOx titration, which is opposite to the response in non-industrial regions. The ozone decrease following a temperature increase in non-industrial regions indicates that ozone production in regions that lack NOx emission sources may be sensitive to NOx transformation in remote source regions. The increase in NO2 from NOx titration over industrial regions results in an increase rate of total nitrate that remains higher than the increase rate of NOx emissions. The presented findings indicate that a change in the ozone concentration is more directly affected by changes in climate and precursor emissions, while a change in the nitrate concentration is affected by local ozone production types and their seasonal transfer. The sensitivity to temperature perturbations shows that a warmer climate accelerates the decomposition of odd nitrogen (NOy) during the night. As a result, the transformation rate of NOx to nitrate decreases. Examinations of the historical emissions and air quality records of a typical NOx-limited area, such as Atlanta and a VOC-limited area, such as Los Angeles further confirm the conclusions drawn from the modeling experiments.

A molecular perspective for global modeling of upper atmospheric NH3 from freezing clouds.

PubMed

Ge, Cui; Zhu, Chongqin; Francisco, Joseph S; Zeng, Xiao Cheng; Wang, Jun

2018-05-30

Ammonia plays a key role in the neutralization of atmospheric acids such as sulfate and nitrates. A few in situ observations have supported the theory that gas-phase NH 3 concentrations should decrease sharply with altitude and be extremely low in the upper troposphere and lower stratosphere (UTLS). This theory, however, seems inconsistent with recent satellite measurements and is also not supported by the aircraft data showing highly or fully neutralized sulfate aerosol particles by ammonium in the UTLS in many parts of the world. Here we reveal the contributions of deep convective clouds to NH 3 in the UTLS by using integrated cross-scale modeling, which includes molecular dynamic simulations, a global chemistry transport model, and satellite and aircraft measurements. We show that the NH 3 dissolved in liquid cloud droplets is prone to being released into the UTLS upon freezing during deep convection. Because NH 3 emission is not regulated in most countries and its future increase is likely persistent from agricultural growth and the warmer climate, the effect of NH 3 on composition and phase of aerosol particles in the UTLS can be significant, which in turn can affect cirrus cloud formation, radiation, and the budgets of NOx and O 3 .

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

NASA Technical Reports Server (NTRS)

Duncan, Bryan N.; Yoshida, Yasuko; deFoy, Benjamin; Lamsal, Lok N.; Streets, David G.; Lu, Zifeng; Pickering, Kenneth E.; Krotkov, Nickolay A.

2013-01-01

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.

Comparison of Weekly Cycle of NO2 Satellite Retrievals and NO(x) Emission Inventories for the Continental United States

NASA Technical Reports Server (NTRS)

Kaynak, B.; Hu, Y.; Martin, R. V.; Sioris, C. E.; Russell, A. G.

2009-01-01

Spatially resolved weekly NO2 variations are obtained from 2003 to 2005 Scanning Imaging Absorption Spectrometer for Atmospheric Cartography (SCIAMACHY) tropospheric NO2 columns for three different types of regions: urban, rural, and rural-point (rural with significant electricity generation unit (EGU) emissions). Regions are compared for magnitudes and weekly profiles. Rural regions do not show any weekly pattern, whereas urban areas show a distinct decrease on the weekends. Rural regions with EGUs show a slight decrease on Sundays. When compared with estimated mobile and stationary nitrogen oxides (NO(x)) emissions from the year 2004 for seven cities, the satellite data have greater variation during weekdays (Monday-Friday). Overall comparisons show that SCIAMACHY derived NO2 correlate well with estimated NO(x) emissions for urban and rural but less for rural-point regions.

On the existence of tropical anvil clouds

NASA Astrophysics Data System (ADS)

Seeley, J.; Jeevanjee, N.; Langhans, W.; Romps, D.

2017-12-01

In the deep tropics, extensive anvil clouds produce a peak in cloud cover below the tropopause. The dominant paradigm for cloud cover attributes this anvil peak to a layer of enhanced mass convergence in the clear-sky upper-troposphere, which is presumed to force frequent detrainment of convective anvils. However, cloud cover also depends on the lifetime of cloudy air after it detrains, which raises the possibility that anvil clouds may be the signature of slow cloud decay rather than enhanced detrainment. Here we measure the cloud decay timescale in cloud-resolving simulations, and find that cloudy updrafts that detrain in the upper troposphere take much longer to dissipate than their shallower counterparts. We show that cloud lifetimes are long in the upper troposphere because the saturation specific humidity becomes orders of magnitude smaller than the typical condensed water loading of cloudy updrafts. This causes evaporative cloud decay to act extremely slowly, thereby prolonging cloud lifetimes in the upper troposphere. As a consequence, extensive anvil clouds still occur in a convecting atmosphere that is forced to have no preferential clear-sky convergence layer. On the other hand, when cloud lifetimes are fixed at a characteristic lower-tropospheric value, extensive anvil clouds do not form. Our results support a revised understanding of tropical anvil clouds, which attributes their existence to the microphysics of slow cloud decay rather than a peak in clear-sky convergence.

The Tropical Upper Troposphere and Lower Stratosphere in the GEOS-2 GCM

NASA Technical Reports Server (NTRS)

Pawson, S.; Takacs, L.; Molod, A.; Nebuda, S.; Chen, M.; Rood, R.; Read, W. L.; Fiorino, M.

1999-01-01

The structure of the tropical upper troposphere and lower stratosphere in the GEOS-2 General Circulation Model (GCM) is discussed. The emphasis of this study is on the reality of monthly-mean temperature and water vapor distributions in the model, compared to reasonable observational estimates. It is shown that although the zonal-mean temperature is in good agreement with observations, the GCM supports an excessive zonal asymmetry near the tropopause compared to the ECMWF Reanalyses. In reality there is a QBO-related variability in the zonally averaged lower stratospheric temperature which is not captured by the model. The observed upper tropospheric temperature and humidity fields show variations related to those in the sea surface temperature, which are not incorporated in the GCM; nevertheless, there is some interannual variability in the GCM, indicating a component arising from internal processes. The model is too moist in the middle troposphere (500 hPa) but too dry in the upper troposphere, suggesting that there is too little vertical transport or too much drying in the GCM. Transport into the stratosphere shows a pronounced annual cycle, with drier air entering the tropical stratosphere when the tropopause is coldest in northern winter; while the alternating dry and moist air masses can be traced ascending through the tropical lower stratosphere, the progression of the anomalies is too rapid.

A WRF-Chem Analysis of Flash Rates, Lightning-NOx Production and Subsequent Trace Gas Chemistry of the 29-30 May 2012 Convective Event in Oklahoma During DC3

NASA Technical Reports Server (NTRS)

Cummings, Kristin A.; Pickering, Kenneth; Barth, Mary; Weinheimer, A.; Bela, M.; Li, Y; Allen, D.; Bruning, E.; MacGorman, D.; Rutledge, S.;

Oxidation of mercury by bromine in the subtropical Pacific free troposphere

NASA Astrophysics Data System (ADS)

Gratz, L. E.; Ambrose, J. L.; Jaffe, D. A.; Shah, V.; Jaeglé, L.; Stutz, J.; Festa, J.; Spolaor, M.; Tsai, C.; Selin, N. E.; Song, S.; Zhou, X.; Weinheimer, A. J.; Knapp, D. J.; Montzka, D. D.; Flocke, F. M.; Campos, T. L.; Apel, E.; Hornbrook, R.; Blake, N. J.; Hall, S.; Tyndall, G. S.; Reeves, M.; Stechman, D.; Stell, M.

2015-12-01

Mercury is a global toxin that can be introduced to ecosystems through atmospheric deposition. Mercury oxidation is thought to occur in the free troposphere by bromine radicals, but direct observational evidence for this process is currently unavailable. During the 2013 Nitrogen, Oxidants, Mercury and Aerosol Distributions, Sources and Sinks campaign, we measured enhanced oxidized mercury and bromine monoxide in a free tropospheric air mass over Texas. We use trace gas measurements, air mass back trajectories, and a chemical box model to confirm the origin and chemical history of the sampled air mass. We find the presence of elevated oxidized mercury to be consistent with oxidation of elemental mercury by bromine atoms in this subsiding upper tropospheric air mass within the subtropical Pacific High, where dry atmospheric conditions are conducive to oxidized mercury accumulation. Our results support the role of bromine as the dominant oxidant of mercury in the upper troposphere.

Global distribution of peroxyacetyl nitrate

NASA Technical Reports Server (NTRS)

Singh, H. B.; Salas, L. J.; Viezee, W.

1986-01-01

Peroxyacetyl nitrate (PAN) atmospheric concentration samples were collected hourly from an ocean vessel 50 mi off the continental coast traveling from Seattle to Chile in 1984. Air concentration data for PAN and light hydrocarbons (LHC) were also taken by aircraft in the same period over Wyoming and Colorado and over the eastern Pacific. The PAN concentrations were higher and more variable in the Northern Hemisphere than in the Southern Hemisphere, increased with altitude, and were higher in the winter than in summer. The summer PAN concentrations were higher in the continental troposphere than in the marine troposphere. The results show that photochemical models of the atmosphere which do not account for the reaction between nonmethane hydrocarbons and PAN will probably overestimate the abundances of NO(x) and HNO3. The collection of further PAN concentration data is recommended as a means to characterizing the moderating role of PAN in the photochemistry of the troposphere.

Stratospheric aerosols from the Sarychev volcano eruption in the 2009 Arctic summer

NASA Astrophysics Data System (ADS)

Jégou, F.; Berthet, G.; Brogniez, C.; Renard, J.-B.; François, P.; Haywood, J. M.; Jones, A.; Bourgeois, Q.; Lurton, T.; Auriol, F.; Godin-Beekmann, S.; Guimbaud, C.; Krysztofiak, G.; Gaubicher, B.; Chartier, M.; Clarisse, L.; Clerbaux, C.; Balois, J. Y.; Verwaerde, C.; Daugeron, D.

2013-07-01

Aerosols from the Sarychev volcano eruption (Kuril Islands, northeast of Japan) were observed in the Arctic lower stratosphere a few days after the strongest SO2 injection which occurred on 15 and 16 June 2009. From the observations provided by the Infrared Atmospheric Sounding Interferometer (IASI) an estimated 0.9 Tg of sulphur dioxide was injected into the upper troposphere and lower stratosphere (UTLS). The resultant stratospheric sulphate aerosols were detected from satellites by the Optical Spectrograph and Infrared Imaging System (OSIRIS) limb sounder and by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and from the surface by the Network for the Detection of Atmospheric Composition Changes (NDACC) lidar deployed at OHP (Observatoire de Haute-Provence, France). By the first week of July the aerosol plume had spread out over the entire Arctic region. The Sarychev-induced stratospheric aerosol over the Kiruna region (north of Sweden) was measured by the Stratospheric and Tropospheric Aerosol Counter (STAC) during eight balloon flights planned in August and September 2009. During this balloon campaign the Micro Radiomètre Ballon (MicroRADIBAL) and the Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NOx (SALOMON) remote-sensing instruments also observed these aerosols. Aerosol concentrations returned to near-background levels by spring 2010. The effective radius, the surface area density (SAD), the aerosol extinction, and the total sulphur mass from STAC in situ measurements are enhanced with mean values in the range 0.15-0.21 μm, 5.5-14.7 μm2 cm-3, 5.5-29.5 × 10-4 km-1, and 4.9-12.6 × 10-10 kg[S] kg-1[air], respectively, between 14 km and 18 km. The observed and modelled e-folding time of sulphate aerosols from the Sarychev eruption is around 70-80 days, a value much shorter than the 12-14 months calculated for aerosols from the 1991 eruption of Mt Pinatubo. The OSIRIS stratospheric aerosol optical depth (AOD) at 750 nm is enhanced by a factor of 6, with a value of 0.02 in late July compared to 0.0035 before the eruption. The HadGEM2 and MIMOSA model outputs indicate that aerosol layers in polar region up to 14-15 km are largely modulated by stratosphere-troposphere exchange processes. The spatial extent of the Sarychev plume is well represented in the HadGEM2 model with lower altitudes of the plume being controlled by upper tropospheric troughs which displace the plume downward and upper altitudes around 18-20 km, in agreement with lidar observations. Good consistency is found between the HadGEM2 sulphur mass density and the value inferred from the STAC observations, with a maximum located about 1 km above the tropopause ranging from 1 to 2 × 10-9 kg[S] kg-1[air], which is one order of magnitude higher than the background level.

Global distribution of alkyl nitrates and their impacts on reactive nitrogen in remote regions constrained by aircraft observations and chemical transport modeling

NASA Astrophysics Data System (ADS)

Fisher, J. A.; Atlas, E. L.; Blake, D. R.; Barletta, B.; Thompson, C. R.; Peischl, J.; Tzompa Sosa, Z. A.; Ryerson, T. B.; Murray, L. T.

2017-12-01

Nitrogen oxides (NO + NO­2 = NOx) are precursors in the formation of tropospheric ozone, contribute to the formation of aerosols, and enhance nitrogen deposition to ecosystems. While direct emissions tend to be localised over continental source regions, a significant source of NOx to the remote troposphere comes from degradation of other forms of reactive nitrogen. Long-lived, small chain alkyl nitrates (RONO2) including methyl, ethyl and propyl nitrates may be particularly significant forms of reactive nitrogen in the remote atmosphere as they are emitted directly by the ocean in regions where reactive nitrogen is otherwise very low. They also act as NOx reservoir species, sequestering NO­x in source regions and releasing it far downwind—and through this process may become increasingly important reservoirs as methane, ethane, and propane emissions grow. However, small RONO2 are not consistently included in global atmospheric chemistry models, and their distributions and impacts remain poorly constrained. In this presentation, we will describe a new RONO2 simulation in the GEOS-Chem chemical transport model evaluated using a large ensemble of aircraft observations collected over a 20-year period. The observations are largely concentrated over the Pacific Ocean, beginning with PEM-Tropics in the late 1990s and continuing through the recent HIPPO and ATom campaigns. Both observations and model show enhanced RONO2 in the tropical Pacific boundary layer that is consistent with a photochemical source in seawater. The model reproduces a similarly large enhancement over the southern ocean by assuming a large pool of oceanic RONO2 here, but the source of the seawater enhancement in this environment remains uncertain. We find that including marine RONO2 in the simulation is necessary to correct a large underestimate in simulated reactive nitrogen throughout the Pacific marine boundary layer. We also find that the impacts on NOx export from continental source regions are limited as RONO2 formation competes with other NO­x reservoirs such as PAN, leading to re-partitioning of reactive nitrogen rather than a net reactive nitrogen source. Further implications for NOx and ozone, as well as the impacts of recent changes in the global distribution of methane, ethane, propane, and NOx emissions, will also be discussed.

Large-Eddy Simulations of Tropical Convective Systems, the Boundary Layer, and Upper Ocean Coupling

DTIC Science & Technology

2014-09-30

warmer profile through greater latent heat release. Resulting temperature profiles all follow essentially moist adiabats in the upper troposphere ...default RRTM ozone concentration profile). Greater convective mixing deepens the tropopause for cases with stronger moisture flux convergence. Case...with tropospheric temperatures about 4 degrees cooler than the original temperature profile. This case represents conditions during the suppressed

Upper tropospheric cloud systems determined from IR Sounders and their influence on the atmosphere

NASA Astrophysics Data System (ADS)

Stubenrauch, Claudia; Protopapadaki, Sofia; Feofilov, Artem; Velasco, Carola Barrientos

2017-02-01

Covering about 30% of the Earth, upper tropospheric clouds play a key role in the climate system by modulating the Earth's energy budget and heat transport. Infrared Sounders reliably identify cirrus down to an IR optical depth of 0.1. Recently LMD has built global cloud climate data records from AIRS and IASI observations, covering the periods from 2003-2015 and 2008-2015, respectively. Upper tropospheric clouds often form mesoscale systems. Their organization and properties are being studied by (1) distinguishing cloud regimes within 2° × 2° regions and (2) applying a spatial composite technique on adjacent cloud pressures, which estimates the horizontal extent of the mesoscale cloud systems. Convective core, cirrus anvil and thin cirrus of these systems are then distinguished by their emissivity. Compared to other studies of tropical mesoscale convective systems our data include also the thinner anvil parts, which make out about 30% of the area of tropical mesoscale convective systems. Once the horizontal and vertical structure of these upper tropospheric cloud systems is known, we can estimate their radiative effects in terms of top of atmosphere and surface radiative fluxes and by computing their heating rates.

Increase in NOx emissions from Indian thermal power plants during 1996-2010: unit-based inventories and multisatellite observations.

PubMed

Lu, Zifeng; Streets, David G

2012-07-17

Driven by rapid economic development and growing electricity demand, NO(x) emissions (E) from the power sector in India have increased dramatically since the mid-1990s. In this study, we present the NO(x) emissions from Indian public thermal power plants for the period 1996-2010 using a unit-based methodology and compare the emission estimates with the satellite observations of NO(2) tropospheric vertical column densities (TVCDs) from four spaceborne instruments: GOME, SCIAMACHY, OMI, and GOME-2. Results show that NO(x) emissions from Indian power plants increased by at least 70% during 1996-2010. Coal-fired power plants, NO(x) emissions from which are not regulated in India, contribute ∼96% to the total power sector emissions, followed by gas-fired (∼4%) and oil-fired (<1%) ones. A number of isolated NO(2) hot spots are observed over the power plant areas, and good agreement between NO(2) TVCDs and NO(x) emissions is found for areas dominated by power plant emissions. Average NO(2) TVCDs over power plant areas were continuously increasing during the study period. We find that the ratio of ΔE/E to ΔTVCD/TVCD changed from greater than one to less than one around 2005-2008, implying that a transition of the overall NO(x) chemistry occurred over the power plant areas, which may cause significant impact on the atmospheric environment.

Evaluating a Space-Based Indicator of Surface Ozone-NOx-VOC Sensitivity Over Midlatitude Source Regions and Application to Decadal Trends

NASA Astrophysics Data System (ADS)

Jin, Xiaomeng; Fiore, Arlene M.; Murray, Lee T.; Valin, Lukas C.; Lamsal, Lok N.; Duncan, Bryan; Folkert Boersma, K.; De Smedt, Isabelle; Abad, Gonzalo Gonzalez; Chance, Kelly; Tonnesen, Gail S.

2017-10-01

Determining effective strategies for mitigating surface ozone (O3) pollution requires knowledge of the relative ambient concentrations of its precursors, NOx, and VOCs. The space-based tropospheric column ratio of formaldehyde to NO2 (FNR) has been used as an indicator to identify NOx-limited versus NOx-saturated O3 formation regimes. Quantitative use of this indicator ratio is subject to three major uncertainties: (1) the split between NOx-limited and NOx-saturated conditions may shift in space and time, (2) the ratio of the vertically integrated column may not represent the near-surface environment, and (3) satellite products contain errors. We use the GEOS-Chem global chemical transport model to evaluate the quantitative utility of FNR observed from the Ozone Monitoring Instrument over three northern midlatitude source regions. We find that FNR in the model surface layer is a robust predictor of the simulated near-surface O3 production regime. Extending this surface-based predictor to a column-based FNR requires accounting for differences in the HCHO and NO2 vertical profiles. We compare four combinations of two OMI HCHO and NO2 retrievals with modeled FNR. The spatial and temporal correlations between the modeled and satellite-derived FNR vary with the choice of NO2 product, while the mean offset depends on the choice of HCHO product. Space-based FNR indicates that the spring transition to NOx-limited regimes has shifted at least a month earlier over major cities (e.g., New York, London, and Seoul) between 2005 and 2015. This increase in NOx sensitivity implies that NOx emission controls will improve O3 air quality more now than it would have a decade ago.

Measurements of NO(x) over the eastern Pacific Ocean and southwestern United States during the spring 1984 NASA GTE aircraft program

NASA Technical Reports Server (NTRS)

Ridley, B. A.; Carroll, M. A.; Dunlap, D. D.; Trainer, M.; Sachse, G. W.; Gregory, G. L.; Condon, E. P.

1989-01-01

Measurements of NO, NO(x) (NO + NO2), O3, and CO are presented from seven aircraft flights made over the eastern Pacific Ocean and the southwestern United States in spring of 1984. The sampling region was characterized by large- and small-scale variability for all of the measurements, likely as a result of vigorous synoptic scale meteorology and the influence of tropopause folds. Median values for NO, NO(x), O3, and CO from the flights made over the ocean in the region of 5.8-7.6 km were 10 parts per trillion by volume (pptv), 32 pptv, 46 parts per billion by volume (ppbv), and 120 ppbv, respectively. Corresponding values from two flights made over the continent at similar altitudes were 16 pptv, 38 pptv, 42 ppbv, and 111 ppbv. There was a strong tendency for NO or NO(x) to be correlated positively with O3 and to be anticorrelated with dew-point/frost-point measurements. No significant overall correlation occurred between NO(x) and CO for the ocean data. The variability of NO(x) was such that regions of net destruction and regions of net production of O(3) were sampled both over the ocean and over the continent. However, in the middle free troposphere over the ocean, net O(3) destruction was predominant.

Importance of chlorine atom oxidation to tropospheric chemistry in an urban, coastal environment

NASA Astrophysics Data System (ADS)

Young, C. J.; Washenfelder, R. A.; Edwards, P.; Gilman, J. B.; Kuster, W. C.; Brown, S. S.

2012-12-01

Chlorine atom contribution to tropospheric chemistry is considered to be small on a global scale. It has been demonstrated to be significant in a few areas, such as the Arctic, using ratios of volatile organic compounds (VOCs) as tracers. During the CalNex campaign in Los Angeles, CA, Cl was shown to be a significant contributor to the primary radical budget. However, ratios of VOCs during this time period show no evidence of Cl atom oxidation. Using the Master Chemical Mechanism model, we investigate this discrepancy. We observe that the VOC ratios are highly dependent on the presence of secondary radicals through radical propagation, which are dependent on NOx levels. Thus, we suggest that in a high-NOx urban environment, VOC ratios are an unsuitable tracer of the importance of Cl chemistry. During the CalNex campaign, Cl atom reactivity is approximately an order of magnitude larger than OH radical reactivity. Further, Cl atoms react preferentially with unsaturated compounds for which OH reaction rates are small. Using the model, we determine the amount of additional ozone that can be expected in Los Angeles as a result of the presence of Cl atom reactivity.

Biomass Burning observed during IAGOS - CARIBIC

NASA Astrophysics Data System (ADS)

Neumaier, Marco; Fischbeck, Garlich; Hermann, Markus; Scharffe, Dieter; Safadi, Layal; Zahn, Andreas

2016-04-01

Biomass Burning observed during IAGOS - CARIBIC Since May 2005 the CARIBIC passenger aircraft (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container - Lufthansa, Airbus 340-600) measures ˜100 trace gases and aerosol components in the UTLS (9-12 km altitude) on 4-6 consecutive long-distance flights per month. Volatile Organic Compounds (VOCs) are measured with a Proton-Transfer-Reaction Mass Spectrometer (PTR-MS). Worldwide ~1.3 Tg/y of acetonitrile (CH3CN) is emitted into the atmosphere almost exclusively from biomass burning (BB) together with other VOCs (e.g. ketones, aldehydes, aromatics), CO, CO2, NOx and aerosol particles. Therefore, and due to its rather long tropospheric lifetime of ~6 months, acetonitrile constitutes a reliable BB tracer. Based on the signal of acetonitrile and CO we checked several algorithms to detect BB plumes in the IAGOS-CARIBIC data set. It turned out that the most intense BB plumes were sampled during summer over North America and during autumn over South America. The results will also be discussed with respect to biases due to flight statistics (i.e. destination, flight season, sampling of tropospheric and stratospheric air, etc.). Two flights that took place during the strong ENSO (El Niño/Southern Oscillation) event in July 2015 between Munich (MUC) and Los Angeles (LAX) will be discussed in more detail by taking into account other VOCs and aerosol particles. Here acetonitrile mixing ratios of up to ~1100 pptv were sampled over Greenland ~0.5 km above the tropopause. It is shown that the sampled air originated from Northern America / Canada where strong wildfires took place. During the flight from LAX to MUC the boundary layer air entered the upper troposphere by isentropic quasi-horizontal mixing and not by fast convective transport. The correlation of some VOCs (i.e. acetone, methanol and acetonitrile) with CO will be discussed and contrasted to findings from the literature. It is shown that in BB affected air masses a good correlation between VOCs and CO is found and that the ΔVOC / ΔCO correlation slopes are significantly smaller compared to correlation slopes measured in the free troposphere.

Extratropical influence of upper tropospheric water vapor on Greenhouse warming

NASA Technical Reports Server (NTRS)

Liu, W. Timothy; Hu, Hua

1997-01-01

Despite its small quantity, the importance of upper tropospheric water vapor is its ability to trap the longwave radiation emitted from the Earth's surface, namely the greenhouse effect. The greenhouse effect is defined quantitatively as the difference between the longwave flux emitted by the Earth's surface and the outgoing longwave radiation (OLR) flux emitted from the top of the atmosphere (TOA) (Raval and Ramanathan 1989).

Global Distribution and Sources of Volatile and Nonvolatile Aerosol In the Remote Troposphere

NASA Technical Reports Server (NTRS)

Singh, Hanwant B.; Avery, M.; Viezee, W.; Che, Y.; Tabazadeh, A.; Hamill, P.; Pueschel, R.; Hannan, J. R.; Anderson, B.; Fuelberg, H. E.;

Long-term tropospheric and lower stratospheric ozone variations from ozonesonde observations

NASA Technical Reports Server (NTRS)

London, J.; Liu, S. C.

1992-01-01

An analysis is presented of the long-term mean pressure-latitude seasonal distribution of tropospheric and lower stratospheric ozone for the four seasons covering, in part, over 20 years of ozonesonde data. The observed patterns show minimum ozone mixing ratios in the equatorial and tropical troposphere except in regions where net photochemical production is dominant. In the middle and upper troposphere, and low stratosphere to 50 mb, ozone increases from the tropics to subpolar latitudes of both hemispheres. In mid stratosphere, the ozone mixing ratio is a maximum over the tropics. The observed vertical ozone gradient is small in the troposphere but increases rapidly above the tropopause. The amplitude of the annual variation increases from a minimum in the tropics to a maximum in polar regions. Also, the amplitude increases with height at all latitudes up to about 30 mb where the phase of the annual variation changes abruptly. The phase of the annual variation is during spring in the boundary layer, summer in mid troposphere, and spring in the upper troposhere and lower stratosphere.

Influence of isoprene chemical mechanism on modelled changes in tropospheric ozone due to climate and land use over the 21st century

NASA Astrophysics Data System (ADS)

Squire, O. J.; Archibald, A. T.; Griffiths, P. T.; Jenkin, M. E.; Smith, D.; Pyle, J. A.

2015-05-01

Isoprene is a~precursor to tropospheric ozone, a key pollutant and greenhouse gas. Anthropogenic activity over the coming century is likely to cause large changes in atmospheric CO2 levels, climate and land use, all of which will alter the global vegetation distribution leading to changes in isoprene emissions. Previous studies have used global chemistry-climate models to assess how possible changes in climate and land use could affect isoprene emissions and hence tropospheric ozone. The chemistry of isoprene oxidation, which can alter the concentration of ozone, is highly complex, therefore it must be parameterised in these models. In this work, we compare the effect of four different reduced isoprene chemical mechanisms, all currently used in Earth system models, on tropospheric ozone. Using a box model we compare ozone in these reduced schemes to that in a more explicit scheme (the Master Chemical Mechanism) over a range of NOx and isoprene emissions, through the use of O3 isopleths. We find that there is some variability, especially at high isoprene emissions, caused by differences in isoprene-derived NOx reservoir species. A global model is then used to examine how the different reduced schemes respond to potential future changes in climate, isoprene emissions, anthropogenic emissions and land use change. We find that, particularly in isoprene-rich regions, the response of the schemes varies considerably. The wide-ranging response is due to differences in the model descriptions of the peroxy radical chemistry, particularly their relative rates of reaction towards NO, leading to ozone formation, or HO2, leading to termination. Also important is the yield of isoprene nitrates and peroxyacyl nitrate precursors from isoprene oxidation. Those schemes that produce less of these NOx reservoir species, tend to produce more ozone locally and less away from the source region. We also note changes in other key oxidants such as NO3 and OH (due to the inclusion of additional isoprene-derived HOx recycling pathways). These have implications for secondary organic aerosol formation, as does the inclusion of an epoxide formation pathway in one of the mechanisms. By combining the emissions and O3 data from all of the global model integrations, we are able to construct isopleth plots comparable to those from the box model analysis. We find that the global and box model isopleths show good qualitative agreement, suggesting that comparing chemical mechanisms with a box model in this framework is a useful tool for assessing mechanistic performance in complex global models. We conclude that as the choice of reduced isoprene mechanism may alter both the magnitude and sign of the ozone response, how isoprene chemistry is parameterised in perturbation experiments such as these is a crucially important consideration. More measurements and laboratory studies are needed to validate these reduced mechanisms especially under high-volatile-organic-compound, low-NOx conditions.

The changing oxidizing environment in London - trends in ozone precursors and their contribution to ozone production

NASA Astrophysics Data System (ADS)

von Schneidemesser, E.; Vieno, M.; Monks, P. S.

2014-01-01

Ground-level ozone is recognized to be a threat to human health (WHO, 2003), have a deleterious impact on vegetation (Fowler et al., 2009), is also an important greenhouse gas (IPCC, 2007) and key to the oxidative ability of the atmosphere (Monks et al., 2009). Owing to its harmful effect on health, much policy and mitigation effort has been put into reducing its precursors - the nitrogen oxides (NOx) and non-methane volatile organic compounds (NMVOCs). The non-linear chemistry of tropospheric ozone formation, dependent mainly on NOx and NMVOC concentrations in the atmosphere, makes controlling tropospheric ozone complex. Furthermore, the concentration of ozone at any given point is a complex superimposition of in-situ produced or destroyed ozone and transported ozone on the regional and hemispheric-scale. In order to effectively address ozone, a more detailed understanding of its origins is needed. Here we show that roughly half (5 μg m-3) of the observed increase in urban (London) ozone (10 μg m-3) in the UK from 1998 to 2008 is owing to factors of local origin, in particular, the change in NO : NO2 ratio, NMVOC : NOx balance, NMVOC speciation, and emission reductions (including NOx titration). In areas with previously higher large concentrations of nitrogen oxides, ozone that was previously suppressed by high concentrations of NO has now been "unmasked", as in London and other urban areas of the UK. The remaining half (approximately 5 μg m-3) of the observed ozone increase is attributed to non-local factors such as long-term transport of ozone, changes in background ozone, and meteorological variability. These results show that a two-pronged approach, local action and regional-to-hemispheric cooperation, is needed to reduce ozone and thereby population exposure, which is especially important for urban ozone.

Glyoxal yield from isoprene oxidation and relation to formaldehyde: chemical mechanism, constraints from SENEX aircraft observations, and interpretation of OMI satellite data

NASA Astrophysics Data System (ADS)

Miller, Christopher Chan; Jacob, Daniel J.; Marais, Eloise A.; Yu, Karen; Travis, Katherine R.; Kim, Patrick S.; Fisher, Jenny A.; Zhu, Lei; Wolfe, Glenn M.; Hanisco, Thomas F.; Keutsch, Frank N.; Kaiser, Jennifer; Min, Kyung-Eun; Brown, Steven S.; Washenfelder, Rebecca A.; González Abad, Gonzalo; Chance, Kelly

2017-07-01

Glyoxal (CHOCHO) is produced in the atmosphere by the oxidation of volatile organic compounds (VOCs). Like formaldehyde (HCHO), another VOC oxidation product, it is measurable from space by solar backscatter. Isoprene emitted by vegetation is the dominant source of CHOCHO and HCHO in most of the world. We use aircraft observations of CHOCHO and HCHO from the SENEX campaign over the southeast US in summer 2013 to better understand the CHOCHO time-dependent yield from isoprene oxidation, its dependence on nitrogen oxides (NOx ≡ NO + NO2), the behavior of the CHOCHO-HCHO relationship, the quality of OMI CHOCHO satellite observations, and the implications for using CHOCHO observations from space as constraints on isoprene emissions. We simulate the SENEX and OMI observations with the Goddard Earth Observing System chemical transport model (GEOS-Chem) featuring a new chemical mechanism for CHOCHO formation from isoprene. The mechanism includes prompt CHOCHO formation under low-NOx conditions following the isomerization of the isoprene peroxy radical (ISOPO2). The SENEX observations provide support for this prompt CHOCHO formation pathway, and are generally consistent with the GEOS-Chem mechanism. Boundary layer CHOCHO and HCHO are strongly correlated in the observations and the model, with some departure under low-NOx conditions due to prompt CHOCHO formation. SENEX vertical profiles indicate a free-tropospheric CHOCHO background that is absent from the model. The OMI CHOCHO data provide some support for this free-tropospheric background and show southeast US enhancements consistent with the isoprene source but a factor of 2 too low. Part of this OMI bias is due to excessive surface reflectivities assumed in the retrieval. The OMI CHOCHO and HCHO seasonal data over the southeast US are tightly correlated and provide redundant proxies of isoprene emissions. Higher temporal resolution in future geostationary satellite observations may enable detection of the prompt CHOCHO production under low-NOx conditions apparent in the SENEX data.

On the Roles of Upper- versus Lower-level Thermal Forcing in Shifting the Eddy-Driven Jet

NASA Astrophysics Data System (ADS)

Zhang, Y.; Nie, Y.; Chen, G.; Yang, X. Q.

2017-12-01

One most drastic atmospheric change in the global warming scenario is the increase in temperature over tropical upper-troposphere and polar surface. The strong warming over those two area alters the spacial distributions of the baroclinicity in the upper-troposphere of subtropics and in the lower-level of subpolar region, with competing effects on the mid-latitude atmospheric circulation. The final destination of the eddy-driven jet in future climate could be "a tug of war" between the impacts of such upper- versus lower-level thermal forcing. In this study, the roles of upper- versus lower-level thermal forcing in shifting the eddy-driven jet are investigated using a nonlinear multi-level quasi-geostrophic channel model. All of our sensitivity experiments show that the latitudinal position of the eddy-driven jet is more sensitive to the upper-level thermal forcing. Such upper-level dominance over the lower-level forcing can be attributed to the different mechanisms through which eddy-driven jet responses to them. The upper-level thermal forcing induces a jet shift mainly by affecting the baroclinic generation of eddies, which supports the latitudinal shift of the eddy momentum flux convergence. The jet response to the lower-level thermal forcing, however, is strongly "eddy dissipation control". The lower-level forcing, by changing the baroclinicity in the lower troposphere, induces a direct thermal zonal wind response in the upper level thus modifies the nonlinear wave breaking and the resultant irreversible eddy mixing, which amplifies the latitudinal shift of the eddy-driven jet. Whether the eddy response is "generation control" or "dissipation control" may strongly depend on the eddy behavior in its baroclinic processes. Only the anomalous eddy generation that penetrates into the upper troposphere can have a striking impact on the eddy momentum flux, which pushes the jet shift more efficiently and dominates the eddy response.

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

NASA Technical Reports Server (NTRS)

Pickering, Kenneth E.; Bucsela, E.; Allen, D.; Prados, A.; Gleason, J.; Kondragunta, S.

2010-01-01

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.

Physical Mechanisms Controlling Upper Tropospheric Water Vapor as Revealed by MLS Data from UARS

NASA Technical Reports Server (NTRS)

Newell, Reginald E.

1998-01-01

The seasonal changes of the upper tropospheric humidity are studied with the water vapor data from the Microwave Limb Sounder on the NASA Upper Atmosphere Research Satellite, and the winds and vertical velocity data obtained from the European Centre for Medium-Range Weather Forecasts. Using the same algorithm for vertical transport as that used for horizontal transport (Zhu and Newell, 1998), we find that the moisture in the tropical upper troposphere may be increased mainly by intensified local convection in a small portion, less than 10%, of the whole area between 40 deg S to 40 deg N. The contribution of large scale background circulations and divergence of horizontal transport is relatively small in these regions. These dynamic processes cannot be revealed by the traditional analyses of moisture fluxes. The negative feedback suggested by Lindzen (1990) also exists, if enhanced convection is concentrated in the tropics, but is apparently not the dominant process in the moisture budget.

Reduction on NOx emissions on urban areas by changing specific vehicle fleets: effects on NO2 and O3 concentration

NASA Astrophysics Data System (ADS)

Goncalves, M.; Jimenez, P.; Baldasano, J.

2007-12-01

The largest amount of NOx emissions in urban areas comes from on-road traffic, which is the largest contributor to urban air pollution (Colvile et al., 2001). Currently different strategies are being tested in order to reduce its effects; many of them oriented to the reduction of the unitary vehicles emissions, by alternative fuels use (such as biofuels, natural gas or hydrogen) or introduction of new technologies (such as hybrid electric vehicles or fuel cells). Atmospheric modelling permits to predict their consequences on tropospheric chemistry (Vautard et al., 2007). Hence, this work assesses the changes on NO2 and O3 concentrations when substituting a 10 per cent of the urban private cars fleets by petrol hybrid electric cars (HEC) or by natural gas cars (NGC) in Madrid and Barcelona urban areas (Spain). These two cities are selected in order to highlight the different patterns of pollutants transport (inland vs. coastal city) and the different responses to emissions reductions. The results focus on a typical summertime episode of air pollution, by means of the Eulerian air quality model ARW- WRF/HERMES/CMAQ, applied with high resolution (1-hr, 1km2) since of the complexity of both areas under study. The detailed emissions scenarios are implemented in the HERMES traffic emissions module, based on the Copert III-EEA/EMEP-CORINAIR (Nztiachristos and Samaras, 2000) methodology. The HEC introduction reduces NOx emissions from on-road traffic in a 10.8 per cent and 8.2 per cent; and the NGC introduction in a 10.3 per cent and 7.8 per cent, for Madrid and Barcelona areas, respectively. The scenarios also affect the NMVOCs reduction (ranging from -3.1 to -6.9 per cent), influencing the tropospheric photochemistry through the NOx/NMVOCs ratio. The abatement of the NO photooxidation but also to the reduction on primary NO2 involves a decrease on NO2 levels centred on urban areas. For example, the NO2 24-hr average concentration in downtown areas reduces up to 8 per cent (-6 μg m-3 on average). The urban areas are VOC-controlled, therefore the reduction on NOx emissions involves a minor increase on tropospheric O3 concentration (Jiménez and Baldasano, 2004), up to 1.5 per cent at some points. Nevertheless, the O3 precursors reduction has positive effects in the downwind areas affected by the urban plume, slightly reducing the O3 levels, but at the regional scale the reduction applied on urban traffic emissions has negligible effects. Both scenarios tested are very similar in terms of emissions reductions and air quality changes, which means that the NOx/NMVOCs ratio do not involve an O3-sensitivity regime variation among scenarios. The HEC scenario is more effective in reducing NO2 levels in urban areas than the NGC scenario (with maximum reductions affecting a larger area) and involves a larger increase in urban O3 concentration.

Subtropical Potential Vorticity Intrusion Drives Increasing Tropospheric Ozone over the Tropical Central Pacific.

PubMed

Nath, Debashis; Chen, Wen; Graf, Hans-F; Lan, Xiaoqing; Gong, Hainan; Nath, Reshmita; Hu, Kaiming; Wang, Lin

2016-02-12

Drawn from multiple reanalysis datasets, an increasing trend and westward shift in the number of Potential Vorticity intrusion events over the Pacific are evident. The increased frequency can be linked to a long-term trend in upper tropospheric equatorial westerly wind and subtropical jets during boreal winter to spring. These may be resulting from anomalous warming and cooling over the western Pacific warm pool and the tropical eastern Pacific, respectively. The intrusions brought dry and ozone rich air of stratospheric origin deep into the tropics. In the tropical upper troposphere, interannual ozone variability is mainly related to convection associated with El Niño/Southern Oscillation. Zonal mean stratospheric overturning circulation organizes the transport of ozone rich air poleward and downward to the high and midlatitudes leading there to higher ozone concentration. In addition to these well described mechanisms, we observe a long-term increasing trend in ozone flux over the northern hemispheric outer tropical (10-25°N) central Pacific that results from equatorward transport and downward mixing from the midlatitude upper troposphere and lower stratosphere during PV intrusions. This increase in tropospheric ozone flux over the Pacific Ocean may affect the radiative processes and changes the budget of atmospheric hydroxyl radicals.

Evidence of Seasonally Dependent Stratosphere-Troposphere Exchange and Purging of Lower Stratospheric Aeroso from a Multi-Year Lidar Dataset

NASA Technical Reports Server (NTRS)

Menzies, R. T.; Tratt, D. M.

1994-01-01

Tropospheric and lower stratospheric aerosol backscatter data obtained from a calibrated backscatter lidar at Pasadena, California (34 deg N latitude)over the 1984-1993 period clearly indicate tightly coupled aerosol optical properties in the upper troposphere and lower stratosphere in the winter and early spring, due to the active mid-latitude stratospheric-tropospheric (ST) exchange processes occurring at this time of year.

Surface measurements of upper tropospheric water vapor isotopic composition on the Chajnantor Plateau, Chile

NASA Astrophysics Data System (ADS)

Galewsky, Joseph; Rella, Christopher; Sharp, Zachary; Samuels, Kimberly; Ward, Dylan

2011-09-01

Simultaneous, real-time measurements of atmospheric water vapor mixing ratio and isotopic composition (δD and δ18O) were obtained using cavity ringdown spectroscopy on the arid Chajnantor Plateau in the subtropical Chilean Andes (elevation 5080 m or 550 hPa; latitude 23°S) during July and August 2010. The measurements show surface water vapor mixing ratio as low as 215 ppmv, δD values as low as -540‰, and δ18O values as low as -68‰, which are the lowest atmospheric water vapor δ values reported from Earth's surface. The results are consistent with previous measurements from the base of the tropical tropopause layer (TTL) and suggest large-scale subsidence of air masses from the upper troposphere to the Earth's surface. The range of measurements is consistent with condensation under conditions of ice supersaturation and mixing with moister air from the lower troposphere that has been processed through shallow convection. Diagnostics using reanalysis data show that the extreme aridity of the Chajnantor Plateau is controlled by condensation in the upper tropical troposphere.

Tropospheric ozone over the North Pacific from ozonesonde observations

NASA Astrophysics Data System (ADS)

Oltmans, S. J.; Johnson, B. J.; Harris, J. M.; Thompson, A. M.; Liu, H. Y.; Chan, C. Y.; VöMel, H.; Fujimoto, T.; Brackett, V. G.; Chang, W. L.; Chen, J.-P.; Kim, J. H.; Chan, L. Y.; Chang, H.-W.

2004-08-01

As part of the Transport and Chemical Evolution over the Pacific (TRACE-P) mission, ozonesondes were used to make ozone vertical profile measurements at nine locations in the North Pacific. At most of the sites there is a multiyear record of observations. From locations in the western Pacific (Hong Kong; Taipei; Jeju Island, Korea; and Naha, Kagoshima, Tsukuba, and Sapporo, Japan), a site in the central Pacific (Hilo, Hawaii), and a site on the west coast of the United States (Trinidad Head, California) both a seasonal and event specific picture of tropospheric ozone over the North Pacific emerges. Ozone profiles over the North Pacific generally show a prominent spring maximum throughout the troposphere. This maximum is tied to the location of the jet stream and its influence on stratosphere-troposphere exchange and the increase in photochemical ozone production through the spring. Prominent layers of enhanced ozone in the middle and upper troposphere north of about 30°N seem to be more closely tied to stratospheric intrusions while biomass burning leads to layers of enhanced ozone in the lower and upper troposphere at Hong Kong (22°N) and Taipei (25°N). The lower free tropospheric layers at Hong Kong are associated with burning in SE Asia, but the upper layer may be associated with either equatorial Northern Hemisphere burning in Africa or SE Asian biomass burning. In the boundary layer at Taipei very high mixing ratios of ozone were observed that result from pollution transport from China in the spring and local urban pollution during the summer. At the ozonesonde site near Tokyo (Tsukuba, 36°N) very large enhancements of ozone are seen in the boundary layer in the summer that are characteristic of urban air pollution. At sites in the mid and eastern Pacific the signature of transport of polluted air from Asia is not readily identifiable from the ozonesonde profile. This is likely due to the more subtle signal and the fact that from the ozone profile and meteorological data by themselves it is difficult to identify such a signal. During the TRACE-P intensive campaign period (February-April 2001), tropospheric ozone amounts were generally typical of those seen in the long-term records of the stations with multiyear soundings. The exception was the upper troposphere over Hong Kong and Taipei where ozone amounts were lower in 2001.

Observations of the upper troposphere and lower stratosphere using the urbana coherent-scatter radar

NASA Technical Reports Server (NTRS)

Goss, L. D.; Bowhill, S. A.

1983-01-01

The Urbana coherent-scatter radar was used to observe the upper troposphere and lower stratosphere, and 134 hours of data were collected. Horizontal wind measurements show good agreement with balloon-measured winds. Gravity waves were frequently observed, and were enhanced during convective activity. Updrafts and downdrafts were observed within thunderstorms. Power returns are related to hydrostatic stability, and changes in echo specularity are shown.

Towards a Model Climatology of Relative Humidity in the Upper Troposphere for Estimation of Contrail and Contrail-Induced Cirrus

NASA Technical Reports Server (NTRS)

Selkirk, Henry B.; Manyin, M.; Ott, L.; Oman, L.; Benson, C.; Pawson, S.; Douglass, A. R.; Stolarski, R. S.

2011-01-01

The formation of contrails and contrail cirrus is very sensitive to the relative humidity of the upper troposphere. To reduce uncertainty in an estimate of the radiative impact of aviation-induced cirrus, a model must therefore be able to reproduce the observed background moisture fields with reasonable and quantifiable fidelity. Here we present an upper tropospheric moisture climatology from a 26-year ensemble of simulations using the GEOS CCM. We compare this free-running model's moisture fields to those obtained from the MLS and AIRS satellite instruments, our most comprehensive observational databases for upper tropospheric water vapor. Published comparisons have shown a substantial wet bias in GEOS-5 assimilated fields with respect to MLS water vapor and ice water content. This tendency is clear as well in the GEOS CCM simulations. The GEOS-5 moist physics in the GEOS CCM uses a saturation adjustment that prevents supersaturation, which is unrealistic when compared to in situ moisture observations from MOZAIC aircraft and balloon sondes as we will show. Further, the large-scale satellite datasets also consistently underestimate super-saturation when compared to the in-situ observations. We place these results in the context of estimates of contrail and contrail cirrus frequency.

Top-down estimates of methane and nitrogen oxide emissions from shale gas production regions using aircraft measurements and a mesoscale Bayesian inversion system together with a flux ratio inversion technique

NASA Astrophysics Data System (ADS)

Cui, Y.; Brioude, J. F.; Angevine, W. M.; McKeen, S. A.; Henze, D. K.; Bousserez, N.; Liu, Z.; McDonald, B.; Peischl, J.; Ryerson, T. B.; Frost, G. J.; Trainer, M.

2016-12-01

Production of unconventional natural gas grew rapidly during the past ten years in the US which led to an increase in emissions of methane (CH4) and, depending on the shale region, nitrogen oxides (NOx). In terms of radiative forcing, CH4 is the second most important greenhouse gas after CO2. NOx is a precursor of ozone (O3) in the troposphere and nitrate particles, both of which are regulated by the US Clean Air Act. Emission estimates of CH4 and NOx from the shale regions are still highly uncertain. We present top-down estimates of CH4 and NOx surface fluxes from the Haynesville and Fayetteville shale production regions using aircraft data collected during the Southeast Nexus of Climate Change and Air Quality (SENEX) field campaign (June-July, 2013) and the Shale Oil and Natural Gas Nexus (SONGNEX) field campaign (March-May, 2015) within a mesoscale inversion framework. The inversion method is based on a mesoscale Bayesian inversion system using multiple transport models. EPA's 2011 National CH4 and NOx Emission Inventories are used as prior information to optimize CH4 and NOx emissions. Furthermore, the posterior CH4 emission estimates are used to constrain NOx emission estimates using a flux ratio inversion technique. Sensitivity of the posterior estimates to the use of off-diagonal terms in the error covariance matrices, the transport models, and prior estimates is discussed. Compared to the ground-based in-situ observations, the optimized CH4 and NOx inventories improve ground level CH4 and O3 concentrations calculated by the Weather Research and Forecasting mesoscale model coupled with chemistry (WRF-Chem).

A Reevaluation of Airborne HO(x) Observations from NASA Field Campaigns

NASA Technical Reports Server (NTRS)

Olson, Jennifer; Crawford, James H.; Chen, Gao; Brune, William H.; Faloona, Ian C.; Tan, David; Harder, Hartwig; Martinez, Monica

2006-01-01

In-situ observations of tropospheric HO(x) (OH and HO2) obtained during four NASA airborne campaigns (SUCCESS, SONEX, PEM-Tropics B and TRACE-P) are reevaluated using the NASA Langley time-dependent photochemical box model. Special attention is given to previously diagnosed discrepancies between observed and predicted HO2 which increase with higher NO(x) levels and at high solar zenith angles. This analysis shows that much of the model discrepancy at high NO(x) during SUCCESS can be attributed to modeling observations at time-scales too long to capture the nonlinearity of HO(x) chemistry under highly variable conditions for NO(x). Discrepancies at high NO(x) during SONEX can be moderated to a large extent by complete use of all available precursor observations. Differences in kinetic rate coefficients and photolysis frequencies available for previous studies versus current recommendations also explain some of the disparity. Each of these causes is shown to exert greater influence with increasing NO(x) due to both the chemical nonlinearity between HO(x) and NO(x) and the increased sensitivity of HO(x) to changes in sources at high NO(x). In contrast, discrepancies at high solar zenith angles will persist until an adequate nighttime source of HO(x) can be identified. It is important to note that this analysis falls short of fully eliminating the issue of discrepancies between observed and predicted HO(x) for high NO(x) environments. These discrepancies are not resolved with the above causes in other data sets from ground-based field studies. Nevertheless, these results highlight important considerations in the application of box models to observationally based predictions of HO(x) radicals.

Measurements of the potential ozone production rate in a forest

NASA Astrophysics Data System (ADS)

Crilley, L.; Sklaveniti, S.; Kramer, L.; Bloss, W.; Flynn, J. H., III; Alvarez, S. L.; Erickson, M.; Dusanter, S.; Locoge, N.; Stevens, P. S.; Millet, D. B.; Alwe, H. D.

2017-12-01

Biogenic volatile organic compounds (BVOC) are a significant source of organic compounds globally and alongside NOx play a key role in the formation of ozone in the troposphere. Understanding how changes in NOx concentrations feed through to altered ozone production in BVOC dominated environments will aid our understanding of future atmospheric composition, notably as developing nations transition from NOx dominated to NOx limited chemistry as a result of mitigation strategies. Here we empirically investigate this ambient ozone formation potential. We report deployment of a custom built instrument to measure in near real time the potential for in situ chemical ozone production, using an artificial light source. Our results are thus indicative of the ozone formation potential for a sampled ambient air mixture, including full VOC complexity, i.e. independent of characterization of individual organic compounds. Ground level measurements were performed as part of the PROPHET-AMOS 2016 field campaign, at a site located within a Northern Michigan forest that has typically low NOx abundance, but high isoprene and terpenoid loadings. As the ambient NOx concentrations were low during the campaign, experiments were performed in which NO was artificially added to the sampled ambient air mixture, to quantify changes in the potential ozone production rate as a function of NOx, and hence the ozone forming characteristics of the ambient air. Preliminarily results from these experiments are presented, and indicate that while ozone production increases with added NO, significant variation was observed for a given NO addition, reflecting differences in the ambient VOC chemical reactivity and ozone formation tendency.

Integrated assessment of health, crop, and climate impacts of mitigating excess diesel NOx emissions in 11 major vehicle markets

NASA Astrophysics Data System (ADS)

Henze, D. K.; Anenberg, S.; Miller, J.; Vicente, F.; Du, L.; Emberson, L.; Lacey, F.; Malley, C.; Minjares, R. J.

2016-12-01

Vehicle emissions contribute to tropospheric ozone and fine particulate matter (PM2.5), impacting human health, crop yields, and climate worldwide. Diesel cars, trucks, and buses produce 70% of global land transportation emissions of nitrogen oxides (NOx), a key PM2.5 and ozone precursor. Despite progressive tightening of regulated NOx emission limits in leading markets, current diesel vehicles emit far more NOx under real-world operating conditions than during laboratory certification testing. Here we show that real-world diesel NOx emissions in 11 markets representing 80% of global diesel vehicle sales are on average 24% higher than certification limits indicate. This excess NOx contributed an estimated 33,000 additional ozone- and PM2.5-related premature deaths globally in 2015, including 6% of all EU-28 ozone- and PM2.5-related premature deaths. Next-generation diesel NOx standards and in-use compliance (more stringent than Euro 6/VI standards) could avoid 358,000 (5%) of global PM2.5- and ozone-related premature deaths in 2040 and up to 4% of ozone-related crop production loss regionally. Impacts of NOx-induced changes in aerosols, methane, and ozone on the global climate are found to present a small net positive radiative forcing (i.e., climate disbenefit), likely outweighed by the climate benefits of reductions to co-emitted black carbon aerosol. In some markets (Australia, Brazil, China, Mexico, and Russia), Euro 6/VI standards alone can achieve most (72-98%) of these health benefits. In India and the EU-28, reducing Euro 6 real-world NOx emissions through strengthened type-approval and in-use emissions testing programs (including market surveillance and expanded emissions test procedure boundaries) would achieve one-third of the health benefits from adopting next generation standards. Our results indicate that implementing stringent and technically feasible NOx emission regulations for diesel vehicles can substantially improve public health.

Study of Nox Emission Characteristics of a 1025t/h Coal-Fired Circulating Fluidized Bed Boiler

NASA Astrophysics Data System (ADS)

Li, Q. Y.; Mi, Z. D.; Zhang, Q. F.

Measurements of emission are carried out in a 1025t/h CFB boiler. The effect of some factors including coal properties, bed temperature, unit load, excess air on the emission of NOx are investigated. The measurement results show that the N concentration in the coal is dominant parameter to predict the NOx emission from a large-scale CFB boiler. NOx emission from the 1025t/h CFB boiler increases with cyclone temperature and upper pressure drop due to post combustion and external cycle.

Measurements of selected C2-C5 hydrocarbons in the troposphere - Latitudinal, vertical, and temporal variations

NASA Technical Reports Server (NTRS)

Singh, Hanwant B.; Viezee, William; Salas, Louis J.

1988-01-01

The tropospheric distribution of 1077 C2-C5 hydrocarbon samples was determined. Shipboard measurements obtained over the eastern Pacific Ocean reveal large north-to-south gradients for most nonmethane hydrocarbons (NMHCs). The results show that NMHC concentrations can decrease by a factor of two or more during the passage of cold fronts in winter and spring, and that upper tropospheric concentrations were lower than those in the lower troposphere.

Impacts and mitigation of excess diesel-related NOx emissions in 11 major vehicle markets

NASA Astrophysics Data System (ADS)

Anenberg, Susan C.; Miller, Joshua; Minjares, Ray; Du, Li; Henze, Daven K.; Lacey, Forrest; Malley, Christopher S.; Emberson, Lisa; Franco, Vicente; Klimont, Zbigniew; Heyes, Chris

2017-05-01

Vehicle emissions contribute to fine particulate matter (PM2.5) and tropospheric ozone air pollution, affecting human health, crop yields and climate worldwide. On-road diesel vehicles produce approximately 20 per cent of global anthropogenic emissions of nitrogen oxides (NOx), which are key PM2.5 and ozone precursors. Regulated NOx emission limits in leading markets have been progressively tightened, but current diesel vehicles emit far more NOx under real-world operating conditions than during laboratory certification testing. Here we show that across 11 markets, representing approximately 80 per cent of global diesel vehicle sales, nearly one-third of on-road heavy-duty diesel vehicle emissions and over half of on-road light-duty diesel vehicle emissions are in excess of certification limits. These excess emissions (totalling 4.6 million tons) are associated with about 38,000 PM2.5- and ozone-related premature deaths globally in 2015, including about 10 per cent of all ozone-related premature deaths in the 28 European Union member states. Heavy-duty vehicles are the dominant contributor to excess diesel NOx emissions and associated health impacts in almost all regions. Adopting and enforcing next-generation standards (more stringent than Euro 6/VI) could nearly eliminate real-world diesel-related NOx emissions in these markets, avoiding approximately 174,000 global PM2.5- and ozone-related premature deaths in 2040. Most of these benefits can be achieved by implementing Euro VI standards where they have not yet been adopted for heavy-duty vehicles.

Nitrous oxide pollution from aircraft to increase by 2050

NASA Astrophysics Data System (ADS)

Bhattacharya, Atreyee

2012-09-01

The transportation industry is not only one of the biggest sources of air pollution and a significant player in greenhouse gas-induced global warming, but, as a new study shows, the industry could also be responsible for episodes of ozone (O3 ) pollution, particularly over the United States and northern Europe. Combustion of fuel in cars, shipping vessels, and low-flying aircraft produce nitrogen oxides (NOx), which not only decrease the lifetime of greenhouse gases such as methane but also react with other molecules in the atmosphere to form tropospheric O3, another, more lethal, air pollutant. Hauglustaine and Koff used a global three-dimensional chemistry-climate model to investigate how different components of the transportation industry—cars, ships, and low-flying aircraft—would contribute to NOx pollution over the next few decades under several projected emission scenarios. They found that as road transportation stagnates or even declines due to stricter regulations and congestion, NOx emissions from cars will decrease over time. However, aircraft will increase in number and could contribute between 25% and 48% of NOx emissions, which will be most severe over the United States and Europe—two regions with the highest growth rate in commercial aviation.

Using Passive Sampling to Asses Ozone Formation in Sparsely Monitored Areas

NASA Astrophysics Data System (ADS)

Crosby, C. M.; Mainord, J.; George, L. A.

2016-12-01

Tropospheric ozone (O3), a secondary pollutant, is detrimental to both human health and the environment. O3 is formed from nitrogen oxides (NOx) and volatile organic compounds, (VOC's) in the presence of sunlight. Hermiston is a low population rural city in Oregon (17,707), where O3 levels are expected to be minimal. However, Hermiston has recently experienced elevated O3 concentrations, approaching EPA levels of non-attainment. These levels were not predicted by airshed modeling of the region, suggesting that precursor emissions are not adequately represented in the model. Due to the limited monitoring in the area, there are no measurements of precursors in the region. In this study, passive Ogawa samplers were used to measure NOx and O3 levels at twenty sites in the area. The concentrations were then mapped in conjunction with wind trajectories derived from HYSPLIT and compared to NOx point sources attained from the National Emissions Inventory (NEI). The measurement campaign revealed areas of elevated NOx concentrations that were not accounted for in the airshed model. Further exploration is needed to identify these sources. This study lays groundwork for the use of passive sampling to ground-truth airshed models in the absence of monitoring networks.

Saharan dust, convective lofting, aerosol enhancement zones, and potential impacts on ice nucleation in the tropical upper troposphere

NASA Astrophysics Data System (ADS)

Twohy, C. H.; Anderson, B. E.; Ferrare, R. A.; Sauter, K. E.; L'Ecuyer, T. S.; van den Heever, S. C.; Heymsfield, A. J.; Ismail, S.; Diskin, G. S.

2017-08-01

Dry aerosol size distributions and scattering coefficients were measured on 10 flights in 32 clear-air regions adjacent to tropical storm anvils over the eastern Atlantic Ocean. Aerosol properties in these regions were compared with those from background air in the upper troposphere at least 40 km from clouds. Median values for aerosol scattering coefficient and particle number concentration >0.3 μm diameter were higher at the anvil edges than in background air, showing that convective clouds loft particles from the lower troposphere to the upper troposphere. These differences are statistically significant. The aerosol enhancement zones extended 10-15 km horizontally and 0.25 km vertically below anvil cloud edges but were not due to hygroscopic growth since particles were measured under dry conditions. Number concentrations of particles >0.3 μm diameter were enhanced more for the cases where Saharan dust layers were identified below the clouds with airborne lidar. Median number concentrations in this size range increased from 100 l-1 in background air to 400 l-1 adjacent to cloud edges with dust below, with larger enhancements for stronger storm systems. Integration with satellite cloud frequency data indicates that this transfer of large particles from low to high altitudes by convection has little impact on dust concentrations within the Saharan Air Layer itself. However, it can lead to substantial enhancement in large dust particles and, therefore, heterogeneous ice nuclei in the upper troposphere over the Atlantic. This may induce a cloud/aerosol feedback effect that could impact cloud properties in the region and downwind.

Global distribution and sources of volatile and nonvolatile aerosol in the remote troposphere

NASA Astrophysics Data System (ADS)

Singh, Hanwant B.; Anderson, B. E.; Avery, M. A.; Viezee, W.; Chen, Y.; Tabazadeh, A.; Hamill, P.; Pueschel, R.; Fuelberg, H. E.; Hannan, J. R.

2002-06-01

Airborne measurements of aerosol (condensation nuclei, CN) and selected trace gases made over areas of the North Atlantic Ocean during Subsonic Assessment (SASS) Ozone and Nitrogen Oxide Experiment (SONEX) (October/November 1997), the south tropical Pacific Ocean during Pacific Exploratory Mission (PEM)-Tropics A (September/October 1996), and PEM-Tropics B (March/April 1999) have been analyzed. The emphasis is on interpreting variations in the number densities of fine (>17 nm) and ultrafine (>8 nm) aerosol in the upper troposphere (8-12 km). These data suggest that large number densities of highly volatile CN (104 - 105 cm-3) are present in the upper troposphere and particularly over the tropical/subtropical region. CN number densities in all regions are largest when the atmosphere is devoid of nonvolatile particles. Through marine convection and long-distance horizontal transport, volatile CN originating from the tropical/subtropical regions can frequently impact the abundance of aerosol in the middle and upper troposphere at mid to high latitudes. Nonvolatile aerosols behave in a manner similar to tracers of combustion (CO) and photochemical pollution (peroxyacetylnitrate (PAN)), implying a continental pollution source from industrial emissions or biomass burning. In the upper troposphere we find that volatile and nonvolatile aerosol number densities are inversely correlated. Results from an aerosol microphysical model suggest that the coagulation of fine volatile particles with fewer but larger nonvolatile particles, of principally anthropogenic origin, is one possible explanation for this relationship. In some instances the larger nonvolatile particles may also directly remove precursors (e.g., H2SO4) and effectively stop nucleation.

Tropical storm redistribution of Saharan dust to the upper troposphere and ocean surface

NASA Astrophysics Data System (ADS)

Herbener, Stephen R.; Saleeby, Stephen M.; Heever, Susan C.; Twohy, Cynthia H.

2016-10-01

As a tropical cyclone traverses the Saharan Air Layer (SAL), the storm will spatially redistribute the dust from the SAL. Dust deposited on the surface may affect ocean fertilization, and dust transported to the upper levels of the troposphere may impact radiative forcing. This study explores the relative amounts of dust that are vertically redistributed when a tropical cyclone crosses the SAL. The Regional Atmospheric Modeling System (RAMS) was configured to simulate the passage of Tropical Storm Debby (2006) through the SAL. A dust mass budget approach has been applied, enabled by a novel dust mass tracking capability of the model, to determine the amounts of dust deposited on the ocean surface and transferred aloft. The mass of dust removed to the ocean surface was predicted to be nearly 2 orders of magnitude greater than the amount of dust transported to the upper troposphere.

Solubility of methanol in low-temperature aqueous sulfuric acid and implications for atmospheric particle composition

NASA Technical Reports Server (NTRS)

Iraci, Laura T.; Essin, Andrew M.; Golden, David M.; Hipskind, R. Stephen (Technical Monitor)

2001-01-01

Using traditional Knudsen cell techniques, we find well-behaved Henry's law uptake of methanol in aqueous 45 - 70 wt% H2SO4 solutions at temperatures between 197 and 231 K. Solubility of methanol increases with decreasing temperature and increasing acidity, with an effective Henry's law coefficient ranging from 10(exp 5) - 10(exp 8) M/atm. Equilibrium uptake of methanol into sulfuric acid aerosol particles in the upper troposphere and lower stratosphere will not appreciably alter gas-phase concentrations of methanol. The observed room temperature reaction between methanol and sulfuric acid is too slow to provide a sink for gaseous methanol at the temperatures of the upper troposphere and lower stratosphere. It is also too slow to produce sufficient quantities of soluble reaction products to explain the large amount of unidentified organic material seen in particles of the upper troposphere.

Evaluation of Satellite-Based Upper Troposphere Cloud Top Height Retrievals in Multilayer Cloud Conditions During TC4

NASA Technical Reports Server (NTRS)

Chang, Fu-Lung; Minnis, Patrick; Ayers, J. Kirk; McGill, Matthew J.; Palikonda, Rabindra; Spangenberg, Douglas A.; Smith, William L., Jr.; Yost, Christopher R.

2010-01-01

Upper troposphere cloud top heights (CTHs), restricted to cloud top pressures (CTPs) less than 500 hPa, inferred using four satellite retrieval methods applied to Twelfth Geostationary Operational Environmental Satellite (GOES-12) data are evaluated using measurements during the July August 2007 Tropical Composition, Cloud and Climate Coupling Experiment (TC4). The four methods are the single-layer CO2-absorption technique (SCO2AT), a modified CO2-absorption technique (MCO2AT) developed for improving both single-layered and multilayered cloud retrievals, a standard version of the Visible Infrared Solar-infrared Split-window Technique (old VISST), and a new version of VISST (new VISST) recently developed to improve cloud property retrievals. They are evaluated by comparing with ER-2 aircraft-based Cloud Physics Lidar (CPL) data taken during 9 days having extensive upper troposphere cirrus, anvil, and convective clouds. Compared to the 89% coverage by upper tropospheric clouds detected by the CPL, the SCO2AT, MCO2AT, old VISST, and new VISST retrieved CTPs less than 500 hPa in 76, 76, 69, and 74% of the matched pixels, respectively. Most of the differences are due to subvisible and optically thin cirrus clouds occurring near the tropopause that were detected only by the CPL. The mean upper tropospheric CTHs for the 9 days are 14.2 (+/- 2.1) km from the CPL and 10.7 (+/- 2.1), 12.1 (+/- 1.6), 9.7 (+/- 2.9), and 11.4 (+/- 2.8) km from the SCO2AT, MCO2AT, old VISST, and new VISST, respectively. Compared to the CPL, the MCO2AT CTHs had the smallest mean biases for semitransparent high clouds in both single-layered and multilayered situations whereas the new VISST CTHs had the smallest mean biases when upper clouds were opaque and optically thick. The biases for all techniques increased with increasing numbers of cloud layers. The transparency of the upper layer clouds tends to increase with the numbers of cloud layers.

The photochemistry of anthropogenic nonmethane hydrocarbons in the troposphere

NASA Technical Reports Server (NTRS)

Brewer, D. A.; Augustsson, T. R.; Levine, J. S.

1983-01-01

A lumped, nonmethane hydrocarbon (NMHC) chemical mechanism is presently applied to a one-dimensional photochemical model of the troposphere. The profiles of OH, HO2, NO(x), and HNO3, showed only slight changes when NMHC chemistry was added. The integrated column of peroxyacetylnitrate (PAN), when NMHC chemistry was included, comprised 17 percent of the odd nitrogen budget. Advection is noted as an important possible mechanism for the removal of PAN at midlatitudes. The inclusion of such intermediate lifetime species as aldehydes and olefins has both provided additional sources of short-lived NMHC radicals, such as the peroxyacetyl radical that is the radical precursor of PAN, and offered a more detailed description of the concentrations of short-lived species and the overall NMHC chemistry.

Quantifying the isotopic composition of NOx emission sources: An analysis of collection methods

NASA Astrophysics Data System (ADS)

Fibiger, D.; Hastings, M.

2012-04-01

We analyze various collection methods for nitrogen oxides, NOx (NO2 and NO), used to evaluate the nitrogen isotopic composition (δ15N). Atmospheric NOx is a major contributor to acid rain deposition upon its conversion to nitric acid; it also plays a significant role in determining air quality through the production of tropospheric ozone. NOx is released by both anthropogenic (fossil fuel combustion, biomass burning, aircraft emissions) and natural (lightning, biogenic production in soils) sources. Global concentrations of NOx are rising because of increased anthropogenic emissions, while natural source emissions also contribute significantly to the global NOx burden. The contributions of both natural and anthropogenic sources and their considerable variability in space and time make it difficult to attribute local NOx concentrations (and, thus, nitric acid) to a particular source. Several recent studies suggest that variability in the isotopic composition of nitric acid deposition is related to variability in the isotopic signatures of NOx emission sources. Nevertheless, the isotopic composition of most NOx sources has not been thoroughly constrained. Ultimately, the direct capture and quantification of the nitrogen isotopic signatures of NOx sources will allow for the tracing of NOx emissions sources and their impact on environmental quality. Moreover, this will provide a new means by which to verify emissions estimates and atmospheric models. We present laboratory results of methods used for capturing NOx from air into solution. A variety of methods have been used in field studies, but no independent laboratory verification of the efficiencies of these methods has been performed. When analyzing isotopic composition, it is important that NOx be collected quantitatively or the possibility of fractionation must be constrained. We have found that collection efficiency can vary widely under different conditions in the laboratory and fractionation does not vary predictably with collection efficiency. For example, prior measurements frequently utilized triethanolamine solution for collecting NOx, but the collection efficiency was found to drop quickly as the solution aged. The most promising method tested is a NaOH/KMnO4 solution (Margeson and Knoll, Anal. Chem., 1985) which can collect NOx quantitatively from the air. Laboratory tests of previously used methods, along with progress toward creating a suitable and verifiable field deployable collection method will be presented.

Effects of Deep Convection on Atmospheric Chemistry

NASA Technical Reports Server (NTRS)

Pickering, Kenneth E.

2007-01-01

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.

The Use of Sage Water Vapor Data for Investigating Climate Change Issues

NASA Technical Reports Server (NTRS)

Rind, D.

2003-01-01

SAGE water vapor data has proven valuable for addressing several of the important issues in climate change research. It has been used to investigate how the upper troposphere water vapor responds to warming and convection, a key question in understanding the water vapor feedback to anthropogenic global warming. In the case of summer versus winter differences, SAGE results showed that the upper tropospheric relative humidity remained approximately constant; this result was in general agreement with how a GCM handled the seasonal difference, and gave credence to the argument that the GCM was not overestimating the water vapor feedback associated with convection. In addition, the convection-water vapor relationship was investigated further using SAGE water vapor and ISCCP cloud data. The results showed that upper tropospheric drying did appear to occur simultaneously with deep convective events in the tropics, only to be replaced by moistening a few hours later, associated (most likely) with the reevaporation of moisture from anvil clouds. The total effect was, again, a moistening of the upper troposphere associated with convection. Calculation of the actual trends in upper tropospheric moisture is a potential goal for SAGE data usage; trends calculated with radiosonde data, or instruments calibrated with radiosonde data have the problem of the effect of changing radiosonde instruments. SAGE data have in effect been used to compare different radiosondes through comparisons, and could continue to do so. SAGE 3 should also help clarify the absolute accuracy of SAGE retrievals in the troposphere. and its consequences. Model results show that water vapor increases can help explain the observations of stratospheric cooling, along with increasing C02 and ozone reduction. SAGE has been shown to provide trends similar to those of some other satellite and in situ retrievals, with increasing water vapor over time. However, SAGE is impacted by aerosol contamination which must be removed from the data; approaches used in the past will be reviewed. The SAGE water vapor errors, if taken literally, would make it hard to justify using SAGE data for such trends, and the error bars must be investigated. Stratospheric water vapor increases, like tropospheric increases, would lead to noticeable warming at the surface, and their changes must be quantified.

Laboratory Studies of Homogeneous and Heterogeneous Chemical Processes of Importance in the Upper Atmosphere

NASA Technical Reports Server (NTRS)

Molina, Mario J.

2003-01-01

The objective of this study was to conduct measurements of chemical kinetics parameters for reactions of importance in the stratosphere and upper troposphere, and to study the interaction of trace gases with ice surfaces in order to elucidate the mechanism of heterogeneous chlorine activation processes, using both a theoretical and an experimental approach. The measurements were carried out under temperature and pressure conditions covering those applicable to the stratosphere and upper troposphere. The main experimental technique employed was turbulent flow-chemical ionization mass spectrometry, which is particularly well suited for investigations of radical-radical reactions.

A comparison of the structure and flow characteristics of the upper troposphere and stratosphere of the Northern and Southern Hemispheres

NASA Technical Reports Server (NTRS)

Adler, R. F.

1974-01-01

The general circulations of the Northern and Southern Hemispheres are compared with regard to the upper troposphere and stratosphere using atmospheric structure obtained from satellite, multi-channel radiance data. Specifically, the data are from the Satellite Infrared Spectrometer (SIRS) instrument aboard the Nimbus 3 spacecraft. The inter-hemispheric comparisons are based on two months of data (one summer month and one winter month) in each hemisphere. Topics studied include: mean meridional circulation in the Southern Hemisphere stratosphere; magnitude and distribution of tropospheric eddy heat flux; magnitudes of energy cycle components; and the relation of vortex structure to the breakdown climatology of the Antarctic stratospheric polar vortex.

Western Pacific Tropospheric Ozone and Potential Vorticity: Implications for Asian Pollution

NASA Technical Reports Server (NTRS)

Browell, Edward V.; Newell, Reginald E.; Davis, Douglas D.; Liu, Shaw C.

1997-01-01

Tropospheric ozone (03) cross sections measured with lidar from a DC-8 aircraft over the western Pacific correspond closely with potential vorticity (PV). Both are transported from the middle latitude stratosphere, although this is not the only source of 03, and both have sinks in the tropical boundary layer. 03 and PV are good indicators of photochemical and transport process interactions. In summer, some Asian pollution, raised by convection to the upper troposphere, passes southward into the tropics and to the Southern Hemisphere. In winter, subsidence keeps the pollution at low altitudes where it moves over the ocean towards the Inter-Tropical Convergence Zone (ITCZ), with photochemical destruction and secondary pollutant generation occurring en route. Convection raises this modified air to the upper troposphere, where some re may enter the stratosphere. Thus winter Asian pollution may at have a smaller direct influence on the global atmosphere than it would if injected at other longitudes and seasons.

The Response of Tropical Tropospheric Ozone to ENSO

NASA Technical Reports Server (NTRS)

Oman, L. D.; Ziemke, J. R.; Douglass, A. R.; Waugh, D. W.; Lang, C.; Rodriguez, J. M.; Nielsen, J. E.

2011-01-01

We have successfully reproduced the Ozone ENSO Index (OEI) in the Goddard Earth Observing System (GEOS) chemistry-climate model (CCM) forced by observed sea surface temperatures over a 25-year period. The vertical ozone response to ENSO is consistent with changes in the Walker circulation. We derive the sensitivity of simulated ozone to ENSO variations using linear regression analysis. The western Pacific and Indian Ocean region shows similar positive ozone sensitivities from the surface to the upper troposphere, in response to positive anomalies in the Nino 3.4 Index. The eastern and central Pacific region shows negative sensitivities with the largest sensitivity in the upper troposphere. This vertical response compares well with that derived from SHADOZ ozonesondes in each region. The OEI reveals a response of tropospheric ozone to circulation change that is nearly independent of changes in emissions and thus it is potentially useful in chemistry-climate model evaluation.

Vertical transport of ozone and CO during super cyclones in the Bay of Bengal as detected by Tropospheric Emission Spectrometer.

PubMed

Fadnavis, S; Beig, G; Buchunde, P; Ghude, Sachin D; Krishnamurti, T N

2011-02-01

Vertical profiles of carbon monoxide (CO) and ozone retrieved from Tropospheric Emission Spectrometer have been analyzed during two super cyclone systems Mala and Sidr. Super cyclones Mala and Sidr traversed the Bay of Bengal (BOB) region on April 24-29, 2006 and November 12-16, 2007 respectively. The CO and ozone plume is observed as a strong enhancement of these pollutants in the upper troposphere over the BOB, indicating deep convective transport. Longitude-height cross-section of these pollutants shows vertical transport to the upper troposphere. CO mixing ratio ~90 ppb is observed near the 146-mb level during the cyclone Mala and near 316 mb during the cyclone Sidr. Ozone mixing ratio ~60-100 ppb is observed near the 316-mb level during both the cyclones. Analysis of National Centers for Environmental Prediction (NCEP) reanalysis vertical winds (omega) confirms vertical transport in the BOB.

A two-dimensional study of ethane and propane oxidation in the troposphere

NASA Technical Reports Server (NTRS)

Kanakidou, M.; Valentin, K. M.; Crutzen, P. J.; Singh, H. B.

1991-01-01

The chemistry of ethane and propane is studied using a global two-dimensional 'zonally averaged' height- and latitude-dependent tropospheric model. The purpose of the study is to derive theoretical estimates of the seasonal and latitudinal distributions of a variety of intermediate organic compounds formed by the photochemical oxidation of C2H6 and C3H8. It is shown that C2H6 and C3H8 emitted at rates of 16 Tg C2H6/a and 23 Tg C3H8/a do not affect the overall photochemistry of the troposphere significantly. Major global effects on O3 and OH concentrations are suggested to be coming from the formation of peroxyacetyl nitrate by the interactions of NOx with other hydrocarbons with strong and spatially correlated anthropogenic or natural sources at the earth's surface. It is pointed out that attention should be given to organic nitrates produced by the oxidation of NMHC other than C2H6 and C3H8.

Trends of Rural Tropospheric Ozone at the Northwest of the Iberian Peninsula

PubMed Central

Saavedra, S.; Rodríguez, A.; Souto, J. A.; Casares, J. J.; Bermúdez, J. L.; Soto, B.

2012-01-01

Tropospheric ozone levels around urban and suburban areas at Europe and North America had increased during 80's–90's, until the application of NOx reduction strategies. However, as it was expected, this ozone depletion was not proportional to the emissions reduction. On the other hand, rural ozone levels show different trends, with peaks reduction and average increments; this different evolution could be explained by either emission changes or climate variability in a region. In this work, trends of tropospheric ozone episodes at rural sites in the northwest of the Iberian Peninsula were analyzed and compared to others observed in different regions of the Atlantic European coast. Special interest was focused on the air quality sites characterization, in order to guarantee their rural character in terms of air quality. Both episodic local meteorological and air quality measurements along five years were considered, in order to study possible meteorological influences in ozone levels, different to other European Atlantic regions. PMID:22649298

Trends of rural tropospheric ozone at the northwest of the Iberian Peninsula.

PubMed

Saavedra, S; Rodríguez, A; Souto, J A; Casares, J J; Bermúdez, J L; Soto, B

2012-01-01

Tropospheric ozone levels around urban and suburban areas at Europe and North America had increased during 80's-90's, until the application of NO(x) reduction strategies. However, as it was expected, this ozone depletion was not proportional to the emissions reduction. On the other hand, rural ozone levels show different trends, with peaks reduction and average increments; this different evolution could be explained by either emission changes or climate variability in a region. In this work, trends of tropospheric ozone episodes at rural sites in the northwest of the Iberian Peninsula were analyzed and compared to others observed in different regions of the Atlantic European coast. Special interest was focused on the air quality sites characterization, in order to guarantee their rural character in terms of air quality. Both episodic local meteorological and air quality measurements along five years were considered, in order to study possible meteorological influences in ozone levels, different to other European Atlantic regions.

Rain-induced emission pulses of NOx and HCHO from soils in African regions after dry spells as viewed by satellite sensors

NASA Astrophysics Data System (ADS)

Zörner, Jan; Penning de Vries, Marloes; Beirle, Steffen; Veres, Patrick; Williams, Jonathan; Wagner, Thomas

2014-05-01

Outside industrial areas, soil emissions of NOx (stemming from bacterial emissions of NO) represent a considerable fraction of total NOx emissions, and may even dominate in remote tropical and agricultural areas. NOx fluxes from soils are controlled by abiotic and microbiological processes which depend on ambient environmental conditions. Rain-induced spikes in NOx have been observed by in-situ measurements and also satellite observations. However, the estimation of soil emissions over broad geographic regions remains uncertain using bottom-up approaches. Independent, global satellite measurements can help constrain emissions used in chemical models. Laboratory experiments on soil fluxes suggest that significant HCHO emissions from soil can occur. However, it has not been previously attempted to detect HCHO emissions from wetted soils by using satellite observations. This study investigates the evolution of tropospheric NO2 (as a proxy for NOx) and HCHO column densities before and after the first rain fall event following a prolonged dry period in semi-arid regions, deserts as well as tropical regions in Africa. Tropospheric NO2 and HCHO columns retrieved from OMI aboard the AURA satellite, GOME-2 aboard METOP and SCIAMACHY aboard ENVISAT are used to study and inter-compare the observed responses of the trace gases with multiple space-based instruments. The observed responses are prone to be affected by other sources like lightning, fire, influx from polluted air masses, as well measurement errors in the satellite retrieval caused by manifold reasons such as an increased cloud contamination. Thus, much care is taken verify that the observed spikes reflect enhancements in soil emissions. Total column measurements of H2O from GOME-2 give further insight into the atmospheric state and help to explain the increase in humidity before the first precipitation event. The analysis is not only conducted for averages of distinct geographic regions, i.e. the Sahel, but also for higher resolution grid boxes to map the spatial pattern of absolute and relative enhancements after the wetting of dry soils. At the beginning of the wet season in the Sahel in April/May/June strong NO2 VCD enhancements compared to the background levels are observed by all three satellite sensors. A significant enhancement in HCHO VCD is also detected with GOME-2. Further analysis shows that spatial patterns and the magnitude of such enhancements over Africa are highly dependent on the season, prevailing temperatures and land cover types.

Radicals and Aerosols in the Troposphere and Lower Stratosphere

NASA Astrophysics Data System (ADS)

Volkamer, Rainer; Koenig, Theodore; Dix, Barbara

2016-06-01

The remote tropical free troposphere (FT) is one of the most relevant atmospheric environments on Earth. About 75% of the global tropospheric O3 and CH4 loss occurs at tropical latitudes. Tropospheric bromine and iodine catalytically destroy tropospheric O3, oxidize atmospheric mercury, and modify oxidative capacity, and aerosols. Oxygenated VOCs (OVOC) modify HOx (= OH + HO2), NOx (= NO + NO2), tropospheric O3, aerosols, and are a sink for BrOx (= Br + BrO). Until recently, atmospheric models were untested for lack of vertically resolved measurements of BrO and IO radicals in the tropical troposphere. BrO and IO are highly reactive trace gases. Even very low concentrations (parts per trillion; 1 pptv = 10-12 volume mixing ratio) can significantly modify the lifetime of climate active gases, and determine (bromine) the rate limiting step of mercury oxidation in air (that is washed out, and subsequently bio-accumulates in fish). Analytical challenges arise when these radicals modify in sampling lines. Sensitive yet robust, portable, and inherently calibrated measurements directly in the open atmosphere have recently been demonstrated by means of limb-measurements of scattered solar photons by the University of Colorado Airborne Multi-AXis DOAS instrument (CU AMAX-DOAS) from research aircraft. The CU AMAX-DOAS instrument is optimized to (1) locate BrO, IO and glyoxal (a short lived OVOC) in the troposphere, (2) decouple stratospheric absorbers, (3) maximize sensitivity at instrument altitude, (4) facilitate altitude control and (5) enable observations over a wide range of solar zenith angles. Further, (6) the filling-in of Fraunhofer lines (Ring-effect) by Raman Scattering offers interesting opportunities for radiative closure studies to assess the effects of aerosols on Climate.

Impacts of the large increase in international ship traffic 2000-2007 on tropospheric ozone and methane.

PubMed

Dalsøren, Stig B; Eide, Magnus S; Myhre, Gunnar; Endresen, Oyvind; Isaksen, Ivar S A; Fuglestvedt, Jan S

2010-04-01

The increase in civil world fleet ship emissions during the period 2000-2007 and the effects on key tropospheric oxidants are quantified using a global Chemical Transport Model (CTM). We estimate a substantial increase of 33% in global ship emissions over this period. The impact of ship emissions on tropospheric oxidants is mainly caused by the relatively large fraction of NOx in ship exhaust. Typical increases in yearly average surface ozone concentrations in the most impacted areas are 0.5-2.5 ppbv. The global annual mean radiative forcing due to ozone increases in the troposphere is 10 mWm(-2) over the period 2000-2007. We find global average tropospheric OH increase of 1.03% over the same period. As a result of this the global average tropospheric methane concentration is reduced by approximately 2.2% over a period corresponding to the turnover time. The resulting methane radiative forcing is -14 mWm(-2) with an additional contribution of -6 mWm(-2) from methane induced reduction in ozone. The net forcing of the ozone and methane changes due to ship emissions changes between 2000 and 2007 is -10 mWm(-2). This is significant compared to the net forcing of these components in 2000. Our findings support earlier observational studies indicating that ship traffic may be a major contributor to recent enhancement of background ozone at some coastal stations. Furthermore, by reducing global mean tropospheric methane by 40 ppbv over its turnover time it is likely to contribute to the recent observed leveling off in global mean methane concentration.

Increasing Anthropogenic Emissions in China Offset Air Quality Policy Efforts in Western United States: A Satellite and Modelling Perspective

NASA Astrophysics Data System (ADS)

Boersma, F. F.; Verstraeten, W. W.; Williams, J. E.; Neu, J. L.; Bowman, K. W.; Worden, J.

2014-12-01

Tropospheric ozone is an important greenhouse gas and a global air pollutant originating from photo-chemical oxidation of ozone precursors in the presence of NOX. Eastern Asia has the fastest growing anthropogenic emissions in the world, possibly affecting both the pollution in the local troposphere as well as in the trans-Pacific region. Local measurements over Asia show that tropospheric ozone has increased by 1 to 3% per year since the start of the millennium. This increase is often invoked to explain positive ozone trends observed in western United States, but to date there is no unambiguous evidence showing that enhanced Asian pollution is responsible for these trends. Here we interpret satellite measurements of tropospheric ozone and its precursor nitrate dioxide from the Aura Tropospheric Emission Spectrometer (TES) and Ozone Monitoring Instrument (OMI) using the TM5 global chemistry-transport model to directly show that tropospheric ozone over China has increased by ~10% from 2005-2010 in response to both a ~15% rise in Chinese emissions and an increased downward ozone transport from the stratosphere. What is more, we demonstrate that Chinese export of ozone and its precursors have offset one-third of the reduction in free tropospheric ozone over the western United States that should have occurred during 2005-2010 via emissions reductions associated with air quality policies in the United States. The issue of export and long-range transport of pollution from other countries indicates that global efforts may be required to address both the global as well as the regional air quality and climate change.

The Origins of Air Parcels Uplifted in a Two Dimensional Gravity Wave in the Tropical Upper Troposphere During the NASA Stratosphere Troposphere Exchange Project (STEP)

NASA Technical Reports Server (NTRS)

Selkirk, Henry B.; Pfister, Leonhard; Chan, K. Roland; Kritz, Mark; Kelly, Ken

1989-01-01

During January and February 1987, as part of the Stratosphere-Troposphere Exchange Project, the NASA ER-2 made 11 flights from Darwin, Australia to investigate dehydration mechanisms in the vicinity of the tropical tropopause. After the monsoon onset in the second week of January, steady easterly flow of 15-25 ms (exp -1) was established in the upper troposphere and lower stratosphere over northern Australia and adjacent seas. Penetrating into this regime were elements of the monsoon convection such as overshooting convective turrets and extensive anvils including cyclone cloud shields. In cases of the latter, the resulting flow obstructions tended to produce mesoscale gravity waves. In several instances the ER- 2 meteorological and trace constituent measurements provide a detailed description of the structure of these gravity waves. Among these was STEP Flight 6, 22-23 January. It is of particular interest to STEP because of the close proximity of ice-laden and dehydrated air on the same isentropic surfaces. Convective events inject large amounts of ice into the upper troposphere and lower stratosphere which may not be completely removed by local precipitation processes. In the present instance, a gravity wave for removed from the source region appears to induce relativity rapid upward motion in the ice-laden air and subsequent dessication. Potential mechanisms for such a localized removal process are under investigation.

Space based inverse modeling of anthropogenic and natural emissions of nitrogen oxides over China: seasonal and interannual variability

NASA Astrophysics Data System (ADS)

Lin, J.-T.

2012-04-01

Nitrogen oxides (NOx ≡ NO + NO2) are important atmospheric constituents affecting the tropospheric chemistry and climate. They are emitted both from anthropogenic and from natural (soil, lightning, biomass burning, etc.) sources, and China has become a major region of increasing importance for anthropogenic sources. In a series of studies, satellite remote sensing for the vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) is used to estimate anthropogenic and natural emissions of NOx over China. Focus is set on variations of emissions over a variety of time scales in response to the economic development of China, from the general growth in recent years to the economic downturn during late 2008 - mid 2009 to the holiday associated with the Chinese New Year. An attempt is made to reduce the effect of potential systematic errors in satellite retrievals by coupling data from multiple satellite instruments flying over China at different time of day. For 2006, anthropogenic emissions are separated from lightning and soil sources over East China by exploiting their different seasonality. For the first time, a systematic evaluation is conducted to quantify uncertainties in various aspects of model meteorology and chemistry affecting emission inversion for China and implications for simulations of other air pollution (e.g., near-surface ozone).

A Hierarchical Modeling Study of the Interactions Among Turbulence, Cloud Microphysics, and Radiative Transfer in the Evolution of Cirrus Clouds

NASA Technical Reports Server (NTRS)

Curry, Judith; Khvorostyanov, V. I.

2005-01-01

This project used a hierarchy of cloud resolving models to address the following science issues of relevance to CRYSTAL-FACE: What ice crystal nucleation mechanisms are active in the different types of cirrus clouds in the Florida area and how do these different nucleation processes influence the evolution of the cloud system and the upper tropospheric humidity? How does the feedback between supersaturation and nucleation impact the evolution of the cloud? What is the relative importance of the large-scale vertical motion and the turbulent motions in the evolution of the crystal size spectra? How does the size spectra impact the life-cycle of the cloud, stratospheric dehydration, and cloud radiative forcing? What is the nature of the turbulence and waves in the upper troposphere generated by precipitating deep convective cloud systems? How do cirrus microphysical and optical properties vary with the small-scale dynamics? How do turbulence and waves in the upper troposphere influence the cross-tropopause mixing and stratospheric and upper tropospheric humidity? The models used in this study were: 2-D hydrostatic model with explicit microphysics that can account for 30 size bins for both the droplet and crystal size spectra. Notably, a new ice crystal nucleation scheme has been incorporated into the model. Parcel model with explicit microphysics, for developing and evaluating microphysical parameterizations. Single column model for testing bulk microphysics parameterizations

Poleward upgliding Siberian atmospheric rivers over sea ice heat up Arctic upper air.

PubMed

Komatsu, Kensuke K; Alexeev, Vladimir A; Repina, Irina A; Tachibana, Yoshihiro

2018-02-13

We carried out upper air measurements with radiosondes during the summer over the Arctic Ocean from an icebreaker moving poleward from an ice-free region, through the ice edge, and into a region of thick ice. Rapid warming of the Arctic is a significant environmental issue that occurs not only at the surface but also throughout the troposphere. In addition to the widely accepted mechanisms responsible for the increase of tropospheric warming during the summer over the Arctic, we showed a new potential contributing process to the increase, based on our direct observations and supporting numerical simulations and statistical analyses using a long-term reanalysis dataset. We refer to this new process as "Siberian Atmospheric Rivers (SARs)". Poleward upglides of SARs over cold air domes overlying sea ice provide the upper atmosphere with extra heat via condensation of water vapour. This heating drives increased buoyancy and further strengthens the ascent and heating of the mid-troposphere. This process requires the combination of SARs and sea ice as a land-ocean-atmosphere system, the implication being that large-scale heat and moisture transport from the lower latitudes can remotely amplify the warming of the Arctic troposphere in the summer.

Evaluation of Space-Based Constraints on Global Nitrogen Oxide Emissions with Regional Aircraft Measurements over and Downwind of Eastern North America

NASA Technical Reports Server (NTRS)

Martin, Randall V.; Sioris, Christopher E.; Chance, Kelly; Ryerson, Thomas B.; Flocke, Frank M.; Bertram, Timothy H.; Wooldridge, Paul J.; Cohen, Ronald C.; Neuman, J. Andy; Swanson, Aaron

2006-01-01

We retrieve tropospheric nitrogen dioxide (NO 2) columns for May 2004 to April 2005 from the SCIAMACHY satellite instrument to derive top-down emissions of nitrogen oxides (NO(x) = NO + NO2) via inverse modeling with a global chemical transport model (GEOS-Chem). Simulated NO 2 vertical profiles used in the retrieval are evaluated with airborne measurements over and downwind of North America (ICARTT); a northern midlatitude lightning source of 1.6 Tg N/yr minimizes bias in the retrieval. Retrieved NO2 columns are validated (r2 = 0.60, slope = 0.82) with coincident airborne in situ measurements. The top-down emissions are combined with a priori information from a bottom-up emission inventory with error weighting to achieve an improved a posteriori estimate of the global distribution of surface NOx emissions. Our a posteriori NOx emission inventory for land surface NOx emissions (46.1 Tg N/yr) is 22% larger than the GEIA-based a priori bottom-up inventory for 1998, a difference that reflects rising anthropogenic emissions, especially from East Asia A posteriori NOx emissions for East Asia (9.8 Tg N/yr) exceed those from other continents. The a posteriori inventory improves the GEOS-Chem simulation of NOx, peroxyacetylnitrate, and nitric acid with respect to airborne in situ measurements over and downwind of New York City. The a posteriori is 7% larger than the EDGAR 3.2FT2000 global inventory, 3% larger than the NEI99 inventory for the United States, and 68% larger than a regional inventory for 2000 for eastern Asia. SCIAMACHY NO2 columns over the North Atlantic show a weak plume from lightning NO(x).

Global O3-CO correlations in a chemistry and transport model during July-August: evaluation with TES satellite observations and sensitivity to input meteorological data and emissions

NASA Astrophysics Data System (ADS)

Choi, Hyun-Deok; Liu, Hongyu; Crawford, James H.; Considine, David B.; Allen, Dale J.; Duncan, Bryan N.; Horowitz, Larry W.; Rodriguez, Jose M.; Strahan, Susan E.; Zhang, Lin; Liu, Xiong; Damon, Megan R.; Steenrod, Stephen D.

2017-07-01

We examine the capability of the Global Modeling Initiative (GMI) chemistry and transport model to reproduce global mid-tropospheric (618 hPa) ozone-carbon monoxide (O3-CO) correlations determined by the measurements from the Tropospheric Emission Spectrometer (TES) aboard NASA's Aura satellite during boreal summer (July-August). The model is driven by three meteorological data sets (finite-volume General Circulation Model (fvGCM) with sea surface temperature for 1995, Goddard Earth Observing System Data Assimilation System Version 4 (GEOS-4 DAS) for 2005, and Modern-Era Retrospective Analysis for Research and Applications (MERRA) for 2005), allowing us to examine the sensitivity of model O3-CO correlations to input meteorological data. Model simulations of radionuclide tracers (222Rn, 210Pb, and 7Be) are used to illustrate the differences in transport-related processes among the meteorological data sets. Simulated O3 values are evaluated with climatological profiles from ozonesonde measurements and satellite tropospheric O3 columns. Despite the fact that the three simulations show significantly different global and regional distributions of O3 and CO concentrations, they show similar patterns of O3-CO correlations on a global scale. All model simulations sampled along the TES orbit track capture the observed positive O3-CO correlations in the Northern Hemisphere midlatitude continental outflow and the Southern Hemisphere subtropics. While all simulations show strong negative correlations over the Tibetan Plateau, northern Africa, the subtropical eastern North Pacific, and the Caribbean, TES O3 and CO concentrations at 618 hPa only show weak negative correlations over much narrower areas (i.e., the Tibetan Plateau and northern Africa). Discrepancies in regional O3-CO correlation patterns in the three simulations may be attributed to differences in convective transport, stratospheric influence, and subsidence, among other processes. To understand how various emissions drive global O3-CO correlation patterns, we examine the sensitivity of GMI/MERRA model-calculated O3 and CO concentrations and their correlations to emission types (fossil fuel, biomass burning, biogenic, and lightning NOx emissions). Fossil fuel and biomass burning emissions are mainly responsible for the strong positive O3-CO correlations over continental outflow regions in both hemispheres. Biogenic emissions have a relatively smaller impact on O3-CO correlations than other emissions but are largely responsible for the negative correlations over the tropical eastern Pacific, reflecting the fact that O3 is consumed and CO generated during the atmospheric oxidation process of isoprene under low-NOx conditions. We find that lightning NOx emissions degrade both positive correlations at mid- and high latitudes and negative correlations in the tropics because ozone production downwind of lightning NOx emissions is not directly related to the emission and transport of CO. Our study concludes that O3-CO correlations may be used effectively to constrain the sources of regional tropospheric O3 in global 3-D models, especially for those regions where convective transport of pollution plays an important role.

Space Shuttle ice nuclei

NASA Astrophysics Data System (ADS)

Turco, R. P.; Toon, O. B.; Whitten, R. C.; Cicerone, R. J.

1982-08-01

Estimates are made showing that, as a consequence of rocket activity in the earth's upper atmosphere in the Shuttle era, average ice nuclei concentrations in the upper atmosphere could increase by a factor of two, and that an aluminum dust layer weighing up to 1000 tons might eventually form in the lower atmosphere. The concentrations of Space Shuttle ice nuclei (SSIN) in the upper troposphere and lower stratosphere were estimated by taking into account the composition of the particles, the extent of surface poisoning, and the size of the particles. Calculated stratospheric size distributions at 20 km with Space Shuttle particulate injection, calculated SSIN concentrations at 10 and 20 km altitude corresponding to different water vapor/ice supersaturations, and predicted SSIN concentrations in the lower stratosphere and upper troposphere are shown.

The effects of deep convection on the concentration and size distribution of aerosol particles within the upper troposphere: A case study

NASA Astrophysics Data System (ADS)

Yin, Yan; Chen, Qian; Jin, Lianji; Chen, Baojun; Zhu, Shichao; Zhang, Xiaopei

2012-11-01

A cloud resolving model coupled with a spectral bin microphysical scheme was used to investigate the effects of deep convection on the concentration and size distribution of aerosol particles within the upper troposphere. A deep convective storm that occurred on 1 December, 2005 in Darwin, Australia was simulated, and was compared with available radar observations. The results showed that the radar echo of the storm in the developing stage was well reproduced by the model. Sensitivity tests for aerosol layers at different altitudes were conducted in order to understand how the concentration and size distribution of aerosol particles within the upper troposphere can be influenced by the vertical transport of aerosols as a result of deep convection. The results indicated that aerosols originating from the boundary layer can be more efficiently transported upward, as compared to those from the mid-troposphere, due to significantly increased vertical velocity through the reinforced homogeneous freezing of droplets. Precipitation increased when aerosol layers were lofted at different altitudes, except for the case where an aerosol layer appeared at 5.4-8.0 km, in which relatively more efficient heterogeneous ice nucleation and subsequent Wegener-Bergeron-Findeisen process resulted in more pronounced production of ice crystals, and prohibited the formation of graupel particles via accretion. Sensitivity tests revealed, at least for the cases considered, that the concentration of aerosol particles within the upper troposphere increased by a factor of 7.71, 5.36, and 5.16, respectively, when enhanced aerosol layers existed at 0-2.2 km, 2.2-5.4 km, and 5.4-8.0 km, with Aitken mode and a portion of accumulation mode (0.1-0.2μm) particles being the most susceptible to upward transport.

Initial studies of middle and upper tropospheric stratiform clouds

NASA Technical Reports Server (NTRS)

Cox, S. K.

1982-01-01

The spatial and temporal occurrence of cloud layers, the development of a physical-numerical model to simulate the life cycles of tropospheric cloud layers, and the design of an observational program to study the properties of these layers are described.

Hydroxyl and Hydroperoxy Radical Chemistry during the MCMA-2006 Field Campaign: Measurement and Model Comparison

NASA Astrophysics Data System (ADS)

Dusanter, S.; Vimal, D.; Stevens, P. S.; Volkamer, R.; Molina, L. T.

2007-12-01

The Mexico City Metropolitan Area (MCMA) field campaign, held in March 2006, was a unique opportunity to collect data in one of the most polluted megacities in the world. Such environments exhibit a complex oxidation chemistry involving a strong coupling between odd hydrogen radicals (HOX=OH+HO2) and nitrogen oxides species (NOX=NO+NO2). High levels of volatile organic compounds (VOCs) and NOX control the HOX budget and lead to elevated tropospheric ozone formation. The HOX-NOX coupling can be investigated by comparing measured and model-predicted HOx concentrations. Atmospheric HOX concentrations were measured by the Indiana University laser-induced fluorescence instrument and data were collected at the Instituto Mexicano del Petroleo between 14 and 31 March. Measured hydroxyl radical (OH) concentrations are comparable to that measured in less polluted urban environments and suggest that the OH concentrations are highly buffered under high NOX conditions. In contrast, hydroperoxy radical (HO2) concentrations are more sensitive to the NOX levels and are highly variable between different urban sites. Enhanced levels of OH and HO2 radicals were observed on several days between 9h30-11h00 AM and suggest an additional HOX source for the morning hours and/or a fast HOX cycling under the high NOX conditions of the MCMA. A preliminary investigation of the HOX chemistry occurring in the MCMA urban atmosphere was performed using a photochemical box model based on the Regional Atmospheric Chemistry Mechanism (RACM). Model comparisons will be presented and the agreement between measured and predicted HOX concentrations will be discussed.

Ships going slow in reducing their NOx emissions: changes in 2005-2012 ship exhaust inferred from satellite measurements over Europe

NASA Astrophysics Data System (ADS)

Folkert Boersma, K.; Vinken, Geert C. M.; Tournadre, Jean

2015-07-01

We address the lack of temporal information on ship emissions, and report on rapid short-term variations of satellite-derived ship NOx emissions between 2005 and 2012 over European seas. Our inversion is based on OMI observed tropospheric NO2 columns and GEOS-Chem simulations. Average European ship NOx emissions increased by ˜15% from 2005 to 2008. This increase was followed by a reduction of ˜12% in 2009, a direct result of the global economic downturn in 2008-2009, and steady emissions from 2009 to 2012. Observations of ship passages through the Suez Canal and satellite altimeter derived ship densities suggests that ships in the Mediterranean Sea have reduced their speed by more than 30% since 2008. This reduction in ship speed is accompanied by a persistent 45% reduction of average, per ship NOx emission factors. Our results indicate that the practice of ‘slow steaming’, i.e. the lowering of vessel speed to reduce fuel consumption, has indeed been implemented since 2008, and can be detected from space. In spite of the implementation of slow steaming, one in seven of all NOx molecules emitted in Europe in 2012 originated from the shipping sector, up from one in nine in 2005. The growing share of the shipping contributions to the overall European NOx emissions suggests a need for the shipping sector to implement additional measures to reduce pollutant emissions at rates that are achieved by the road transport and energy producing sectors in Europe.

Thermosphere Extension of the Whole Atmosphere Community Climate Model

DTIC Science & Technology

2010-12-04

tropospheric ozone and related tracers: Description and evaluation of MOZART, version 2, J. Geophys. Res., 108(D24), 4784, doi:10.1029/2002JD002853. Immel, T... troposphere to the upper thermosphere and their variability on interannual, seasonal, and daily scales. These quantities are compared with observational and...gravity waves are excited by tropospheric processes. As their amplitudes grow exponen- tially with altitude, they will cause larger variability

Effects of latent heat in various cloud microphysics processes on autumn rainstorms with different intensities on Hainan Island, China

NASA Astrophysics Data System (ADS)

Li, Jiangnan; Wu, Kailu; Li, Fangzhou; Chen, Youlong; Huang, Yanbin; Feng, YeRong

2017-06-01

In this study, we used the Weather Research and Forecasting (WRF) and WRF-3DVAR models to perform a series of simulations of two autumn rainstorms on Hainan Island. The results of neighborhood fractions and Hanssen skill scoring (FSS, HSS) methods show that the control experiments reproduced well two heavy rainfall episodes. Effects of latent heat in various cloud microphysical processes are different at distinct intensities or stages of precipitation. In the absence of any heating effect of deposition, precipitation weakened. The greater was the precipitation, the more significant was the weakening effect. Ascending movement at upper troposphere could be weakened or descending movement at lower troposphere enhanced. With decreases in the strength of precipitation, cloud ice, snow, graupel, and rainwater, increases in latent heat lessened. With weak precipitation, at upper troposphere the rainwater content increased and snow and ice content decreased, whereas at middle troposphere, the ice, snow, and graupel contents increased. Latent heating increased at middle and lower troposphere and decreased at upper troposphere. The absence of any heating effect of freezing had little effect on precipitation. By removing the evaporative cooling of cloud water, the interactions between vertical movement and cloud microphysical processes resulted in a weakening of strong precipitation and an intensification of weak precipitation. However, in the preliminary stages of these two precipitation events, snow, graupel, cloud ice, and rainwater all increased, and precipitation was enhanced in both. In the later stages, strong precipitation systems weakened and weak precipitation systems strengthened. Latent heating first increased and then dropped in strong precipitation systems, whereas they continuously increased in weak precipitation systems.

The Correlation Between Tropical Convection and Upper Tropospheric Momentum Flux Convergence

NASA Technical Reports Server (NTRS)

O'CStarr, David; Boehm, Matthew T.

2003-01-01

In this study, the relationship between tropical convection and the meridional convergence of zonal momentum flux in the tropical upper troposphere is investigated using NOAA interpolated outgoing longwave radiation data and NCEP-NCAR reanalysis wind data. In particular, a variety of correlation coefficients are calculated between the data sets, both of which are filtered to isolate disturbances with frequencies and wavenumbers consistent with the Madden-Julian oscillation. The results show regions of significant correlation during each season, with the magnitude and area covered by significant correlation coefficients varying with season. Furthermore, it is found that the correlation structures look very similar to theoretical calculations of the atmospheric response to a region of tropical heating. This result suggests that tropical waves, in particular mixed Rossby-gravity waves, play an important role in the meridional transport zonal momentum into the deep tropical upper troposphere. Finally, these findings have implications to the generation of rising motion near the tropical tropopause, which in turn has ramifications for vertical moisture transport and tropopause cirrus formation.

Modeling of tropospheric NO2 column over different climatic zones and land use/land cover types in South Asia

NASA Astrophysics Data System (ADS)

ul-Haq, Zia; Rana, Asim Daud; Tariq, Salman; Mahmood, Khalid; Ali, Muhammad; Bashir, Iqra

2018-03-01

We have applied regression analyses for the modeling of tropospheric NO2 (tropo-NO2) as the function of anthropogenic nitrogen oxides (NOx) emissions, aerosol optical depth (AOD), and some important meteorological parameters such as temperature (Temp), precipitation (Preci), relative humidity (RH), wind speed (WS), cloud fraction (CLF) and outgoing long-wave radiation (OLR) over different climatic zones and land use/land cover types in South Asia during October 2004-December 2015. Simple linear regression shows that, over South Asia, tropo-NO2 variability is significantly linked to AOD, WS, NOx, Preci and CLF. Also zone-5, consisting of tropical monsoon areas of eastern India and Myanmar, is the only study zone over which all the selected parameters show their influence on tropo-NO2 at statistical significance levels. In stepwise multiple linear modeling, tropo-NO2 column over landmass of South Asia, is significantly predicted by the combination of RH (standardized regression coefficient, β = - 49), AOD (β = 0.42) and NOx (β = 0.25). The leading predictors of tropo-NO2 columns over zones 1-5 are OLR, AOD, Temp, OLR, and RH respectively. Overall, as revealed by the higher correlation coefficients (r), the multiple regressions provide reasonable models for tropo-NO2 over South Asia (r = 0.82), zone-4 (r = 0.90) and zone-5 (r = 0.93). The lowest r (of 0.66) has been found for hot semi-arid region in northwestern Indus-Ganges Basin (zone-2). The highest value of β for urban area AOD (of 0.42) is observed for megacity Lahore, located in warm semi-arid zone-2 with large scale crop-residue burning, indicating strong influence of aerosols on the modeled tropo-NO2 column. A statistical significant correlation (r = 0.22) at the 0.05 level is found between tropo-NO2 and AOD over Lahore. Also NOx emissions appear as the highest contributor (β = 0.59) for modeled tropo-NO2 column over megacity Dhaka.

Monitoring the distribution of tropospheric ozone concentration over Pakistan by using OMI/MLS satellite observations

NASA Astrophysics Data System (ADS)

Noreen, Asma; Fahim Khokhar, Muhammad; Murtaza, Rabbia; Zeb, Naila

2016-07-01

Pakistan is a semi-arid, agricultural country located in Indian Sub-continent, Asia. Due to exponential population growth, poor control and regulatory measures and practices in industries, it is facing a major problem of air pollution. The concentration of greenhouse gases and aerosols are showing an increasing trend in general. One of these greenhouse gases is tropospheric ozone, one of the criteria pollutant, which has a radiative forcing (RF) of about 0.4 ± 0.2 Wm-2, contributing about 14% of the present total RF. Spatial distribution and temporal evolution of tropospheric ozone concentration over Pakistan during 2004 to 2014 was studied by using combined OMI/MLS product, which was derived by tropospheric ozone residual (TOR) method. Results showed an overall increase of 3.2 ± 2.2 DU in tropospheric ozone concentration over Pakistan since October 2004. The mean spatial distribution showed high concentrations of ozone in the Punjab and southern Sindh where there is high population densities along with rapid urbanization and enhanced anthropogenic activities. The seasonal variations were observed in the provinces of the country and TO3 VCDs were found to be high during summer while minimum during winter. The statistical analysis by using seasonal Mann Kendal test also showed strong positive trends over the four provinces as well as in major cities of Pakistan. These variations were driven by various factors such as seasonality in UV-B fluxes, seasonality in ozone precursor gases such as NOx and VOCs and agricultural fire activities in Pakistan. A strong correlation of 97% was found between fire events and tropospheric ozone concentration over the country. The results also depicted the influence of UV-B radiations on the tropospheric ozone concentration over different regions of Pakistan especially in Baluchistan and Sindh provinces.

Trends and sources of ozone and sub-micron aerosols at the Mt. Bachelor Observatory during 2004-2015

NASA Astrophysics Data System (ADS)

Zhang, L.; Jaffe, D. A.; Hee, J.

2016-12-01

Tropospheric ozone (O3) and airborne particles have significant impacts on human health and the environment. The Mt. Bachelor Observatory (MBO, 2.8 km a.s.l.) in Central Oregon, USA, now has one of the longest continuous free tropospheric records of O3, CO and aerosols in North America. In this study, we report on sources and trends of O3 and sub-micron aerosol scattering at MBO for 2004-2015. For O3, the seasonal cycle shows a bimodal pattern with peaks in April and July, while aerosol scattering (σsp) is lognormally distributed with a very high average in August and a smaller maximum in May. Mean O3 concentrations show a positive and significant trend in all seasons except winter, with an increase of approximately 0.6 ppb/year. This trend appears to be driven by Asian pollution in spring and regional wildfires in summer. For aerosol scattering, we see a significant increase only in summer, driven by recent increases in wildfire activity in the western US. Monthly criteria for isolating free troposphere (FT) and boundary layer (BL) air masses at MBO were obtained based on comparison of MBO water vapor (WV) distributions to those of Salem (SLE) and Medford (MFR), Oregon at equivalent pressure level. In all seasons, FT O3 is, on average, higher than BL O3, but the seasonal patterns are rather similar. For σsp the mean in summer is significantly higher than the FT, indicating the importance of regional wildfire smoke. We have identified four types of air masses that impact O3, CO and aerosols: Asian long range transport (ALRT), regional wildfires, regional industrial pollution, and upper troposphere and lower stratosphere (UTLS) intrusions. Over the 12 years of observations, we have identified 204 individual plume events based on the criteria of 8 consecutive polluted hours with elevated σsp, O3 or CO. Multi-pollutant correlations and backward trajectories were used to differentiate background source categories. A series of enhancement ratios (ERs) including Δσsp/ΔCO, Δσsp/ΔO3, Δσsp/ΔPAN, ΔO3/ΔCO, ΔPAN/ΔCO, ΔNOy/ΔCO, ΔO3/ΔH2O, ΔO3/ΔPAN and ΔNOx/ΔPAN and aerosol optical properties were calculated to characterize each category.

Variations of GHGs from the lower-troposphere to the UT/LS revealed by two Japanese regular aircraft observation programs

NASA Astrophysics Data System (ADS)

Niwa, Yosuke; Machida, Toshinobu; Sawa, Yousuke; Tsuboi, Kazuhiro; Matsueda, Hidekazu; Imasu, Ryoichi

2014-05-01

A Japan-centered observation network consisting of two regular aircraft programs have revealed the greenhouse gases variations from the lower-troposphere to the upper-troposphere/lower-stratosphere (UT/LS) regions. In the Comprehensive Observation Network for Trace gases by Airliner (CONTRAIL) project, in-situ continuous measurement equipment (CME) onboard commercial passenger aircraft world-widely observes CO2 profiles in vertical over tens of airports and in horizontal in the UT/LS regions. The CONTRAIL-CME has revealed three-dimensional structure of the global CO2 distribution and has exposed significant inter-hemispheric transport of CO2 through the upper-troposphere. In inverse modeling, the CME data have provided strong constraints on CO2 flux estimation especially for the Asian tropics. Automatic flask air sampling equipment (ASE) is also onboard the CONTRAIL aircraft and has been observing CO2 mixing ratios as well as those of methane, carbon monoxide, nitrous oxide and other trace species in the upper-troposphere between Japan and Australia. The observation period of the ASE has reached 20 years. In recent years, the ASE program has extended to the northern subarctic UT/LS region and has given an insight of transport mechanisms in the UT/LS by observing seasonal GHGs variations. In the other aircraft observation program by Japan Meteorological Agency, variations of GHGs have been observed by flask-sampling onboard a C-130H aircraft horizontally in the mid-troposphere over the western North Pacific as well as vertically over Minamitorishima-Island. The C-130H aircraft has persistently observed high mixing ratios of CH4 in the mid-troposphere, which seems to be originated from fossil fuel combustion throughout the year as well as from biogenic sources during summer in the Asian regions. Those above aircraft observation programs have a significant role for constraining GHGs flux estimates by filling the data gap of the existing surface measurement network specifically in the regions of Asia and the western North Pacific.

Comparisons of Upper Tropospheric Humidity Retrievals from TOVS and METEOSAT

NASA Technical Reports Server (NTRS)

Escoffier, C.; Bates, J.; Chedin, A.; Rossow, W. B.; Schmetz, J.

1999-01-01

Two different methods for retrieving Upper Tropospheric Humidities (UTH) from the TOVS (TIROS Operational Vertical Sounder) instruments aboard NOAA polar orbiting satellites are presented and compared. The first one, from the Environmental Technology Laboratory, computed by J. Bates and D. Jackson (hereafter BJ method), estimates UTH from a simplified radiative transfer analysis of the upper tropospheric infrared water vapor channel at wavelength measured by HIRS (6.3 micrometer). The second one results from a neural network analysis of the TOVS (HIRS and MSU) data developed at, the Laboratoire de Meteorologie Dynamique (hereafter the 3I (Improved Initialization Inversion) method). Although the two methods give very similar retrievals in temperate regions (30-60 N and S), an absolute bias up to 16% appears in the convective zone of the tropics. The two datasets have also been compared with UTH retrievals from infrared radiance measurements in the 6.3 micrometer channel from the geostationary satellite METEOSAT (hereafter MET method). The METEOSAT retrievals are systematically drier than the TOVS-based results by an absolute bias between 5 and 25%. Despite the biases, the spatial and temporal correlations are very good. The purpose of this study is to explain the deviations observed between the three datasets. The sensitivity of UTH to air temperature and humidity profiles is analysed as are the clouds effects. Overall, the comparison of the three retrievals gives an assessment of the current uncertainties in water vapor amounts in the upper troposphere as determined from NOAA and METEOSAT satellites.

A Study of Cirrus Clouds and Aerosols in the Upper Troposphere using Models and Satellite Data

NASA Technical Reports Server (NTRS)

Bergstrom, Robert W.

2004-01-01

This report is the final report for the Cooperative Agreement NCC2-1213. It is a compilation of publications produced under this Cooperative Agreement and conference presentations. The tasks for the Aerosol Physical Chemistry Model for the Upper Troposphere include: Task 1: To compare APCM predictions against the SUCCESS data and other aircraft campaigns and to investigate the role of aerosol composition on cirrus cloud nucleation; Task 2: To study the seasonal evolution and spatial distribution of upper-tropospheric tropical and polar cirrus; Task 3: To investigate CLAES cirrus data with other complementary (TOGA-COARE and CEPEX) data. Tasks for Upper Tropospheric Cirrus Clouds include: Task 1: Assemble 3-hourly (or more frequent) meteorological satellite data fiom geostationary satellites to obtain a global, or nearly global, dataset of infiared brightness temperatures as a function of time for airborne experimental periods; Task 2: Explore methods to improve the cloud top altitude distributions calculated fiom meteorological satellite data. This will focus on linlung the 6.5 micron channel geostationary brightness temperatures and the 10.5 micron brightness temperatures; Task 3: Explore methods to differentiate convective fiom stratiform cloudiness; Task 4: Perform trajectory analyses using an existing trajectory modeling package that links the cloud data with air mass histories; Task 5: Apply techniques from tasks 1 through 4 to provide meteorological support to the CRYSTAL-FACE mission, both in its preparation and deployment phases. The report include four published articles and two slide presentations.

Modeling the effects of UV variability and the QBO on the troposphere-stratosphere system. Part II: The troposphere

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rind, D.; Balachandran, N.K.

1995-08-01

Results of experiments with a GCM involving changes in UV input ({plus_minus} 25%, {plus_minus}5% at wavelengths below 0.3 {mu}) and simulated equatorial QBO are presented, with emphasis on the tropospheric response. The QBO and UV changes alter the temperature in the lower stratosphere/upper troposphere warms, tropospheric eddy energy is reduced, leading to extratropical tropospheric cooling of some 0.5{degrees}C on the zonal average, and surface temperature changes up to {plus_minus}5{degrees}C locally. Opposite effects occur when the extratropical lower stratosphere/upper troposphere cools. Cooling or warming of the comparable region in the Tropics decreases/increases static stability, accelerating/decelerating the Hadley circulation. Tropospheric dynamical changesmore » are on the order of 5%. The combined UV/QBO effect in the troposphere results from its impact on the middle atmosphere; in the QBO east phase, more energy is refracted to higher latitudes, due to the increased horizontal shear of the zonal wind, but with increased UV, this energy propagates preferentially out of the polar lower stratosphere, in response to the increased vertical shear of the zonal winds; therefore, it is less effective in warming the polar lower stratosphere. Due to their impacts on planetary wave generation and propagation, all combinations of UV and QBO phases affect the longitudinal patterns of tropospheric temperatures and geopotential heights. The modeled perturbations often agree qualitatively with observations and are of generally similar orders of magnitude. The results are sensitive to the forcing employed. In particular, the nature of the tropospheric response depends upon the magnitude (and presumably wavelength) of the solar irradiance perturbation. The results of the smaller UV variations ({plus_minus}5%) are more in agreement with observations, showing clear differences between the UV impact in the east and west QBO phase. 34 refs., 15 figs., 3 tabs.« less

Hydrogen Cyanide in the Upper Troposphere: GEM-AQ Simulation and Comparison with ACE-FTS Observations

NASA Technical Reports Server (NTRS)

Lupu, A.; Kaminski, J. W.; Neary, L.; McConnell, J. C.; Toyota, K.; Rinsland, C. P.; Bernath, P. F.; Walker, K. A.; Boone, C. D.; Nagahama, Y.;

Influence of isentropic transport on seasonal ozone variations in the lower stratosphere and subtropical upper troposphere

NASA Technical Reports Server (NTRS)

Jing, P.; Cunnold, D. M.; Yang, E.-S.; Wang, H.-J.

2005-01-01

The isentropic cross-tropopause ozone transport has been estimated in both hemispheres in 1999 based on the potential vorticity mapping of Stratospheric Aerosol and Gas Experiment 11 ozone measurements and contour advection calculations using the NASA Goddard Space Flight Center Global and Modeling Assimilation Office analysis. The estimated net isentropic stratosphere-to-troposphere ozone flux is approx.118 +/- 61 x 10(exp9)kg/yr globally within the layer between 330 and 370 K in 1999; 60% of it is found in the Northern Hemisphere, and 40% is found in the Southern Hemisphere. The monthly average ozone fluxes are strongest in summer and weakest in winter in both hemispheres. The seasonal variations of ozone in the lower stratosphere (LS) and upper troposphere (UT) have been analyzed using ozonesonde observations from ozonesonde stations in the extratropics and subtropics, respectively. It is shown that observed ozone levels increase in the UT over subtropical ozonesonde stations and decrease in the LS over extratropical stations in late spring/early summer and that the ozone increases in the summertime subtropical UT are unlikely to be explained by photochemical ozone production and diabatic transport alone. We conclude that isentropic transport is a significant contributor to ozone levels in the subtropical upper troposphere, especially in summer.

Regional Impact on Pollution Event in the Upper Troposphere during CARIBIC Flights between South China and the Philippines

NASA Astrophysics Data System (ADS)

Lai, S. C.; Baker, A. R.; Schuck, T. J.; van Velthoven, P.; Oram, D. E.; Zahn, A.; Hermann, M.; Weigelt, A.; Slemr, S.; Brenninkmeijer, C. A. M.

2010-05-01

The research project CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrumented Container, phase II) is designed to conduct regular, long-term and detailed observations of the free troposphere and UT/LS regions where passenger aircraft happen to cruise. A fully-automated measurement container (1.5 tons) was equipped onboard an Airbus 340-600 operated by Lufthansa Airlines during regular passenger flights to conduct real time trace gas and aerosol measurements and to collect aerosol and air samples on a near monthly basis. During May 2005 - March 2008, CARIBIC observations have been performed along the flight tracks of Frankfurt-Guangzhou-Manila. Data have been collected in the upper troposphere during a total of 81 flights over the region between South China and the Philippines. Carbon monoxide was used an indicator to identify the pollution events and to access the regional impacts of fossil fuel burning and biomass/biofuel burning on upper tropospheric air. Five regions, i.e. Northeast Asia, South China, Indochina Peninsula, India and Indonesia/Philippines, are identified as the major source regions to be related to the observed pollution events. The characteristics of the events from these regions are investigated. The contributions of different source categories are also estimated.

The Influence of Ozone Precursor Emissions from Four World Regions on Tropospheric Composition and Radiative Climate Forcing

NASA Technical Reports Server (NTRS)

Fry, Meridith; Naik, Vaishali; West, J. Jason; Schwarzkopf, M. Daniel; Fiore, Arlene M.; Collins, William J.; Dentener, Frank J.; Shindell, Drew T.; Atherton, Cyndi; Bergmann, Daniel;

Quantifying Sulfate, Organics, and Lubrication Oil in Particles Emitted from Military Aircraft Engines

DTIC Science & Technology

2012-10-01

Measurements. Part 1: Theory. Aerosol Sci. Tech., 38, 1185-1205 Finlayson-Pitts, B. J. and Pitts, J. N. 1997. Tropospheric air pollution: Ozone ...2004). Wetting and Hydration of Insoluble Soot Particles in the Upper Troposphere . J. Environ. Monitoring, 6:939-945. Petzold, A., Gysel, M...nanoparticles: role of ambient ionization in tropospheric aerosol formation. Journal of Geophysical Research, 106(5): 4797–4814. Yu, F. (2005). Quasi

Dispersion and photochemical evolution of reactive pollutants in street canyons

NASA Astrophysics Data System (ADS)

Kwak, Kyung-Hwan; Baik, Jong-Jin; Lee, Kwang-Yeon

2013-05-01

Dispersion and photochemical evolution of reactive pollutants in street canyons with canyon aspect ratios of 1 and 2 are investigated using a computational fluid dynamics (CFD) model coupled with the carbon bond mechanism IV (CBM-IV). Photochemical ages of NOx and VOC are expressed as a function of the NO2-to-NOx and toluene-to-xylene ratios, respectively. These are found to be useful for analyzing the O3 and OH oxidation processes in the street canyons. The OH oxidation process (O3 oxidation process) is more pronounced in the upper (lower) region of the street canyon with a canyon aspect ratio of 2, which is characterized by more (less) aged air. In the upper region of the street canyon, O3 is chemically produced as well as transported downward across the roof level, whereas O3 is chemically reduced in the lower region of the street canyon. The O3 chemical production is generally favorable when the normalized photochemical ages of NOx and VOC are larger than 0.55 and 0.28, respectively. The sensitivities of O3 chemical characteristics to NOx and VOC emission rates, photolysis rate, and ambient wind speed are examined for the lower and upper regions of the street canyon with a canyon aspect ratio of 2. The O3 concentration and the O3 chemical production rate divided by the O3 concentration increase as the NOx emission rate decreases and the VOC emission rate and photolysis rate increase. The O3 concentration is less sensitive to the ambient wind speed than to other factors considered. The relative importance of the OH oxidation process compared to the O3 oxidation process increases with increasing NOx emission rate and photolysis rate and decreasing VOC emission rate. In this study, both O3 and OH oxidation processes are found to be important in street-canyon scale chemistry. The methodology of estimating the photochemical ages can potentially be adopted to neighborhood scale chemistry.

Sensitivity of Tropospheric Chemical Composition to Halogen-Radical Chemistry Using a Fully Coupled Size-Resolved Multiphase Chemistry-Global Climate System: Halogen Distributions, Aerosol Composition, and Sensitivity of Climate-Relevant Gases

DOE Office of Scientific and Technical Information (OSTI.GOV)

Long, M.; Keene, W. C.; Easter, Richard C.

Observations and model studies suggest a significant but highly non-linear role for halogens, primarily Cl and Br, in multiphase atmospheric processes relevant to tropospheric chemistry and composition, aerosol evolution, radiative transfer, weather, and climate. The sensitivity of global atmospheric chemistry to the production of marine aerosol and the associated activation and cycling of inorganic Cl and Br was tested using a size-resolved multiphase coupled chemistry/global climate model (National Center for Atmospheric Research’s Community Atmosphere Model (CAM); v3.6.33). Simulation results showed strong meridional and vertical gradients in Cl and Br species. The simulation reproduced most available observations with reasonable confidence permittingmore » the formulation of potential mechanisms for several previously unexplained halogen phenomena including the enrichment of Br- in submicron aerosol, and the presence of a BrO maximum in the polar free troposphere. However, simulated total volatile Br mixing ratios were generally high in the troposphere. Br in the stratosphere was lower than observed due to the lack of long-lived organobromine species in the simulation. Comparing simulations using chemical mechanisms with and without reactive Cl and Br species demonstrated a significant temporal and spatial sensitivity of primary atmospheric oxidants (O3, HOx, NOx), CH4, and non-methane hydrocarbons (NMHC’s) to halogen cycling. Simulated O3 and NOx were globally lower (65% and 35%, respectively, less in the planetary boundary layer based on median values) in simulations that included halogens. Globally, little impact was seen in SO2 and non-sea-salt SO42- processing due to halogens. Significant regional differences were evident: The lifetime of nss-SO42- was extended downwind of large sources of SO2. The burden and lifetime of DMS (and its oxidation products) were lower by a factor of 5 in simulations that included halogens, versus those without, leading to a 20% reduction in nss-SO42- in the southern hemisphere planetary boundary layer based on median values.« less

Variability of Upper-Tropospheric Precipitable from Satellite and Model Reanalysis Datasets

NASA Technical Reports Server (NTRS)

Jedlovec, Gary J.; Iwai, Hisaki

1999-01-01

Numerous datasets have been used to quantify water vapor and its variability in the upper-troposphere from satellite and model reanalysis data. These investigations have shown some usefulness in monitoring seasonal and inter-annual variations in moisture either globally, with polar orbiting satellite data or global model output analysis, or regionally, with the higher spatial and temporal resolution geostationary measurements. The datasets are not without limitations, however, due to coverage or limited temporal sampling, and may also contain bias in their representation of moisture processes. The research presented in this conference paper inter-compares the NVAP, NCEP/NCAR and DAO reanalysis models, and GOES satellite measurements of upper-tropospheric,precipitable water for the period from 1988-1994. This period captures several dramatic swings in climate events associated with ENSO events. The data are evaluated for temporal and spatial continuity, inter-compared to assess reliability and potential bias, and analyzed in light of expected trends due to changes in precipitation and synoptic-scale weather features. This work is the follow-on to previous research which evaluated total precipitable water over the same period. The relationship between total and upper-level precipitable water in the datasets will be discussed as well.

Introducing and Validating the New Aura CO Product Derived from Joined TES and MLS Measurements

NASA Astrophysics Data System (ADS)

Luo, M.; Schwartz, M. J.; Read, W. G.; Herman, R. L.; Kulawik, S. S.; Worden, J.; Livesey, N. J.; Bowman, K. W.; Sweeney, C.

2014-12-01

The new Aura CO product consists of CO vertical profiles derived from TES and MLS measurements. This product has been released to the public. We describe the algorithms for generating the product and the evaluations of it using in-situ measurements. TES and MLS standalone CO profile retrievals are sensitive respectively to lower-mid troposphere and upper troposphere and above. We pair TES nadir and MLS limb tangent locations within 6-8 min and less than 220 km. The paired radiance measurements of the two instruments per location are optimally combined to retrieve a single CO profile along with other interfering species. This combined CO profile has improved vertical resolution and vertical range over the two standalone products, especially in the upper-troposphere/lower-stratosphere. For example, the degree of freedom for signal (DOFS) between surface and 50hPa for TES alone is < 2, and for the combined CO profiles is 2-4. We will present the comparison results between the Aura CO and AirCore, HIPPO, and MOZAIC observations. The new Aura CO product provides a unique data set to studies on tropospheric transport of air pollutants and troposphere-stratospheric exchange processes.

Investigation of Dynamic and Physical Processes in the Upper Troposphere and Lower Stratosphere

NASA Technical Reports Server (NTRS)

Selkirk, Henry B.; Pfister, Leonhard (Technical Monitor)

2002-01-01

Research under this Cooperative Agreement has been funded by several NASA Earth Science programs: the Atmospheric Effects of Radiation Program (AEAP), the Upper Atmospheric Research Program (UARP), and most recently the Atmospheric Chemistry and Modeling Assessment Program (ACMAP). The purpose of the AEAP was to understand the impact of the present and future fleets of conventional jet traffic on the upper troposphere and lower stratosphere, while complementary airborne observations under UARP seek to understand the complex interactions of dynamical and chemical processes that affect the ozone layer. The ACMAP is a more general program of modeling and data analysis in the general area of atmospheric chemistry and dynamics, and the Radiation Sciences program.

Atmospheric mercury speciation dynamics at the high-altitude Pic du Midi Observatory, southern France

NASA Astrophysics Data System (ADS)

Fu, Xuewu; Marusczak, Nicolas; Heimbürger, Lars-Eric; Sauvage, Bastien; Gheusi, François; Prestbo, Eric M.; Sonke, Jeroen E.

2016-05-01

Continuous measurements of atmospheric gaseous elemental mercury (GEM), particulate bound mercury (PBM) and gaseous oxidized mercury (GOM) at the high-altitude Pic du Midi Observatory (PDM Observatory, 2877 m a.s.l.) in southern France were made from November 2011 to November 2012. The mean GEM, PBM and GOM concentrations were 1.86 ng m-3, 14 pg m-3 and 27 pg m-3, respectively and we observed 44 high PBM (peak PBM values of 33-98 pg m-3) and 61 high GOM (peak GOM values of 91-295 pg m-3) events. The high PBM events occurred mainly in cold seasons (winter and spring) whereas high GOM events were mainly observed in the warm seasons (summer and autumn). In cold seasons the maximum air mass residence times (ARTs) associated with high PBM events were observed in the upper troposphere over North America. The ratios of high PBM ARTs to total ARTs over North America, Europe, the Arctic region and Atlantic Ocean were all elevated in the cold season compared to the warm season, indicating that the middle and upper free troposphere of the Northern Hemisphere may be more enriched in PBM in cold seasons. PBM concentrations and PBM / GOM ratios during the high PBM events were significantly anti-correlated with atmospheric aerosol concentrations, air temperature and solar radiation, suggesting in situ formation of PBM in the middle and upper troposphere. We identified two distinct types of high GOM events with the GOM concentrations positively and negatively correlated with atmospheric ozone concentrations, respectively. High GOM events positively correlated with ozone were mainly related to air masses from the upper troposphere over the Arctic region and middle troposphere over the temperate North Atlantic Ocean, whereas high GOM events anti-correlated with ozone were mainly related to air masses from the lower free troposphere over the subtropical North Atlantic Ocean. The ARTs analysis demonstrates that the lower and middle free troposphere over the North Atlantic Ocean was the largest source region of atmospheric GOM at the PDM Observatory. The ratios of high GOM ARTs to total ARTs over the subtropical North Atlantic Ocean in summer were significantly higher than those over the temperate and sub-arctic North Atlantic Ocean as well as that over the North Atlantic Ocean in other seasons, indicating abundant in situ oxidation of GEM to GOM in the lower free troposphere over the subtropical North Atlantic Ocean in summer.

Planning, Implementation, and Scientific Goals of the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) Field Missions

NASA Technical Reports Server (NTRS)

Toon, Owen B.; Maring, Hal; Dibb, Jack; Ferrare, Richard A.; Jacob, Daniel J.; Jensen, Eric J.; Luo, Z. Johnny; Mace, Gerald G.; Pan, Laura L.; Pfister, Leonhard;

Lagrangian Photochemical Box-Model Calculations of Asian Pacific Rim Outflow During TRACE-P

NASA Astrophysics Data System (ADS)

Hamlin, A.; Crawford, J.; Olson, J.; Avery, M.; Sachse, G.; Barrick, J.; Blake, D.; Tan, D.; Sandholm, S.; Kondo, Y.; Singh, H.; Eisele, F.; Zondlo, M.; Flocke, F.; Talbot, R.

2006-12-01

NASA's TRACE-P (TRAnsport and Chemical Evolution over the Pacific) mission was conducted over the northwestern Pacific February-April, 2001. During two transit flights across the Pacific, extensive pollution was observed from an Asian outflow event that split into two branches over the central Pacific, one subsiding and moving southward over the central Pacific and the other continuing eastward in the upper troposphere. The subsiding branch was observed as a widespread stagnant pollution layer between 2 and 4 km over the central Pacific during transit flights from Kona, HI to Guam. In this region, high levels of O3 (70 ppbv), CO (217 ppbv), and NOx (114 pptv) were well in excess of typical values observed during TRACE-P along the Asian coast. Evidence suggests that the subsiding branch experienced extensive photochemical processing compared to the branch that remained at altitude. To examine the processes controlling the chemical evolution of ozone and its precursors in this outflow event, data collected during the TRACE-P mission have been combined with lagrangian photochemical box model calculations. One of the largest sources of uncertainty in these calculations was associated with predicted water vapor levels along the transport trajectories calculated using the HYSPLIT model. Water vapor levels predicted by HYSPLIT trajectory calculations in the subsiding layer ranged from 3390 to 4880 ppm, while the median level observed in the pollution layer was only 637 ppm. Simulations of ozone production and associated radical chemistry differed dramatically when using water vapor levels based on trajectory calculations versus observed water vapor levels. Levels of PAN and HO2NO2, NOx reservoir species, are also influenced by uncertainties in temperature along the trajectories. These results highlight the importance of accurately representing the humidification and warming of subsiding air masses in 3-D chemical- transport models.

Characterization of Emissions and Air Quality Modeling for Predicting the Impacts of Prescribed Burns at DoD Lands

DTIC Science & Technology

2012-10-01

Sum of NOx and its oxidation products NOAA National Oceanic and Atmospheric Administration O3 Ozone OAQPS Office of Air Quality Planning and...Emission related parameters such as emission strength, timing, and vertical distribution (plume fraction penetrating into the free troposphere ) proved to...emissions and the effect of PB on ozone levels in Columbus-Phenix City metropolitan areas are also of concern. Forest fires produce nitrogen oxides

Direct Measurements of the Convective Recycling of the Upper Troposphere

NASA Technical Reports Server (NTRS)

Bertram, Timothy H.; Perring, Anne E.; Wooldridge, Paul J.; Crounse, John D.; Kwan, Alan J.; Wennberg, Paul O.; Scheuer, Eric; Dibb, Jack; Avery, Melody; Sachse, Glen;

Nitric Acid Uptake and Decomposition on Black Carbon (Soot) Surfaces: Its Implications for the Upper Troposphere and Lower Stratosphere

NASA Technical Reports Server (NTRS)

Choi, W.; Leu, M. T.

1998-01-01

Black carbon particles (soot) are formed as a result of incomplete combustion processes and are ubiquitous in the atmosphere. The lower troposphere contains plenty of soot particles whose principal sources are fossil fuel and biomass combustion at the ground level.

Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) Observations of Polar Winter Conditions in 2009; Comparisons with Years 2002-2008

DTIC Science & Technology

2011-02-03

focused upon the tropospheric forcing, for example the role of blocking systems (large-scale, quasi-stationary, high-pressure systems that may steer...disruptions of the stratosphere may in turn perturb the troposphere and even affect surface weather. In early February 2009, London received heavy snowfall...global measurements from twelve SSW periods, found cooling in the equatorial lower stratosphere and upper troposphere that is associated with increased

Understanding Wave-mean Flow Feedbacks and Tropospheric Annular Variability

NASA Astrophysics Data System (ADS)

Lorenz, D. J.

2016-12-01

The structure of internal tropospheric variability is important for determining the impact of the stratosphere on the troposphere. This study aims to better understand the fundamental dynamical mechanisms that control the feedbacks between the eddies and the mean flow, which in turn select the tropospheric annular mode. Recent work using Rossby Wave Chromatography suggests that "barotropic processes", which directly impact the meridional propagation of wave activity (specifically the reflectivity of the poleward flank of the mid-latitude jet), are more important for the positive feedback between the annular mode and the eddies than "baroclinic processes", which involve changes in the generation of wave activity by baroclinic instability. In this study, experiments with a fully nonlinear quasi-geostrophic model are discussed which provide independent confirmation of the importance of barotropic versus baroclinic processes. The experiments take advantage of the steady-state balance at upper-levels between the meridional gradient in diabatic heating and the second derivative of the upper-level EP flux divergence. Simulations with standard Newtonian heating are compared to simulations with constant-in-time heating taken from the climatology of the standard run and it is found that the forced annular mode response to changes in surface friction is very similar. Moreover, as expected from the annular mode response, the eddy momentum fluxes are also very similar. This is despite the fact that the upper-level EP flux divergence is very different between the two simulations (upper-level EP flux divergence must remain constant in the constant heating simulation while in the standard simulation there is no such constraint). The upper-level balances are maintained by a large change in the baroclinic wave source (i.e. vertical EP flux), which is accompanied by little momentum flux change. Therefore the eddy momentum fluxes appear to be relatively insensitive to the wave activity source. A more detailed comparison suggests a helpful rule-of-thumb relating the amplitude of the baroclinic wave source to the upper-level vorticity flux forced by this wave source.

Biomass burning influences on ozone during the SAMBBA aircraft campaign.

NASA Astrophysics Data System (ADS)

Keslake, Tim; Chiperfield, Martyn; Mann, Graham; Flemming, Johannes; Morgan, Will; Darbyshire, Eoghan; Remy, Sam; Dhomse, Sandip; Pope, Richard; Reddington, Carly

2017-04-01

Ozone (O3) is an air pollutant and a greenhouse gas. It is detrimental to human and plant health, damaging plant stomata and therefore limiting photosynthesis. O3 is both formed and lost via the interconversion between nitric oxide (NO) and nitrogen dioxide (NO2); the relative amount of O3 produced depends on the amount of NOx (NO + NO2) and volatile organic compounds (VOCs), which indirectly compete with O3 to oxidise NO back into NO2, leading to more O3. The Amazon region has some of the lowest background O3 levels on the planet (˜20 ppb) and is a NOx-limited environment for ozone production. During the tropical dry season emissions of NOx and VOCs from both tropical and savannah fires lead to a large increase in O3mixing ratios over the Amazon. With a predicted increase in non-agricultural fire activities, due to a changing climate it is important to understand how much O3is being formed in the Amazon and the sensitivity of this to fire and other emissions. The amount of O3 is potentially of additional importance as the Amazon forest is the largest single land carbon sink on the planet, with an estimated net annual sink of 2.4 pG C yr-1, which could be limited by O3 plant damage. Despite this, detailed observation of O3and its precursors in the Amazon have been limited. However, the SAMBBA field campaign (September- October 2012) provides an opportunity to observe in-situ O3formation. The ECMWF C-IFS (Composition Integrated Forecast System) developed under MACC and continued under CAMS, provides global operational forecasts and re-analyses of atmospheric composition at high spatial resolution (T255, ˜80km). In this study, we present results from C-IFS experiments for the SAMBBA period, with and without composition data assimilation, exploring how well the C-IFS represents biomass burning influences on O3in the Amazon. The aim is to test our understanding of O3formation and precursor emissions as well as the capability of the C-IFS for air quality forecasts. The flight campaign showed average O3 values of 43 ppb, over tropical vegetation in the dry season with larger values observed in the upper troposphere during the wet season (61ppb). The largest surface O3values were observed over the eastern savannah region (75 ppb), where NOx emissions were most significant. Comparisons to the C-IFS show that the model persistently underestimated O3value compared to the in-situ observations (MFB -39%). The bias is thought to be caused by an underestimation of both fire and lightning NOx emissions in the model. When NOx emissions are improved by assimilation of OMI satellite NO2 data in the Eastern region, O3values show a smaller overestimation compared to the observations (MFB 4%).

Injection of Lightning-Produced NOx, Water Vapor, Wildfire Emissions, and Stratospheric Air to the UT/LS as Observed from DC3 Measurements

NASA Astrophysics Data System (ADS)

Huntrieser, H.; Lichtenstern, M.; Scheibe, M.; Aufmhoff, H.; Schlager, H.; Minikin, A.; Weinzierl, B.; Pollack, I. B.; Peischl, J.; Ryerson, T. B.; Weinheimer, A. J.; Honomichl, S.; Ridley, B. A.; Hair, J. W.; Schwartz, M. J.; Rappenglück, B.; Pickering, K. E.; Cummings, K.; Biggerstaff, M. I.; Heimerl, K.; Pucik, T.; Fütterer, D.; Ackermann, L.; Betten, D.; Butler, C. F.; Barth, M. C.

2015-12-01

In summer 2012 the Deep Convective Clouds and Chemistry Project (DC3) field campaign investigated a number of severe thunderstorms over the Central U.S. and their impact on the upper tropospheric (UT) - lower stratospheric (LS) composition and chemistry. In addition, during DC3 some of the largest and most destructive wildfires in New Mexico and Colorado state history were burning, influencing the air quality in the DC3 thunderstorm inflow and outflow region. Besides three instrumented aircraft platforms measuring a variety of trace species in-situ and remotely (e.g. CO, O3, SO2, NOx, VOC, CN, and black carbon), dense networks of ground-based instruments (e.g. radar and lightning) complemented the airborne measurements. Satellite measurements (e.g. GOES, MODIS, and GOME-2) and model forecasts (e.g. WRF-Chem and FLEXPART) were used to monitor the rapid development of the thunderstorms (which frequently developed huge anvils with overshooting tops) and the spread of smoke plumes in the vicinity of the storms. In-situ probing of fresh and aged (12-24 h) anvil outflows showed injection of lightning-produced NOx and wildfire emissions into the UTLS. Vertical cross sections of lidar and Doppler radar measurements supported these observations and gave detailed information on dynamical processes within and in the vicinity of the storms. Besides very strong updrafts in the storm core, surrounding downdrafts caused a direct in-mixing of O3-rich LS air masses into the boundaries of the anvil outflow. The wrapping of O3-rich LS air masses around and below the anvil outflow was also a prominent feature in several storms. The in-situ probing of the aged anvil outflow showed a pronounced influence on the UT composition and chemistry with average O3 enhancements in the range of 20-50 nmol mol-1 and evidence of new particle formation. A 10-year global climatology of H2O data from Aura-MLS confirms that the Central U.S. is a preferred region for convective injection into the LS.

Injection of Lightning-Produced NOx, Water Vapor, Wildfire Emissions, and Stratospheric Air to the UT/LS as Observed from DC3 Measurements

NASA Astrophysics Data System (ADS)

Huntrieser, H.; Lichtenstern, M.; Scheibe, M.; Aufmhoff, H.; Schlager, H.; Minikin, A.; Weinzierl, B.; Pollack, I. B.; Peischl, J.; Ryerson, T. B.; Weinheimer, A. J.; Honomichl, S.; Ridley, B. A.; Hair, J. W.; Schwartz, M. J.; Rappenglück, B.; Pickering, K. E.; Cummings, K.; Biggerstaff, M. I.; Heimerl, K.; Pucik, T.; Fütterer, D.; Ackermann, L.; Betten, D.; Butler, C. F.; Barth, M. C.

2014-12-01

In summer 2012 the Deep Convective Clouds and Chemistry Project (DC3) field campaign investigated a number of severe thunderstorms over the Central U.S. and their impact on the upper tropospheric (UT) - lower stratospheric (LS) composition and chemistry. In addition, during DC3 some of the largest and most destructive wildfires in New Mexico and Colorado state history were burning, influencing the air quality in the DC3 thunderstorm inflow and outflow region. Besides three instrumented aircraft platforms measuring a variety of trace species in-situ and remotely (e.g. CO, O3, SO2, NOx, VOC, CN, and black carbon), dense networks of ground-based instruments (e.g. radar and lightning) complemented the airborne measurements. Satellite measurements (e.g. GOES, MODIS, and GOME-2) and model forecasts (e.g. WRF-Chem and FLEXPART) were used to monitor the rapid development of the thunderstorms (which frequently developed huge anvils with overshooting tops) and the spread of smoke plumes in the vicinity of the storms. In-situ probing of fresh and aged (12-24 h) anvil outflows showed injection of lightning-produced NOx and wildfire emissions into the UTLS. Vertical cross sections of lidar and Doppler radar measurements supported these observations and gave detailed information on dynamical processes within and in the vicinity of the storms. Besides very strong updrafts in the storm core, surrounding downdrafts caused a direct in-mixing of O3-rich LS air masses into the boundaries of the anvil outflow. The wrapping of O3-rich LS air masses around and below the anvil outflow was also a prominent feature in several storms. The in-situ probing of the aged anvil outflow showed a pronounced influence on the UT composition and chemistry with average O3 enhancements in the range of 20-50 nmol mol-1 and evidence of new particle formation. A 10-year global climatology of H2O data from Aura-MLS confirms that the Central U.S. is a preferred region for convective injection into the LS.

Atmospheric Hydroxyl Radical Production from Electronically Excited NO2 and H2O

NASA Astrophysics Data System (ADS)

Li, Shuping; Matthews, Jamie; Sinha, Amitabha

2008-03-01

Hydroxyl radicals are often called the “detergent” of the atmosphere because they control the atmosphere’s capacity to cleanse itself of pollutants. Here, we show that the reaction of electronically excited nitrogen dioxide with water can be an important source of tropospheric hydroxyl radicals. Using measured rate data, along with available solar flux and atmospheric mixing ratios, we demonstrate that the tropospheric hydroxyl contribution from this source can be a substantial fraction (50%) of that from the traditional O(1D) + H2O reaction in the boundary-layer region for high solar zenith angles. Inclusion of this chemistry is expected to affect modeling of urban air quality, where the interactions of sunlight with emitted NOx species, volatile organic compounds, and hydroxyl radicals are central in determining the rate of ozone formation.

Atmospheric hydroxyl radical production from electronically excited NO2 and H2O.

PubMed

Li, Shuping; Matthews, Jamie; Sinha, Amitabha

2008-03-21

Hydroxyl radicals are often called the "detergent" of the atmosphere because they control the atmosphere's capacity to cleanse itself of pollutants. Here, we show that the reaction of electronically excited nitrogen dioxide with water can be an important source of tropospheric hydroxyl radicals. Using measured rate data, along with available solar flux and atmospheric mixing ratios, we demonstrate that the tropospheric hydroxyl contribution from this source can be a substantial fraction (50%) of that from the traditional O(1D) + H2O reaction in the boundary-layer region for high solar zenith angles. Inclusion of this chemistry is expected to affect modeling of urban air quality, where the interactions of sunlight with emitted NOx species, volatile organic compounds, and hydroxyl radicals are central in determining the rate of ozone formation.

The Evolution of Tropospheric Temperature Field and its Relationship With The Onset of Asian Summer Monsoon

NASA Technical Reports Server (NTRS)

He, H.; Sui, C-H.; Jian, M.; Wen, Z.

2000-01-01

The mean state and year-to-year variations of the tropospheric temperature fields and their relationship with the establishment of the summertime East Asian monsoon (EAM) and the Indian monsoon (INM) are studied using the NCEP reanalysis data of 15 years (1982-1996). The results show that the seasonal shift of the South Asian High in the upper troposphere and the establishment of the EAM and the INM are closely related to the seasonal warming which causes a reversal of the meridional gradient of upper tropospheric mean temperature over the monsoon regions. On the average of 15 years, the reversal time of the temperature gradient in the EAM region (INM region) is concurrent with (one pentad earlier than) the onset time of the summer monsoon. In most years of the 15-year period, the reversal of temperature gradient coincides or precedes the onset time of the summer monsoon in both the EAM region and the INM region. The results suggest an important role of thermal processes on the establishment of the Asian monsoon. The contributors to the upper tropospheric warming over the EAM region are the strong horizontal warm advection and the diabetic heating against the adiabatic cooling due to upward motion. In the INM region, strong adiabatic heating by subsidence and the diabetic heating are major warming processes against the strong horizontal cold advection related to the persistent northwestlies to the southwestern periphery of the Tibetan Plateau. It appears that the early or late establishment of the Asian summer monsoon is not directly related to the differential warming near the surface.

New Particle Formation in the Mid-Latitude Upper Troposphere

NASA Astrophysics Data System (ADS)

Axisa, Duncan

Primary aerosol production due to new particle formation (NPF) in the upper troposphere and the impact that this might have on cloud condensation nuclei (CCN) concentration can be of sufficient magnitude to contribute to the uncertainty in radiative forcing. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Therefore, new particle formation must be accurately defined, parametrized and accounted for in models. This research involved the deployment of instruments, data analysis and interpretation of particle formation events during the Mid-latitude Airborne Cirrus Properties Experiment (MACPEX) campaign. The approach combined field measurements and observations with extensive data analysis and modeling to study the process of new particle formation and growth to CCN active sizes. Simultaneous measurements of O3, CO, ultrafine aerosol particles and surface area from a high-altitude research aircraft were used to study tropospheric-stratospheric mixing as well as the frequency and location of NPF. It was found that the upper troposphere was an active region in the production of new particles by gas-to-particle conversion, that nucleation was triggered by convective clouds and mixing processes, and that NPF occurred in regions with high relative humidity and low surface area. In certain cases, mesoscale and synoptic features enhanced mixing and facilitated the formation of new particles in the northern mid-latitudes. A modeling study of particle growth and CCN formation was done based on measured aerosol size distributions and modeled growth. The results indicate that when SO2 is of sufficient concentration NPF is a significant source of potential CCN in the upper troposphere. In conditions where convective cloud outflow eject high concentrations of SO2, a large number of new particles can form especially in the instance when the preexisting surface area is low. The fast growth of nucleated clusters produces a particle mode that becomes CCN active within 24-hours.

Laboratory Studies of Homogeneous and Heterogeneous Chemical Processes of Importance in the Upper Atmosphere

NASA Technical Reports Server (NTRS)

Molina, Mario J.

2001-01-01

The objective of this study is to conduct measurements of chemical kinetics parameters for reactions of importance in the stratosphere and upper troposphere, and to study the interaction of trace gases such as HCl with ice surfaces in order to elucidate the mechanism of heterogeneous chlorine activation processes, using both a theoretical and an experimental approach. The measurements will be carried out under temperature and pressure conditions covering those applicable to the stratosphere and upper troposphere. The techniques to be employed include turbulent flow - chemical ionization mass spectrometry, and optical ellipsometry. The next section summarizes our research activities during the second year of the project, and the section that follows consists of the statement of work for the third year.

Subtropical westerly jet waveguide and winter persistent heavy rainfall in south China

NASA Astrophysics Data System (ADS)

Ding, Feng; Li, Chun

2017-07-01

Using observed daily precipitation and National Centers for Environmental Prediction-National Center for Atmospheric Research reanalysis data, what induced winter large spatial persistent heavy rainfall (PHR) events in south China was examined, based on composite analyses of 30 large spatial PHR events during 1951-2015. The results showed that wave trains within North Africa-Asia (NAA) westerly jet existed in upper troposphere during these PHR processes. The wave trains shared the characteristic of a Rossby wave. The Rossby wave originated from northwest Europe, entered into the NAA jet through strong cold air advection to form convergence over the Mediterranean, and then propagated eastward along subtropical NAA jet. The Rossby wave propagated toward Southeast Asia and caused strong divergence in the upper troposphere. The strong divergence in the upper troposphere induced vertical convection and favored large spatial PHR events in south China. In addition, the enhanced India-Burma trough and subtropical high in the northwestern Pacific supplied enough water vapor transportation. This mechanism would be useful to the medium-range forecast of such winter rainfall processes over south China.

Atmos/Atlas 3 Infrared Profile Measurements of Trace Gases in The November 1994 Tropical and Subtropical Upper Troposphere

NASA Technical Reports Server (NTRS)

Rinsland, C. P.; Gunson, M. R.; Wang, P.-H.; Arduini, R. F.; Baum, B. A.; Minnis, P.; Minnis, P.; Goldman, A.; Abrams, M. C.; Zander, R.;

Elevated O3 in Fresh and Aged Lightning-NOx Plumes Interacting with Biomass Burning Plumes over the Central U.S. during DC3 (Invited)

NASA Astrophysics Data System (ADS)

Huntrieser, H.; Lichtenstern, M.; Scheibe, M.; Aufmhoff, H.; Schlager, H.; Pucik, T.; Minikin, A.; Weinzierl, B.; Heimerl, K.; Fütterer, D.; Rappenglück, B.; Ackermann, L.; Pickering, K. E.; Cummings, K.; Barth, M. C.

2013-12-01

During the Deep Convective Clouds and Chemistry Experiment (DC3) in summer 2012 a variety of different thunderstorm systems were investigated over the Central U.S. by the DLR research aircraft Falcon together with the NCAR GV and NASA DC-8 aircraft. In addition, the complete DC3 field phase was characterized by a number of extended wildfires burning in the surroundings of the thunderstorms. Here we mainly focus on trace gas in situ measurements, such as NOx, CO, O3, CH4, SO2, NMHC, and a variety of aerosol measurements carried out by the Falcon in the fresh (~0-6 h) and aged (~12-24 h) anvil outflow at ~10-12 km altitude. It is well-known that thunderstorms modify the trace gas composition in the upper troposphere (UT) and may affect O3 mixing ratios, an important greenhouse gas in the UT. However, a complete picture of the different processes affecting the UT-O3 composition in vicinity of thunderstorms and its large-scale effects is still missing. From the DC3 data set we present an example of small-scale effects on the O3 composition in the anvil outflow, such as immediate O3 production by an aircraft-induced flash. But we also show how the efficient convective transport that extended over the whole updraft region may transport O3-poorer air masses from the, in general, rather unpolluted inflow region (with regard to anthropogenic emissions) over the Central U.S. directly to the UT. However, in a few cases enhanced O3 mixing ratios were observed in the anvil outflow attributed to different chemical and dynamical processes. In the two most powerful convective systems, an intense MCS over Missouri/Arkansas and a supercell over Texas, extended biomass burning (BB) plumes from New Mexico interacted with the thunderstorms. Ozone production was obvious in the BB plumes transported mainly in the lower troposphere at ~2-5 km altitude (ΔO3/ΔCO=0.1). However, if these air masses affected by BB emissions (containing high amounts of O3 precursors such as CH4 and NMHC) were ingested into the surrounding thunderstorms (with high HOx and NOx) and transported to the UT region, the ΔO3/ΔCO slope increased dramatically to values up to ~0.6-2.5. In addition to enhanced O3 production rates in thunderstorm outflows interacting with BB plumes, the pronounced downward mixing of O3-rich air mass from the stratosphere down to 8 km was observed in an aged anvil outflow from a squall line active over Colorado which was advected to Kansas the day after. Overall, from the local DC3 Falcon measurements the effect of downward mixing of O3-rich stratospheric air masses seems to cause the largest increase in O3 mixing ratios in the aged anvil outflow.

Five blind men and the elephant: what can the NASA Aura ozone measurements tell us about stratosphere-troposphere exchange?

NASA Astrophysics Data System (ADS)

Tang, Q.; Prather, M. J.

2012-03-01

We examine whether the individual ozone (O3) measurements from the four Aura instruments can quantify the stratosphere-troposphere exchange (STE) flux of O3, an important term of the tropospheric O3 budget. The level 2 (L2) Aura swath data and the nearly coincident ozone sondes for the years 2005-2006 are compared with the 4-D, high-resolution (1° × 1° × 40-layer × 0.5 h) model simulation of atmospheric ozone for the same period from the University of California, Irvine chemistry transport model (CTM). The CTM becomes a transfer standard for comparing individual profiles from these five, not-quite-coincident measurements of atmospheric ozone. Even with obvious model discrepancies identified here, the CTM can readily quantify instrument-instrument biases in the tropical upper troposphere and mid-latitude lower stratosphere. In terms of STE processes, all four Aura datasets have some skill in identifying stratosphere-troposphere folds, and we find several cases where both model and measurements see evidence of high-O3 stratospheric air entering the troposphere. In many cases identified in the model, however, the individual Aura profile retrievals in the upper troposphere and lower stratosphere show too much noise, as expected from their low sensitivity and coarse vertical resolution at and below the tropopause. These model-measurement comparisons of individual profiles do provide some level of confidence in the model-derived STE O3 flux, but it will be difficult to integrate this flux from the satellite data alone.

Tropospheric Waves, Jet Streams, and United States Weather Patterns. Resource Paper No. 11.

ERIC Educational Resources Information Center

Harman, Jay R.

Intended as a supplement to undergraduate college geography courses, this resource paper reviews the mechanism by which surface weather features are linked with the mid-atmospheric circulation within the westerly wind belt. Specifically, vertical atmospheric motions associated with certain aspects of the upper tropospheric flow, including jet…

Organic nitrate chemistry and its implications for nitrogen budgets in an isoprene- and monoterpene-rich atmosphere: constraints from aircraft (SEAC4RS) and ground-based (SOAS) observations in the Southeast US

PubMed Central

Fisher, J. A.; Jacob, D. J.; Travis, K. R.; Kim, P. S.; Marais, E. A.; Miller, C. Chan; Yu, K.; Zhu, L.; Yantosca, R. M.; Sulprizio, M. P.; Mao, J.; Wennberg, P. O.; Crounse, J. D.; Teng, A. P.; Nguyen, T. B.; St. Clair, J. M.; Cohen, R. C.; Romer, P.; Nault, B. A.; Wooldridge, P. J.; Jimenez, J. L.; Campuzano-Jost, P.; Day, D. A.; Hu, W.; Shepson, P. B.; Xiong, F.; Blake, D. R.; Goldstein, A. H.; Misztal, P. K.; Hanisco, T. F.; Wolfe, G. M.; Ryerson, T. B.; Wisthaler, A.; Mikoviny, T.

2018-01-01

Formation of organic nitrates (RONO2) during oxidation of biogenic volatile organic compounds (BVOCs: isoprene, monoterpenes) is a significant loss pathway for atmospheric nitrogen oxide radicals (NOx), but the chemistry of RONO2 formation and degradation remains uncertain. Here we implement a new BVOC oxidation mechanism (including updated isoprene chemistry, new monoterpene chemistry, and particle uptake of RONO2) in the GEOS-Chem global chemical transport model with ∼25 × 25 km2 resolution over North America. We evaluate the model using aircraft (SEAC4RS) and ground-based (SOAS) observations of NOx, BVOCs, and RONO2 from the Southeast US in summer 2013. The updated simulation successfully reproduces the concentrations of individual gas- and particle-phase RONO2 species measured during the campaigns. Gas-phase isoprene nitrates account for 25-50% of observed RONO2 in surface air, and we find that another 10% is contributed by gas-phase monoterpene nitrates. Observations in the free troposphere show an important contribution from long-lived nitrates derived from anthropogenic VOCs. During both campaigns, at least 10% of observed boundary layer RONO2 were in the particle phase. We find that aerosol uptake followed by hydrolysis to HNO3 accounts for 60% of simulated gas-phase RONO2 loss in the boundary layer. Other losses are 20% by photolysis to recycle NOx and 15% by dry deposition. RONO2 production accounts for 20% of the net regional NOx sink in the Southeast US in summer, limited by the spatial segregation between BVOC and NOx emissions. This segregation implies that RONO2 production will remain a minor sink for NOx in the Southeast US in the future even as NOx emissions continue to decline. PMID:29681921

Air motion determination by tracking humidity patterns in isentropic layers

NASA Technical Reports Server (NTRS)

Mancuso, R. L.; Hall, D. J.

1975-01-01

Determining air motions by tracking humidity patterns in isentropic layers was investigated. Upper-air rawinsonde data from the NSSL network and from the AVE-II pilot experiment were used to simulate temperature and humidity profile data that will eventually be available from geosynchronous satellites. Polynomial surfaces that move with time were fitted to the mixing-ratio values of the different isentropic layers. The velocity components of the polynomial surfaces are part of the coefficients that are determined in order to give an optimum fitting of the data. In the mid-troposphere, the derived humidity motions were in good agreement with the winds measured by rawinsondes so long as there were few or no clouds and the lapse rate was relatively stable. In the lower troposphere, the humidity motions were unreliable primarily because of nonadiabatic processes and unstable lapse rates. In the upper troposphere, the humidity amounts were too low to be measured with sufficient accuracy to give reliable results. However, it appears that humidity motions could be used to provide mid-tropospheric wind data over large regions of the globe.

Improvement of OMI Ozone Profile Retrievals in the Troposphere and Lower Troposphere by the Use of the Tropopause-Based Ozone Profile Climatology

NASA Technical Reports Server (NTRS)

Bak, Juseon; Liu, X.; Wei, J.; Kim, J. H.; Chance, K.; Barnet, C.

2011-01-01

An advance algorithm based on the optimal estimation technique has beeen developed to derive ozone profile from GOME UV radiances and have adapted it to OMI UV radiances. OMI vertical resolution : 7-11 km in the troposphere and 10-14 km in the stratosphere. Satellite ultraviolet measurements (GOME, OMI) contain little vertical information for the small scale of ozone, especially in the upper troposphere (UT) and lower stratosphere (LS) where the sharp O3 gradient across the tropopause and large ozone variability are observed. Therefore, retrievals depend greatly on the a-priori knowledge in the UTLS

Carbon monoxide measurements in the troposphere

NASA Technical Reports Server (NTRS)

Reichle, H. G., Jr.; Beck, S. M.; Haynes, R. E.; Hesketh, W. D.; Holland, J. A.; Hypes, W. D.; Orr, H. D., III; Sherrill, R. T.; Wallio, H. A.; Casas, J. C.

1982-01-01

Approximately 35 hours of radiometric measurements were obtained of the CO mixing ratio in the middle troposphere, upper troposphere, and lower stratosphere, by means of the Measurement of Air Pollution from Satellites (MAPS) experiment carried in the OSTA-1 payload of the second Space Shuttle flight. In view of gas filter radiometer data in the 4.67-micron band, gathered over the 38 N-38 S latitude region during both daytime and nighttime, the performance of MAPS was excellent. Significant gradients have been found in the middle tropospheric CO mixing ratio with both latitude and longitude over the North Atlantic, the Mediterranean Sea, and the Middle East.

The use of satellite data to determine the distribution of ozone in the troposphere

NASA Technical Reports Server (NTRS)

Fishman, Jack; Watson, Catherine E.; Brackett, Vincent G.; Fakhruzzaman, Khan; Veiga, Robert E.

1991-01-01

Measurements from two independent satellite data sets have been used to derive the climatology of the integrated amount of ozone in the troposphere. These data have led to the finding that large amounts of ozone pollution are generated by anthropogenic activity originating from both the industrialized regions of the Northern Hemisphere and from the southern tropical regions of Africa. To verify the existence of this ozone anomaly at low latitudes, an ozonesonde capability has been established at Ascension Island (8 deg S, 15 deg W) since July 1990. According to the satellite analyses, Ascension Island is located downwind of the primary source region of this ozone pollution, which likely results from the photochemical oxidation of emissions emanating from the widespread burning of savannas and other biomass. These in situ measurements confirm the existence of large amounts of ozone in the lower atmosphere. A summary of these ozonesonde data to date will be presented. In addition, we will present some ozone profile measurements from SAGE II which can be used to provide upper tropospheric ozone measurements directly in the tropical troposphere. A preliminary comparison between the satellite observations and the ozonesonde profiles in the upper troposphere and lower stratosphere will also be presented.

Chemical Composition and Dynamics of the Upper Troposphere and the Lower Stratosphere: Overview of the Project

NASA Astrophysics Data System (ADS)

Sofieva, V. F.; Liu, C.; Huang, F.; Kyrola, E.; Liu, Y.; Ialongo, I.; Hakkarainen, J.; Zhang, Y.

2016-08-01

The DRAGON-3 cooperation study on the upper troposphere and the lower stratosphere (UTLS) is based on new satellite data and modern atmospheric models. The objectives of the project are: (i) assessment of satellite data on chemical composition in UTLS, (ii) dynamical and chemical structures of the UTLS and its variability, (iii) multi-scale variability of stratospheric ozone, (iv) climatology of the stratospheric aerosol layer and its variability, and (v) updated ozone climatology and its relation to tropopause/multiple tropopauses.In this paper, we present the main results of the project.

Interpretation of Aura satellite observations of CO and aerosol index related to the December 2006 Australia fires

NASA Astrophysics Data System (ADS)

Luo, M.; Boxe, C.; Jiang, J.; Nassar, R.; Livesey, N.

2009-11-01

Enhanced Carbon Monoxide (CO) in the upper troposphere (UT) is shown by collocated Tropospheric Emission Spectrometer (TES) and Microwave Limb Sounder (MLS) measurements near and down-wind from the known wildfire region of SE Australia from 12-19 December 2006. Enhanced UV aerosol index (AI) derived from Ozone Monitoring Instrument (OMI) measurements correlate with these high CO concentrations. HYSPLIT model back trajectories trace selected air parcels to the SE Australia fire region as their initial location, where TES observes enhanced CO in the upper and lower troposphere. Simultaneously, they show a lack of vertical advection along their tracks. TES retrieved CO vertical profiles in the higher and lower southern latitudes are examined together with the averaging kernels and show that TES CO retrievals are most sensitive at approximately 300-400 hPa. The enhanced CO observed by TES at the upper (215 hPa) and lower (681 hPa) troposphere are, therefore, influenced by mid-tropospheric CO. GEOS-Chem model simulations with an 8-day emission inventory, as the wildfire source over Australia, are sampled to the TES/MLS observation times and locations. These simulations only show CO enhancements in the lower troposphere near and down-wind from the wildfire region of SE Australia with drastic underestimates of UT CO. Although CloudSat along-track ice-water content curtains are examined to see whether possible vertical convection events can explain the high UT CO values, sparse observations of collocated Aura CO and CloudSat along-track ice-water content measurements for the single event precludes any conclusive correlation. Vertical convection that uplift fire-induced CO (i.e. most notably referred to as pyro-cumulonimbus, pyroCb) may provide an explanation for the incongruence between these simulations and the TES/MLS observations of enhanced CO in the UT. Future GEOS-Chem simulations are needed to validate this conjecture as the the PyroCb mechanism is currently not incorporated in GEOS-Chem.

Description and Evaluation of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry Model (NMMB-MONARCH) Version 1.0: Gas-Phase Chemistry at Global Scale

NASA Technical Reports Server (NTRS)

Badia, Alba; Jorba, Oriol; Voulgarakis, Apostolos; Dabdub, Donald; Garcia-Pando, Carlos Perez; Hilboll, Andreas; Goncalves, Maria; Janjic, Zavisa

2017-01-01

This paper presents a comprehensive description and benchmark evaluation of the tropospheric gas-phase chemistry component of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (NMMBMONARCH), formerly known as NMMB/BSC-CTM, that can be run on both regional and global domains. Here, we provide an extensive evaluation of a global annual cycle simulation using a variety of background surface stations (EMEP, WDCGG and CASTNET), ozonesondes (WOUDC, CMD and SHADOZ), aircraft data (MOZAIC and several campaigns), and satellite observations (SCIAMACHY and MOPITT).We also include an extensive discussion of our results in comparison to other state-of-the-art models. We note that in this study, we omitted aerosol processes and some natural emissions (lightning and volcano emissions). The model shows a realistic oxidative capacity across the globe. The seasonal cycle for CO is fairly well represented at different locations (correlations around 0.3-0.7 in surface concentrations), although concentrations are underestimated in spring and winter in the Northern Hemisphere, and are overestimated throughout the year at 800 and 500 hPa in the Southern Hemisphere. Nitrogen species are well represented in almost all locations, particularly NO2 in Europe (root mean square error - RMSE - below 5 ppb). The modeled vertical distributions of NOx and HNO3 are in excellent agreement with the observed values and the spatial and seasonal trends of tropospheric NO2 columns correspond well to observations from SCIAMACHY, capturing the highly polluted areas and the biomass burning cycle throughout the year. Over Asia, the model underestimates NOx from March to August, probably due to an underestimation of NOx emissions in the region. Overall, the comparison of the modeled CO and NO2 with MOPITT and SCIAMACHY observations emphasizes the need for more accurate emission rates from anthropogenic and biomass burning sources (i.e., specification of temporal variability).

Decline in tropospheric NO2 and the effects of the 2008-09 economic crisis observed by OMI over Europe

NASA Astrophysics Data System (ADS)

Castellanos, P.; Boersma, F. F.

2011-12-01

We present a trend analysis of tropospheric NO2 for the time period of 2004-2010. Necessary for monitoring pollution abatement strategies, NO2 trends analyses are often based on surface networks, which suffer from high NO2 biases and spatial representativity issues inherent to the standard monitoring method (thermal reduction of NO2 followed by reaction with ozone and chemiluminescence). Space based NO2 trends are unbiased and self-consistent, but over Europe they have not been as obvious as those observed over North America and East Asia. In this work we exploit the daily NO2 column observations from the Ozone Monitoring Instrument (OMI) in order to isolate long-term (timescales greater than one year) variability in NO2 over Europe without imposing a parametric fit to the data. In general, we find between 2005 and 2008, 1-5% per year declines in NO2 concentration in many polluted regions (e.g. Germany, Netherlands, Belgium, Italy, Spain), but also 1-5% per year increases over the English Channel and the southern North Sea (a major shipping channel), as well as the United Kingdom, northern France and Eastern Europe. In 2009, NO2 almost exclusively decreased over Europe at a rate of 5-10% per year, coinciding with the abrupt decrease in industrial production and construction prompted by the global economic crisis. By 2010, in many areas the NO2 rate of change returned to pre-2009 levels suggesting economic recovery. We employ a simple fitting model to separate the forcing by meteorological variability, which can influence apparent NO2 trends, from that of NOx emissions. We calculate 1-3% per year NOx emissions reduction rates over most of Europe and an additional 15-30% per year decrease in NOx emissions during the economic crisis time period.

Measurements of in situ chemical ozone (oxidant) production rates

NASA Astrophysics Data System (ADS)

Huang, Hao; Faloon, Kate; Najera, Juan; Bloss, William

2013-04-01

Tropospheric ozone is a major air pollutant, harmful to human health, agricultural crops and vegetation, the main precursor to the atmospheric oxidants which initiate the degradation of most reactive gases emitted to the atmosphere, and an important greenhouse gas in its own right. The capacity to understand and predict tropospheric ozone levels is a key goal for atmospheric science - but one which is challenging, as ozone is formed in the atmosphere from the complex oxidation of VOCs in the presence of NOx and sunlight, on a timescale such that in situ chemical processes, deposition and transport all affect ozone levels. Known uncertainties in emissions, chemistry, dynamics and deposition affect the accuracy of predictions of current and future ozone levels, and hinder development of optimal air quality policies to mitigate against ozone exposure. Recently new approaches to directly measure the local chemical ozone production rate, bypassing the many uncertainties in emissions and chemical schemes, have been developed (Cazorla & Brune, AMT 2010). Here, we describe the development of an analogous Ozone Production Rate (OPR) approach: Air is sampled into parallel reactors, within which ozone formation either occurs as in the ambient atmosphere, or is suppressed. Comparisons of ozone levels exiting a pair of such reactors determines the net chemical oxidant production rate, after correction for perturbation of the NOx-O3 photochemical steady state, and when operated under conditions such that wall effects are minimised. We report preliminary measurements of local chemical ozone production made during the UK NERC ClearfLo (Clean Air for London) campaign at an urban background location in London in January and July 2012. The OPR system was used to measure the local chemical oxidant formation rate, which is compared with observed trends in O3 and NOx and the prevailing meteorology, and with the predictions of a detailed zero-dimensional atmospheric chemistry model, constrained by observations of long-lived species.

Study of Nox Levels At The Castellon Area (spain) By Means of Passive Samplers

NASA Astrophysics Data System (ADS)

Delgado, J. M.; Esteve, V.

Nitrogen oxides are emitted by mobile sources like traffic, heating engines and indus- tries. In the case of La Plana de Castellon area, the cities, the industrial area called El Serrallo (with its oil refinery and power plant), the tile factories and the main roads (A7-E15 and N-340), all they are the main pollutant focus of NOx. Those pollutants are precursors of tropospheric ozone formation. The aim of this work is the study of nitrogen oxides levels in La Plana de Castellon area, by means of passive samplers and stand relationships between NOx levels and ozone levels both measured with pas- sive samplers. The measurement campaign is made during summer, the higher pho- tochemical activity period (from May to September) in order to obtain the necessary data of NOx levels to make the relationship with measured ozone levels. Measuring campaing has been divided into sampling periods of one week. Twelve samples are collected each sampling period to cover an interest area of 1400 Km2, Two of these samples are laboratory blanks, four are situated at reference points (beside an auto- matic NOx sampler), one is situated at A7-E15 expressway, other at the main road N-340 and another one in a hard traffic road. The other three are placed in the main cities (Castellon and Benicassim). We employ Radielloo samplers developed by Dr. Cocheo at Fondazione Salvatore Maugeri. Samples located far from the main roads, at countryside show the lowest levels of NOx, lower than 10 ppb. Samples located at Castellon city show a difference between downtown and boundaries of about 33% higher at downtown, raising from 11 ppb to 14,5 ppb of NOx. The highest levels of NOx are measured at roads and their surroundings with medium levels of 14,3 ppb of NOx. Moreover, the sample located close to the expressway raises its level until 18 ppb of NOx, 53,4% higher than the media of all the samples measured. We would like to thank Dr. M. Wolfson(Harvard University), Dr. Carlos Felis (Conselleria de Medi Ambient) and Ms. C. Clemente for their contribution and work on this project as well as to Generalitat Valenciana for the FPI grant.

Changes in tropospheric composition and air quality due to stratospheric ozone depletion.

PubMed

Solomon, Keith R; Tang, Xiaoyan; Wilson, Stephen R; Zanis, Prodromos; Bais, Alkiviadis F

2003-01-01

Increased UV-B through stratospheric ozone depletion leads to an increased chemical activity in the lower atmosphere (the troposphere). The effect of stratospheric ozone depletion on tropospheric ozone is small (though significant) compared to the ozone generated anthropogenically in areas already experiencing air pollution. Modeling and experimental studies suggest that the impacts of stratospheric ozone depletion on tropospheric ozone are different at different altitudes and for different chemical regimes. As a result the increase in ozone due to stratospheric ozone depletion may be greater in polluted regions. Attributable effects on concentrations are expected only in regions where local emissions make minor contributions. The vertical distribution of NOx (NO + NO2), the emission of volatile organic compounds and the abundance of water vapor, are important influencing factors. The long-term nature of stratospheric ozone depletion means that even a small increase in tropospheric ozone concentration can have a significant impact on human health and the environment. Trifluoroacetic acid (TFA) and chlorodifluoroacetic acid (CDFA) are produced by the atmospheric degradation of hydrochlorofluorocarbons (HCFCs) and hydrofluorocarbons (HFCs). TFA has been measured in rain, rivers, lakes, and oceans, the ultimate sink for these and related compounds. Significant anthropogenic sources of TFA other than degradation HCFCs and HFCs have been identified. Toxicity tests under field conditions indicate that the concentrations of TFA and CDFA currently produced by the atmospheric degradation of HFCs and HCFCs do not present a risk to human health and the environment. The impact of the interaction between ozone depletion and future climate change is complex and a significant area of current research. For air quality and tropospheric composition, a range of physical parameters such as temperature, cloudiness and atmospheric transport will modify the impact of UV-B. Changes in the chemical composition of the atmosphere including aerosols will also have an impact. For example, tropospheric OH is the 'cleaning' agent of the troposphere. While increased UV-B increases the OH concentration, increases in concentration of gases like methane, carbon monoxide and volatile organic compounds will act as sinks for OH in troposphere and hence change air quality and chemical composition in the troposphere. Also, changes in the aerosol content of the atmosphere resulting from global climate change may affect ozone photolysis rate coefficients and hence reduce or increase tropospheric ozone concentrations.

Vertical structure of tropospheric winds on gas giants

NASA Astrophysics Data System (ADS)

Scott, R. K.; Dunkerton, T. J.

2017-04-01

Zonal mean zonal velocity profiles from cloud-tracking observations on Jupiter and Saturn are used to infer latitudinal variations of potential temperature consistent with a shear stable potential vorticity distribution. Immediately below the cloud tops, density stratification is weaker on the poleward and stronger on the equatorward flanks of midlatitude jets, while at greater depth the opposite relation holds. Thermal wind balance then yields the associated vertical shears of midlatitude jets in an altitude range bounded above by the cloud tops and bounded below by the level where the latitudinal gradient of static stability changes sign. The inferred vertical shear below the cloud tops is consistent with existing thermal profiling of the upper troposphere. The sense of the associated mean meridional circulation in the upper troposphere is discussed, and expected magnitudes are given based on existing estimates of the radiative timescale on each planet.

Interhemispheric comparison of atmospheric circulation features as evaluated from Nimbus satellite data. A comparison of the structure and flow characteristics of the upper troposphere and stratosphere of the Northern and Southern Hemispheres. Ph.D. Thesis. Annual Report, 1 Nov. 1973 - 31 Oct. 1974

NASA Technical Reports Server (NTRS)

Reiter, E. R.; Adler, R.; Fields, A.

1974-01-01

The general circulations of the Northern and Southern Hemispheres are compared with regard to the upper troposphere and stratosphere, using atmospheric structure obtained from multi-channel radiance data from the satellite infrared spectrometer instrument aboard the Nimbus 3 spacecraft. The inter-hemispheric comparisons are based on two months of data (one summer month and one winter month) in each hemisphere. Topics studied include: (1) mean meridional circulation in the Southern Hemisphere stratosphere; (2) magnitude and distribution of tropospheric eddy heat flux; (3) relative importance of standing and transient eddies in the two hemispheres; (4) magnitudes of energy cycle components; and (5) the relation of vortex structure to the breakdown climatology of the Antarctic stratospheric polar vortex.

The synoptic setting and possible energy sources for mesoscale wave disturbances

NASA Technical Reports Server (NTRS)

Uccellini, Louis W.; Koch, Steven E.

1987-01-01

Published data on 13 cases of mesoscale wave disturbances and their environment were examined to isolate common features for these cases and to determine possible energy sources for the waves. These events are characterized by either a singular wave of depression or wave packets with periods of 1-4 h, horizontal wavelengths of 50-500 km, and surface-pressure perturbation amplitudes of 0.2-7.0 mb. These wave events are shown to be associated with a distinct synoptic pattern (including the existence of a strong inversion in the lower troposphere and the propagation of a jet streak toward a ridge axis in the upper troposphere) while displaying little correlation with the presence of convective storm cells. The observed development of the waves is consistent with the hypothesis that the energy source needed to initiate and sustain the wave disturbances may be related to a geostrophic adjustment process associated with upper-tropospheric jet streaks.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bony, Sandrine; Stevens, Bjorn; Coppin, David

General circulation models show that as the surface temperature increases, the convective anvil clouds shrink. By analyzing radiative–convective equilibrium simulations, our work shows that this behavior is rooted in basic energetic and thermodynamic properties of the atmosphere: As the climate warms, the clouds rise and remain at nearly the same temperature, but find themselves in a more stable atmosphere; this enhanced stability reduces the convective outflow in the upper troposphere and decreases the anvil cloud fraction. By warming the troposphere and increasing the upper-tropospheric stability, the clustering of deep convection also reduces the convective outflow and the anvil cloud fraction.more » When clouds are radiatively active, this robust coupling between temperature, high clouds, and circulation exerts a positive feedback on convective aggregation and favors the maintenance of strongly aggregated atmospheric states at high temperatures. This stability iris mechanism likely contributes to the narrowing of rainy areas as the climate warms. Whether or not it influences climate sensitivity requires further investigation.« less

The possible influences of the increasing anthropogenic emissions in India on tropospheric ozone and OH

NASA Astrophysics Data System (ADS)

Liu, Yu; Li, Weiliang; Zhou, Xiuji; Isaksen, I. S. A.; Sundet, J. K.; He, Jinhai

2003-11-01

A 3-D chemical transport model (OSLO CTM2) is used to investigate the influences of the increasing anthropogenic emission in India. The model is capable of reproducing the observational results of the INDOEX experiment and the measurements in summer over India well. The model results show that when NO x and CO emissions in India are doubled, ozone concentration increases, and global average OH decreases a little. Under the effects of the Indian summer monsoon, NO x and CO in India are efficiently transported into the middle and upper troposphere by the upward current and the convective activities so that the NO x , CO, and ozone in the middle and upper troposphere significantly increase with the increasing NO x and CO emissions. These increases extensively influence a part of Asia, Africa, and Europe, and persist from June to September.

Factors dominating 3-dimensional ozone distribution during high tropospheric ozone period.

PubMed

Chen, Xiaoyang; Liu, Yiming; Lai, Anqi; Han, Shuangshuang; Fan, Qi; Wang, Xuemei; Ling, Zhenhao; Huang, Fuxiang; Fan, Shaojia

2018-01-01

Data from an in situ monitoring network and five ozone sondes are analysed during August of 2012, and a high tropospheric ozone episode is observed around the 8th of AUG. The Community Multi-scale Air Quality (CMAQ) model and its process analysis tool were used to study factors and mechanisms for high ozone mixing ratio at different levels of ozone vertical profiles. A sensitive scenario without chemical initial and boundary conditions (ICBCs) from MOZART4-GEOS5 was applied to study the impact of stratosphere-troposphere exchange (STE) on vertical ozone. The simulation results indicated that the first high ozone peak near the tropopause was dominated by STE. Results from process analysis showed that: in the urban area, the second peak at approximately 2 km above ground height was mainly caused by local photochemical production. The third peak (near surface) was mainly caused by the upwind transportation from the suburban/rural areas; in the suburban/rural areas, local photochemical production of ozone dominated the high ozone mixing ratio from the surface to approximately 3 km height. Furthermore, the capability of indicators to distinguish O 3 -precursor sensitivity along the vertical O 3 profiles was investigated. Two sensitive scenarios, which had cut 30% anthropogenic NO X or VOC emissions, showed that O 3 -precursor indicators, specifically the ratios of O 3 /NOy, H 2 O 2 /HNO 3 or H 2 O 2 /NO Z , could partly distinguish the O 3 -precursor sensitivity between VOCs-sensitive and NOx-sensitive along the vertical profiles. In urban area, the O 3 -precursor relationship transferred from VOCs-sensitive within the boundary layer to NOx-sensitive at approximately 1-3 km above ground height, further confirming the dominant roles of transportation and photochemical production in high O 3 peaks at the near-ground layer and 2 km above ground height, respectively. Copyright © 2017 Elsevier Ltd. All rights reserved.

Upper tropospheric ice sensitivity to sulfate geoengineering

NASA Astrophysics Data System (ADS)

Visioni, Daniele; Pitari, Giovanni; Mancini, Eva

2017-04-01

In light of the Paris Agreement which aims to keep global warming under 2 °C in the next century and considering the emission scenarios produced by the IPCC for the same time span, it is likely that to remain below that threshold some kind of geoengineering technique will have to be deployed. Amongst the different methods, the injection of sulfur into the stratosphere has received much attention considering its effectiveness and affordability. Aside from the rather well established surface cooling sulfate geoengineering (SG) would produce, the investigation on possible side-effects of this method is still ongoing. For instance, some recent studies have investigated the effect SG would have on upper tropospheric cirrus clouds, expecially on the homogenous freezing mechanisms that produces the ice particles (Kuebbeler et al., 2012). The goal of the present study is to better understand the effect of thermal and dynamical anomalies caused by SG on the formation of ice crystals via homogeneous freezing by comparing a complete SG simulation with a RCP4.5 reference case and with a number of sensitivity studies where atmospheric temperature changes in the upper tropospheric region are specified in a schematic way as a function of the aerosol driven stratospheric warming and mid-lower tropospheric cooling. These changes in the temperature profile tend to increase atmospheric stabilization, thus decreasing updraft and with it the amount of water vapor available for homogeneous freezing in the upper troposphere. However, what still needs to be assessed is the interaction between this dynamical effect and the thermal effects of tropospheric cooling (which would increase ice nucleation rates) and stratospheric warming (which would probably extend to the uppermost troposphere via SG aerosol gravitational settling, thus reducing ice nucleation rates), in order to understand how they combine together. Changes in ice clouds coverage could be important for SG, because cirrus ice clouds scatter incoming shortwave and reflect outgoing infrared radiation, with the longwave absorption dominating. This means that a cirrus ice thinning would produce a negative radiative forcing, going in the same direction as the direct effect of incoming radiation scattering by the sulfate aerosol, thus influencing the amount of sulfur needed to counteract the positive RF due to the future increase in greenhouse gases. References: Kuebbeler, M., Lohmann, U., and Feichter, J.: Effects of stratospheric sulfate aerosol geo-engineering on cirrus clouds, Geophysical Research Letters, 39, doi:10.1029/2012GL053797, l23803, 2012.

LASE validation experiment: preliminary processing of relative humidity from LASE derived water vapor in the middle to upper troposphere

NASA Technical Reports Server (NTRS)

Brackett, Vincent G.; Ismail, Syed; Browell, Edward V.; Kooi, Susan A.; Clayton, Marian B.; Ferrare, Richard A.; Minnis, Patrick; Getzewich, Brian J.; Staszel, Jennifer

1998-01-01

Lidar Atmospheric Sensing Experiment (LASE) is the first fully engineered, autonomous airborne DIAL (Differentials Absorption Lidar) system to measure water vapor, aerosols, and clouds throughout the troposphere. This system uses a double-pulsed Ti:sapphire laser, which is pumped by a frequency-doubled flashlamp-pumped Nd: YAG laser, to transmit light in the 815 mn absorption band of water vapor. LASE operates by locking to a strong water vapor line and electronically tuning to any spectral position on the absorption line to choose the suitable absorption cross-section for optimum measurements over a range of concentrations in the atmosphere. During the LASE Validation Experiment, which was conducted over Wallops Island during September, 1995, LASE operated on either the strong water line for measurements in middle to upper troposphere, or on the weak water line for measurements made in the middle to lower troposphere including the boundary layer. Comparisons with water vapor measurements made by airborne dew point and frost point hygrometers, NASA/GSFC (Goddard Space Flight Center) Raman Lidar, and radiosondes showed the LASE water vapor mixing ratio measurements to have an accuracy of better than 6% or 0.01 g/kg, whichever is larger, throughout the troposphere. In addition to measuring water vapor mixing ratio profiles, LASE simultaneously measures aerosol backscattering profiles at the off-line wavelength near 815 nm from which atmospheric scattering ratio (ASR) profiles are calculated. ASR is defined as the ratio of total (aerosol + molecular) atmospheric scattering to molecular scattering. Assuming a region with very low aerosol loading can be identified, such as that typically found just below the tropopause, then the ASR can be determined. The ASR profiles are calculated by normalizing the scattering in the region containing enhanced aerosols to the expected scattering by the "clean" atmosphere at that altitude. Images of the total ASR clearly depict cloud regions, including multiple cloud layers, thin upper level cirrus, etc., throughout the troposphere. New data products that are being derived from the LASE aerosol and water measurements include: 1) aerosol extinction coefficient, 2) aerosol optical thickness, 3) precipitable water vapor, and 4) relative humidity (RH). These products can be compared with airborne in-situ, and ground and satellite remote sensing measurements,. This paper presents a preliminary examination of RH profiles in the middle to upper troposphere that are generated from LASE measured water vapor mixing ratio profiles coupled with rawinsonde profiles of temperature and pressure.

Effects of the 2004 El Nino on Tropospheric Ozone and Water Vapor

NASA Technical Reports Server (NTRS)

Chandra, S.; Ziemke, J. R.; Schoeberl, M. R.; Froidevaux, L.; Read, W. G.; Levelt, P. F.; Bhartia, P. K.

2007-01-01

The global effects of the 2004 El Nino on tropospheric ozone and H2O based on Aura OM1 and MLS measurements are analyzed. Although it was a weak El Nino from a historical perspective, it produced significant changes in these parameters in tropical latitudes. Tropospheric ozone increased by 10-20% over most of the western Pacific region and decreased by about the same amount over the eastern Pacific region. H2O in the upper troposphere showed similar changes but with opposite sign. These zonal changes in tropospheric ozone and H2O are caused by the eastward shift in the Walker circulation in the tropical pacific region during El Nino. For the 2004 El Nino, biomass burning did not have a significant effect on the ozone budget in the troposphere unlike the 1997 El Nino. Zonally averaged tropospheric column ozone did not change significantly either globally or over the tropical and subtropical latitudes.

Peroxyacetyl nitrate measurements during CITE 2 - Atmospheric distribution and precursor relationships

NASA Technical Reports Server (NTRS)

Singh, H. B.; Condon, E.; Vedder, J.; O'Hara, D.; Ridley, B. A.; Gandrud, B. W.; Shetter, J. D.; Beck, S. M.; Gregory, G. L.; Lebel, P. J.

1990-01-01

Results are reported from airborne PAN measurements obtained at altitudes 0-6 km over the continental U.S. and the eastern Pacific during the NASA Global Tropospheric Experiment Chemical Instrumentation Test and Evaluation 2 (CITE 2) in summer 1986. The CITE 2 flights and instrumentation are described, and the results are presented in extensive graphs and characterized in detail. It is shown that PAN is an important reactive N-containing species in the troposphere. Although the PAN mixing ratios were highly variable, in general high mixing ratios of 100-300 parts per trillion by volume (pptv) were found at 4-6 km, and very low ratios (5-20 pptv) were detected in the marine boundary layer. Good correlation was seen between the CITE 2 PAN values and those for O3, NO(y), NO(x), HNO3, C2H6, CO, and CFCl3.

Photochemical oxidant processes in the presence of dust: An evaluation of the impact of dust on particulate nitrate and ozone formation

NASA Technical Reports Server (NTRS)

Zhang, Yang; Sunwoo, Young; Kotamarthi, Veerabhadra; Carmichael, Gregory R.

1994-01-01

The influence of dust on the tropospheric photochemical oxidant cycle is studied through the use of a detailed coupled aerosol and gas-phase chemistry model. Dust is a significant component of the troposphere throughout Asia and provides a surface for a variety of heterogeneous reactions. Dust is found to be an important surface for particulate nitrate formation. For dust loading and ambient concentrations representative of conditions in East Asia, particulate nitrate levels of 1.5-11.5 micrograms/cubic meter are predicted, consistent with measured levels in this region. Dust is also found to reduce NO(x) levels by up to 50%, HO2 concentrations by 20%-80%, and ozone production rates by up to 25%. The magnitude of the influence of dust is sensitive to mass concentration of the aerosol, relative humidity, and the value of the accommodation coefficient.

Lightning NOx and Impacts on Air Quality

NASA Technical Reports Server (NTRS)

Murray, Lee T.

2016-01-01

Lightning generates relatively large but uncertain quantities of nitrogen oxides, critical precursors for ozone and hydroxyl radical (OH), the primary tropospheric oxidants. Lightning nitrogen oxide strongly influences background ozone and OH due to high ozone production efficiencies in the free troposphere, effecting small but non-negligible contributions to surface pollutant concentrations. Lightning globally contributes 3-4 ppbv of simulated annual-mean policy-relevant background (PRB) surface ozone, comprised of local, regional, and hemispheric components, and up to 18 ppbv during individual events. Feedbacks via methane may counter some of these effects on decadal time scales. Lightning contributes approximately 1 percent to annual-mean surface particulate matter, as a direct precursor and by promoting faster oxidation of other precursors. Lightning also ignites wildfires and contributes to nitrogen deposition. Urban pollution influences lightning itself, with implications for regional lightning-nitrogen oxide production and feedbacks on downwind surface pollution. How lightning emissions will change in a warming world remains uncertain.

Future local and remote influences on Mediterranean ozone air quality and climate forcing

NASA Astrophysics Data System (ADS)

Arnold, Steve; Martin, Maria Val; Emmons, Louisa; Rap, Alex; Heald, Colette; Lamarque, Jean-Francois; Tilmes, Simone

2013-04-01

The Mediterranean region is expected to display large increases in population over the coming decades, and to exhibit strong sensitivity to projected climate change, with increasing frequency of extreme summer temperatures and decreases in precipitation. Understanding of how these changes will affect atmospheric composition in the region is limited. The eastern Mediterranean basin has been shown to exhibit a pronounced summertime local maximum in tropospheric ozone, which impacts both local air quality and the atmospheric radiation balance. In summer, the region is subject to import of pollution from Northern Europe in the boundary layer and lower troposphere, from North American sources in the large-scale westerly flow of the free mid and upper-troposphere, as well as import of pollution lofted in the Asian monsoon and carried west to the eastern Mediterranean in anticyclonic flow in the upper troposphere over north Africa. In addition, interactions with the land-surface through biogenic emission sources and dry deposition play important roles in the Mediterranean ozone budget. Here we use the NCAR Community Earth System Model (CESM) to investigate how tropospheric ozone in the Mediterranean region responds to climate, land surface and global emissions changes between present day and 2050. We simulate climate and atmospheric composition for the year 2050, based on greenhouse gas abundances, trace gas and aerosol emissions and land cover and use from two representative concentration pathway (RCP) scenarios (RCP4.5 & RCP8.5), designed for use by the Coupled Model Intercomparison Project Phase 5(CMIP5) experiments in support of the IPCC. By comparing these simulations with a present-day scenario, we investigate the effects of predicted changes in climate and emissions on air quality and climate forcing over the Mediterranean region. The simulations suggest decreases in boundary layer ozone and sulfate aerosol throughout the tropospheric column over the Mediterranean under both RCP scenarios, and a significant increase in ozone between 5-10km. Using tagged regional NOy and tropospheric ozone tracers, we show that this ozone increase is coincident with an increase in easterly import of ozone and precursors in upper tropospheric outflow from Asian monsoon convection in 2050. We present a breakdown of the projected Mediterranean ozone changes by precursor source (anthropogenic and biogenic), and contributions due to changes in climate. Finally, we estimate the implications of the predicted changes in tropospheric composition for Mediterranean air quality and climate in 2050, and the consequences for the effectiveness of European policies aimed at protecting the region's climate and public health.

Impact of near-surface atmospheric composition on ozone formation in Russia

NASA Astrophysics Data System (ADS)

Berezina, Elena; Moiseenko, Konstantin; Skorokhod, Andrey; Belikov, Igor; Pankratova, Natalia; Elansky, Nikolai

2017-04-01

One of the consequences of the human impact on the atmosphere is increasing in tropospheric ozone concentration, with the highest ozone level being observed in industrially developed and highly populated regions of the world. In these regions, main anthropogenic sources of carbon monoxide (CO), methane (CH4) and volatile organic compounds (VOCs) are concentrated. The oxidation of these compounds, when interacting with hydroxyl and nitrogen oxides at rather high temperature and sunlight, leads to ozone formation. CO and CH4 are slowly oxidized in the atmosphere and cause an increase in global and regional background ozone. However, the oxidation of some VOCs occurs during daylight hours and is accompanied by an increase in ozone concentration near VOCs sources, particularly in urban and industrial areas. The contribution of biogenic VOCs to ozone generation is estimated to be from 40 to 70% of the total contribution of all chemical ozone precursors in the troposphere [1], with isoprene playing the main role in ozone formation [2]. The impact of aromatic hydrocarbons to ozone formation is reported to be about 40% of the total ozone generation from the oxidation of anthropogenic VOCs [3]. In this study, the results of VOCs measurements (isoprene, benzene, toluene, phenol, styrene, xylene and propilbenzene) by proton mass spectrometry in different regions of Russia along the Trans-Siberian railway from Moscow to Vladivostok from TROICA-12 campaign on a mobile laboratory in summer 2008 are analyzed. It is shown that the TROICA-12 measurements were carried out mostly in moderately polluted (2≤NOx<20 ppb) environment ( 78% of measurements) with the remaining part of the measurements divided between weakly polluted (NOx≤2 ppb) and highly polluted (NOx>20 ppb) conditions ( 20 and 2% of measurements, correspondingly). The lower troposphere chemical regime in the campaign is found to be mainly NOx sensitive, both in rural and urban environments, with typical morning NMHC/NOx ratios being well above 20. Hence, ozone production rates are expected to be controlled by regional NOx emissions and their complex interplay with both natural and anthropogenic sources of VOCs. The quantitative contribution of aromatic VOCs to ozone formation in urban areas and in Russian regions along the railway is estimated. The greatest impact of aromatic VOCs to ozone formation (up to 7.5 ppb of O3) is obtained in the large cities along the Trans-Siberian Railway, with the highest concentrations of aromatic VOCs (1-1.7 ppb) and nitrogen oxides (> 20 ppb) being observed. The results show a significant contribution of anthropogenic emissions of VOCs to the photochemical ozone generation (30-50%) in the large cities along the Trans-Siberian railway in hot and dry weather conditions against natural isoprene emissions determining the regional balance of ground-level ozone in summer. This study was supported by the Russian Science Foundation (grant no. 14-47-00049) and by the Russian Foundation for Basic Research (grant no. 16-35-00158). References: 1. Xie, X., Shao, M., Liu, Y., Lu, S., Chang, C. C., and Chen, Z. M. // Atmos. Environ., 2008, 42, pp. 6000-6010. 2. Guenther, A., Geron, C., Pierce, T., Lamb, B., Harley, P., Fall, R. // Atmospheric Environment, 2000, 34, pp. 2205-2230. 3. Dreyfus, G. B., Schade G. W., Goldstein A. H. // J. Geophys. Res., 2002, 107(D19): 4365, doi:10.1029/2001JD001490.

Microwave Limb Sounder/El Niño Watch - Water Vapor Measurement, October, 1997

NASA Image and Video Library

1997-10-30

This image shows atmospheric water vapor in Earth upper troposphere, about 10 kilometers 6 miles above the surface, as measured by NASA Microwave Limb Sounder MLS instrument flying aboard the Upper Atmosphere Research Satellite.

Sensitivity to grid resolution in the ability of a chemical transport model to simulate observed oxidant chemistry under high-isoprene conditions

NASA Astrophysics Data System (ADS)

Yu, Karen; Jacob, Daniel J.; Fisher, Jenny A.; Kim, Patrick S.; Marais, Eloise A.; Miller, Christopher C.; Travis, Katherine R.; Zhu, Lei; Yantosca, Robert M.; Sulprizio, Melissa P.; Cohen, Ron C.; Dibb, Jack E.; Fried, Alan; Mikoviny, Tomas; Ryerson, Thomas B.; Wennberg, Paul O.; Wisthaler, Armin

2016-04-01

Formation of ozone and organic aerosol in continental atmospheres depends on whether isoprene emitted by vegetation is oxidized by the high-NOx pathway (where peroxy radicals react with NO) or by low-NOx pathways (where peroxy radicals react by alternate channels, mostly with HO2). We used mixed layer observations from the SEAC4RS aircraft campaign over the Southeast US to test the ability of the GEOS-Chem chemical transport model at different grid resolutions (0.25° × 0.3125°, 2° × 2.5°, 4° × 5°) to simulate this chemistry under high-isoprene, variable-NOx conditions. Observations of isoprene and NOx over the Southeast US show a negative correlation, reflecting the spatial segregation of emissions; this negative correlation is captured in the model at 0.25° × 0.3125° resolution but not at coarser resolutions. As a result, less isoprene oxidation takes place by the high-NOx pathway in the model at 0.25° × 0.3125° resolution (54 %) than at coarser resolution (59 %). The cumulative probability distribution functions (CDFs) of NOx, isoprene, and ozone concentrations show little difference across model resolutions and good agreement with observations, while formaldehyde is overestimated at coarse resolution because excessive isoprene oxidation takes place by the high-NOx pathway with high formaldehyde yield. The good agreement of simulated and observed concentration variances implies that smaller-scale non-linearities (urban and power plant plumes) are not important on the regional scale. Correlations of simulated vs. observed concentrations do not improve with grid resolution because finer modes of variability are intrinsically more difficult to capture. Higher model resolution leads to decreased conversion of NOx to organic nitrates and increased conversion to nitric acid, with total reactive nitrogen oxides (NOy) changing little across model resolutions. Model concentrations in the lower free troposphere are also insensitive to grid resolution. The overall low sensitivity of modeled concentrations to grid resolution implies that coarse resolution is adequate when modeling continental boundary layer chemistry for global applications.

Changes in growth, leaf abscission, and biomass associated with seasonal tropospheric ozone exposures of Populus tremuloides clones and seedlings

Treesearch

D.F. Karnosky; Z.E. Gagnon; R.E. Dickson; M.D. Coleman; E.H. Lee; J.G. Isebrands

1996-01-01

The effects of single-season tropospheric ozone (03) exposures on growth, leaf abscission, and biomass of trembling aspen (Populus tremuloides Michx.) rooted cuttings and seedlings were studied. Plants were grown in the Upper Peninsula of Michigan in open-top chambers with 03 exposures that ranged from...

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

NASA Technical Reports Server (NTRS)

Allen, Dale; Pickering, Kenneth; Stenchikov, Georgiy; Thompson, Anne M.; Kondo, Yutaka

1999-01-01

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 Use of a Satellite Climatological Data Set to Infer Large Scale Three Dimensional Flow Characteristics

NASA Technical Reports Server (NTRS)

Lerner, Jeffrey A.; Jedlovec, Gary J.; Atkinson, Robert J.

1998-01-01

Ever since the first satellite image loops from the 6.3 micron water vapor channel on the METEOSAT-1 in 1978, there have been numerous efforts (many to a great degree of success) to relate the water vapor radiance patterns to familiar atmospheric dynamic quantities. The realization of these efforts is becoming evident with the merging of satellite derived winds into predictive models (Velden et al., 1997; Swadley and Goerss, 1989). Another parameter that has been quantified from satellite water vapor channel measurements is upper tropospheric relative humidity (UTH) (e.g., Soden and Bretherton, 1996; Schmetz and Turpeinen, 1988). These humidity measurements, in turn, can be used to quantify upper tropospheric water vapor and its transport to more accurately diagnose climate changes (Lerner et al., 1998; Schmetz et al. 1995a) and quantify radiative processes in the upper troposphere. Also apparent in water vapor imagery animations are regions of subsiding and ascending air flow. Indeed, a component of the translated motions we observe are due to vertical velocities. The few attempts at exploiting this information have been met with a fair degree of success. Picon and Desbois (1990) statistically related Meteosat monthly mean water vapor radiances to six standard pressure levels of the European Centre for Medium Range Weather Forecast (ECMWF) model vertical velocities and found correlation coefficients of about 0.50 or less. This paper presents some preliminary results of viewing climatological satellite water vapor data in a different fashion. Specifically, we attempt to infer the three dimensional flow characteristics of the mid- to upper troposphere as portrayed by GOES VAS during the warm ENSO event (1987) and a subsequent cold period in 1998.

Temperature Trends in the Tropical Upper Troposphere and Lower Stratosphere: Connections with Sea Surface Temperatures and Implications for Water Vapor and Ozone

NASA Technical Reports Server (NTRS)

Garfinkel, C. I.; Waugh, D. W.; Oman, L. D.; Wang, L.; Hurwitz, M. M.

2013-01-01

Satellite observations and chemistry-climate model experiments are used to understand the zonal structure of tropical lower stratospheric temperature, water vapor, and ozone trends. The warming in the tropical upper troposphere over the past 30 years is strongest near the Indo-Pacific warm pool, while the warming trend in the western and central Pacific is much weaker. In the lower stratosphere, these trends are reversed: the historical cooling trend is strongest over the Indo-Pacific warm pool and is weakest in the western and central Pacific. These zonal variations are stronger than the zonal-mean response in boreal winter. Targeted experiments with a chemistry-climate model are used to demonstrate that sea surface temperature (hereafter SST) trends are driving the zonal asymmetry in upper tropospheric and lower stratospheric tropical temperature trends. Warming SSTs in the Indian Ocean and in the warm pool region have led to enhanced moist heating in the upper troposphere, and in turn to a Gill-like response that extends into the lower stratosphere. The anomalous circulation has led to zonal structure in the ozone and water vapor trends near the tropopause, and subsequently to less water vapor entering the stratosphere. The radiative impact of these changes in trace gases is smaller than the direct impact of the moist heating. Projected future SSTs appear to drive a temperature and water vapor response whose zonal structure is similar to the historical response. In the lower stratosphere, the changes in water vapor and temperature due to projected future SSTs are of similar strength to, though slightly weaker than, that due directly to projected future CO2, ozone, and methane.

Increase in upper tropospheric and lower stratospheric aerosol levels and its potential connection with Asian pollution.

PubMed

Vernier, J-P; Fairlie, T D; Natarajan, M; Wienhold, F G; Bian, J; Martinsson, B G; Crumeyrolle, S; Thomason, L W; Bedka, K M

2015-02-27

Satellite observations have shown that the Asian Summer Monsoon strongly influences the upper troposphere and lower stratosphere (UTLS) aerosol morphology through its role in the formation of the Asian Tropopause Aerosol Layer (ATAL). Stratospheric Aerosol and Gas Experiment II solar occultation and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar observations show that summertime UTLS Aerosol Optical Depth (AOD) between 13 and 18 km over Asia has increased by three times since the late 1990s. Here we present the first in situ balloon measurements of aerosol backscatter in the UTLS from Western China, which confirm high aerosol levels observed by CALIPSO since 2006. Aircraft in situ measurements suggest that aerosols at lower altitudes of the ATAL are largely composed of carbonaceous and sulfate materials (carbon/sulfur elemental ratio ranging from 2 to 10). Back trajectory analysis from Cloud-Aerosol Lidar with Orthogonal Polarization observations indicates that deep convection over the Indian subcontinent supplies the ATAL through the transport of pollution into the UTLS. Time series of deep convection occurrence, carbon monoxide, aerosol, temperature, and relative humidity suggest that secondary aerosol formation and growth in a cold, moist convective environment could play an important role in the formation of ATAL. Finally, radiative calculations show that the ATAL layer has exerted a short-term regional forcing at the top of the atmosphere of -0.1 W/m 2 in the past 18 years. Increase of summertime upper tropospheric aerosol levels over Asia since the 1990s Upper tropospheric enhancement also observed by in situ backscatter measurements Significant regional radiative forcing of -0.1 W/m 2 .

Decomposing variations of geopotential height in the troposphere and stratosphere into stationary and travelling waves

NASA Astrophysics Data System (ADS)

Guryanov, Vladimir; Eliseev, Alexey

2016-07-01

The ERA-Interim geopotential height in the Northern Hemisphere from November to March, 1992-2015 in the layer from between pressure levels 1000 mb and 1 mb is expanded into stationary and travelling zonal waves with zonal wavenumbers, k, from 1 to 10, and with periods, T, from 2 to 156 days (the so called Hayashi spectra). Among the studied waves, the largest amplitude is attained by the stationary and travelling waves with zonal wavenumber k=1 and with periods from 3 to 4 weeks in the upper stratosphere over the latitudinal belt 60-70oN. The stationary waves with k from 1 to 3 and with T from 2 to 3 weeks are most pronounced in the stratosphere. In turn, the largest amplitudes of the travelling waves with zonal wavenumbers k ≥ 5 are found in the troposphere. The dominant periods of the latter waves are about 1 week or slightly higher, and this dominant period basically decrease with increasing wavenumber. In the upper stratosphere, the eastward travelling waves generally dominate over westward ones. The only exception is the longest zonal mode with k=1, for which the amplitude of the westward travelling wave is larger than that for the eastward one. The period of the travelling waves dominating in the upper stratosphere is close to 3 weeks. In the upper troposphere, the amplitudes of the eastward waves with k from 4 to 10 is several-fold larger than those for their westward counterparts. The latter is reflected in the larger average wavenumber of the eastward travelling wave in comparison to that of the westarward one. The period of the gravest of the dominant travelling waves in the upper troposphere is close to one week, and it decreases to 2-4 days for the dominant travelling waves with k=8-10.

A Ring-‘Rain’ influence for Saturn’s Cloud Albedo and Temperatures? Evidence Pro or Con from Voyager, HST, and Cassini

NASA Astrophysics Data System (ADS)

West, Robert A.; Li, Liming

2015-11-01

J. E. P. Connerney [Geophys. Res. Lett, 13, 773-776, 1986] pointed out that ‘latitudinal variations in images of Saturn’s disk, upper atmospheric temperatures, and ionospheric electron densities are found in magnetic conjugacy with features in Saturn’s ring plane’, and proposed ‘that these latitudinal variations are the result of a variable influx of water, transported along magnetic field lines from sources in Saturn’s ring plane’. Observations of H3+ support a ring-ionosphere connection [O'Donoghue et al., Nature 496, 7444, 2013]. What about cloud albedo and temperature? Connerney attributed a hemispheric asymmetry in haze and temperature to an asymmetry in water flux and predicted that ‘the presently-observed north-south asymmetry (upper tropospheric temperatures, aerosols) will persist throughout the Saturn year’. We can now test these ideas with data from the Cassini mission, from the Hubble Space Telescope, and from ground-based observations. Analyses of ground-based images and especially Hubble data established that the hemispheric asymmetry of the aerosol population does change, and seasonal effects are dominant, although non-seasonal variations are also observed [Karkoschka and Tomasko, Icarus 179, 195-221, 2005]. Upper tropospheric temperatures also vary as expected in response to seasonal forcing [Fletcher et al., Icarus 208, 337-352, 2009]. Connerney also identified dark bands in Voyager Green-filter images on magnetic conjugacy with the E ring and edges of the A and B rings. In Cassini Green-filter images there is some correspondence between dark bands and ring features in magnetic conjugacy, but collectively the correlation is not strong. Cassini 727-nm methane band images do not suggest depletion of aerosols in the upper troposphere at ring edge magnetic conjugacy latitudes as proposed by Connerney. We conclude that ring rain does not have a significant influence on upper tropospheric aerosols and temperatures on Saturn. Part of this work was performed by the Jet Propulsion Lab, Calif. Institute of Technology.

Tropospheric Nitrogen Dioxide Column Density Trends Seen from the 10-year Record of OMI Measurements over East Asia

NASA Astrophysics Data System (ADS)

Irie, H.; Muto, T.; Itahashi, S.; Kurokawa, J. I.

2015-12-01

The Ozone Monitoring Instrument (OMI) aboard the Aura satellite recorded the 10-year (2005-2014) of tropospheric nitrogen dioxide (NO2) vertical column density (VCD) data. The data set taken over East Asia was analyzed to estimate linear trends on national and grid bases for two periods of 2005-2011 and 2011-2014. The most striking features are leveling-off or decreasing trends seen in NO2 VCDs over China for 2011-2014 after continuous increases for 2005-2011. In particular, a significant reduction by ~14% occurred from 2013 through 2014, attaining to the level of 2009. The grid-basis trend analysis implies that the turnaround seen in the trends occurred on a province or larger spatial scale and was likely due mainly to the technical improvement such as the widespread use of de-NOx units. Another prominent features are seen in Japan, where NO2 VCDs decreased at a rate of ~4% per year from 2005 to 2011. The rate was almost unchanged between the two periods 2005-2011 and 2011-2014, while the significant power substitution of thermal power generation for the nuclear power generation took place in Japan after 2011, when a massive earthquake occurred off the Pacific coast of northern Japan. This reflects a less contribution of NOx emissions from the power plant sector than that from the transport sector in the Pacific Belt Zone lying over metropolitan areas.

Evaluation of the cloud fields in the UK Met Office HadGEM3-UKCA model using the CCCM satellite data product to advance our understanding of the influence of clouds on tropospheric composition and chemistry

NASA Astrophysics Data System (ADS)

Varma, S.; Voulgarakis, A.; Liu, H.; Crawford, J. H.

2016-12-01

What drives the variability of trace gases and aerosols in the troposphere is not well understood, as is the role of clouds in modulating this variability via radiative, transport, deposition, and lightning effects that are associated with them. Such uncertainties are expected to be of particular importance in the tropical troposphere, a region that receives significant surface emissions and moisture via deep convection and upwelling, and experiences large amounts of lightning production of nitrogen oxides (NOx). Accurately simulating tropospheric composition and its variability is of utmost importance as both could have a significant effect on the region's temperature and circulation, as well as on surface climate and the amount of UV radiation in the troposphere. In this presentation, we will examine the key cloud processes which are expected to have an influence on tropospheric composition with a specific focus on their roles in modifying solar radiation and photolysis rates of trace gases through the backscattering of shortwave radiation. We will pay particular attention to the UT/LS which is less well understood and where clouds could have a significant impact due to backscattering. We will also utilize CCCM (a unique 3-D cloud data product merged from multiple A-Train satellites (CERES, CloudSat, CALIPSO, and MODIS) developed at the NASA Langley Research Center to evaluate the cloud fields and their vertical distribution in the HadGEM3-UKCA model and to adjust the cloud fields where appropriate. This evaluation will initially involve the comparison of effective cloud optical depth (ECOD) as calculated from CCCM and HadGEM3-UKCA using the approximate random overlap approximation followed by the application of 3-D scaling factors to the model's ECOD. We will then examine the impacts of the cloud field adjustment on tropospheric chemistry, with a focus on oxidants in the UT/LS.

Dynamics and Composition of the Asian Summer Monsoon Anticyclone

NASA Astrophysics Data System (ADS)

Gottschaldt, K. D.; Schlager, H.; Baumann, R.; Bozem, H.; Cai, D. S.; Eyring, V.; Hoor, P. M.; Graf, P.; Joeckel, P.; Jurkat, T.; Voigt, C.; Grewe, V.; Zahn, A.; Ziereis, H.

2017-12-01

This study places trace gas observations in the upper-tropospheric Asian summer monsoon anticyclone (ASMA) obtained with the HALO research aircraft during the ESMVal campaign into the context of regional, intra-annual variability by hindcasts with the EMAC model. The simulations demonstrate that tropospheric trace gas profiles in the monsoon season are distinct from the rest of the year. Air uplifted from the lower troposphere to the tropopause layer dominates the eastern part of the ASMA's interior, while the western part is characterized by subsidence down to the mid-troposphere. Soluble compounds are being washed out when uplifted by convection in the eastern part, where lightning simultaneously replenishes reactive nitrogen in the upper troposphere. Net photochemical ozone production is significantly enhanced in the ASMA, contrasted by an ozone depleting regime in the mid-troposphere and more neutral conditions in autumn and winter. An analysis of multiple monsoon seasons in the simulation shows that stratospherically influenced tropopause layer air is regularly entrained at the eastern ASMA flank, and then transported in the southern fringe around the interior region. Observed and simulated tracer-tracer relations reflect photochemical O3 production, as well as in-mixing from the lower troposphere and the tropopause layer. The simulation additionally shows entrainment of clean air from the equatorial region by northerly winds at the western ASMA flank. Although the in situ measurements were performed towards the end of summer, the main ingredients needed for their interpretation are present throughout the monsoon season.Subseasonal dynamical instabilities of the ASMA effectively overcome horizontal transport barriers, occur quite frequently, and are of paramount importance for the trace gas composition of the ASMA and its outflow into regions around the world.

Characterization of NOx emission in the suburbs of Tokyo based on simultaneous and real-time observations of atmospheric Ox and NOx

NASA Astrophysics Data System (ADS)

Matsumoto, J.

2013-12-01

Nitrogen oxides, NOx (NO, NO2), and volatile organic compounds, VOCs, are important as precursors of photochemical oxidants (tropospheric ozone, O3). To predict and control photochemical oxidants, NOx emission should be captured precisely. In addition, the ratio of NO2/NOx in the exhaust gas is also important as the initial balance between NO and NO2 in the atmosphere. Monitoring the NO2/NOx ratio in the exhaust gases is essential. Especially, the influence of the NOx emission on the real atmosphere should be explored. However, conversion reactions among NO, NO2 and O3 are typically in the time scale of minutes. The NO2/NOx ratio can change rapidly just after emission. Real-time observations of these compounds in the second time scale are essential. In view of photochemical oxidant, near emission sources of NO, ozone concentration can be easily perturbed by reaction with locally emitted NO. As an index of oxidant, the sum of O3 and NO2 (Ox = O3 + NO2) is useful. In this study, a simultaneous and real-time analyzer of atmospheric Ox and NOx has been developed utilizing the dual NO2 detectors based on laser-induced fluorescence technique (LIF), and characterization of NOx emission was explored through the observations of Ox and NOx in the suburbs of Tokyo. The dual LIF detectors consisted of one laser head, two LIF cells, and one common vacuum pump. As the Ox monitor, the excess NO was added to the sample and O3 was converted to NO2, and then the sum of O3 and NO2 in the sample was quantified at the 1st LIF cell. As the NOx monitor, the excess O3 was added to the sample and NO was converted to NO2, and then the sum of NO and NO2 in the sample was quantified at the 2nd LIF cell. Both the ';Ox' and ';NOx' channels in the dual LIF analyzer were simultaneously monitoring Ox and NOx in the sample air, respectively. The temporal resolution of observed data was 1 s. Typical conversion efficiencies of O3 and NO to NO2 were more than 0.98. The lower detection limits were 0.1 ppbv for Ox and 0.5 ppbv for NOx (60-s integration, S/N = 3). The observation test in the suburbs of Tokyo was conducted in April 2013 at Tokorozawa Campus, Waseda University. During the campaign, 48 cases of ';NOx spikes', for which NOx levels significantly varied in the second time scale due to local NOx emission, were captured. NO2/NOx ratio in the exhaust gas was estimated as the slope of regression line between 1-s series data of Ox and those of NOx observed during each spike. The average of acquired NO2/NOx ratio was 0.10. Thus, as a result of observations of real atmosphere, the present NO2/NOx ratio in the exhaust gases in the suburbs of Tokyo was 0.10 as average, which was mainly due to exhausts of automobiles. However, when the individual cases were considered, NO2/NOx could vary from 0.00 to 0.30. Such a wide range of NO2/NOx ratio may be due to (1) difference of source types (eg. automobiles, power generator) and (2) difference of conditions of sources (eg. engines, filters of exhaust). For example, NO2/NOx ratio for hybrid electric vehicles may be different from those for conventional cars. When diffusion of such new model cars can change NOx emission in near future, the present method of simultaneous and real-time monitoring of Ox and NOx in the atmosphere can be useful and promising for characterization of NOx emission.

AO/NAO Response to Climate Change. 1; Respective Influences of Stratospheric and Tropospheric Climate Changes

NASA Technical Reports Server (NTRS)

Rind, D.; Perlwitz, J.; Lonergan, P.

2005-01-01

We utilize the GISS Global Climate Middle Atmosphere Model and 8 different climate change experiments, many of them focused on stratospheric climate forcings, to assess the relative influence of tropospheric and stratospheric climate change on the extratropical circulation indices (Arctic Oscillation, AO; North Atlantic Oscillation, NAO). The experiments are run in two different ways: with variable sea surface temperatures (SSTs) to allow for a full tropospheric climate response, and with specified SSTs to minimize the tropospheric change. The results show that tropospheric warming (cooling) experiments and stratospheric cooling (warming) experiments produce more positive (negative) AO/NAO indices. For the typical magnitudes of tropospheric and stratospheric climate changes, the tropospheric response dominates; results are strongest when the tropospheric and stratospheric influences are producing similar phase changes. Both regions produce their effect primarily by altering wave propagation and angular momentum transports, but planetary wave energy changes accompanying tropospheric climate change are also important. Stratospheric forcing has a larger impact on the NAO than on the AO, and the angular momentum transport changes associated with it peak in the upper troposphere, affecting all wavenumbers. Tropospheric climate changes influence both the A0 and NAO with effects that extend throughout the troposphere. For both forcings there is often vertical consistency in the sign of the momentum transport changes, obscuring the difference between direct and indirect mechanisms for influencing the surface circulation.

The effects of aircraft on climate and pollution. Part II: 20-year impacts of exhaust from all commercial aircraft worldwide treated individually at the subgrid scale.

PubMed

Jacobson, M Z; Wilkerson, J T; Naiman, A D; Lele, S K

2013-01-01

This study examines the 20-year impacts of emissions from all commercial aircraft flights worldwide on climate, cloudiness, and atmospheric composition. Aircraft emissions from each individual flight worldwide were modeled to evolve from the subgrid to grid scale with the global model described and evaluated in Part I of this study. Simulations with and without aircraft emissions were run for 20 years. Aircraft emissions were found to be responsible for -6% of Arctic surface global warming to date, -1.3% of total surface global warming, and -4% of global upper tropospheric warming. Arctic warming due to aircraft slightly decreased Arctic sea ice area. Longer simulations should result in more warming due to the further increase in CO2. Aircraft increased atmospheric stability below cruise altitude and decreased it above cruise altitude. The increase in stability decreased cumulus convection in favor of increased stratiform cloudiness. Aircraft increased total cloud fraction on average. Aircraft increased surface and upper tropospheric ozone by -0.4% and -2.5%, respectively and surface and upper-tropospheric peroxyacetyl nitrate (PAN) by -0.1% and -5%, respectively. Aircraft emissions increased tropospheric OH, decreasing column CO and CH4 by -1.7% and -0.9%, respectively. Aircraft emissions increased human mortality worldwide by -620 (-240 to 4770) deaths per year, with half due to ozone and the rest to particulate matter less than 2.5 micrometers in diameter (PM2.5).

A growing threat to the ozone layer from short-lived anthropogenic chlorocarbons

NASA Astrophysics Data System (ADS)

Oram, David E.; Ashfold, Matthew J.; Laube, Johannes C.; Gooch, Lauren J.; Humphrey, Stephen; Sturges, William T.; Leedham-Elvidge, Emma; Forster, Grant L.; Harris, Neil R. P.; Mead, Mohammed Iqbal; Abu Samah, Azizan; Moi Phang, Siew; Ou-Yang, Chang-Feng; Lin, Neng-Huei; Wang, Jia-Lin; Baker, Angela K.; Brenninkmeijer, Carl A. M.; Sherry, David

2017-10-01

Large and effective reductions in emissions of long-lived ozone-depleting substance (ODS) are being achieved through the Montreal Protocol, the effectiveness of which can be seen in the declining atmospheric abundances of many ODSs. An important remaining uncertainty concerns the role of very short-lived substances (VSLSs) which, owing to their relatively short atmospheric lifetimes (less than 6 months), are not regulated under the Montreal Protocol. Recent studies have found an unexplained increase in the global tropospheric abundance of one VSLS, dichloromethane (CH2Cl2), which has increased by around 60 % over the past decade. Here we report dramatic enhancements of several chlorine-containing VSLSs (Cl-VSLSs), including CH2Cl2 and CH2ClCH2Cl (1,2-dichloroethane), observed in surface and upper-tropospheric air in East and South East Asia. Surface observations were, on occasion, an order of magnitude higher than previously reported in the marine boundary layer, whilst upper-tropospheric data were up to 3 times higher than expected. In addition, we provide further evidence of an atmospheric transport mechanism whereby substantial amounts of industrial pollution from East Asia, including these chlorinated VSLSs, can rapidly, and regularly, be transported to tropical regions of the western Pacific and subsequently uplifted to the tropical upper troposphere. This latter region is a major provider of air entering the stratosphere, and so this mechanism, in conjunction with increasing emissions of Cl-VSLSs from East Asia, could potentially slow the expected recovery of stratospheric ozone.

Annual variations of water vapor in the stratosphere and upper troposphere observed by the Stratospheric Aerosol and Gas Experiment II

NASA Technical Reports Server (NTRS)

Mccormick, M. P.; Chiou, E. W.; Mcmaster, L. R.; Chu, W. P.; Larsen, J. C.; Rind, D.; Oltmans, S.

1993-01-01

Data collected by the Stratospheric Aerosol and Gas Experiment II are presented, showing annual variations of water vapor in the stratosphere and the upper troposphere. The altitude-time cross sections of water vapor were found to exhibit annually repeatable patterns in both hemispheres, with a yearly minimum in water vapor appearing in both hemispheres at about the same time, supporting the concept of a common source for stratospheric dry air. A linear regression analysis was applied to the three-year data set to elucidate global values and variations of water vapor ratio.

A search for formic acid in the upper troposphere - A tentative identification of the 1105-per cm nu-6 band Q branch in high-resolution balloon-borne solar absorption spectra

NASA Technical Reports Server (NTRS)

Goldman, A.; Murcray, F. H.; Murcray, D. G.; Rinsland, C. P.

1984-01-01

Infrared solar absorption spectra recorded at 0.02-per cm resolution during a balloon flight from Alamogordo, NM (33 deg N), on March 23, 1981, have been analyzed for the possible presence of absorption by formic acid (HCOOH). An absorption feature at 1105 per cm has been tentatively identified in upper tropospheric spectra as due to the nu-6 band Q branch. A preliminary analysis indicates a concentration of about 0.6 ppbv and 0.4 ppbv near 8 and 10 km, respectively.

The nature of large-scale turbulence in the Jovian atmosphere

NASA Technical Reports Server (NTRS)

Mitchell, J. L.

1982-01-01

The energetics and spectral characteristis of quasi-geostrophic turbulence in Jupiter's atmosphere are examined using sequences of Voyager images and infrared temperature soundings. Using global wind measurements momentum transports associated with zonally symmetric stresses and turbulent stresses are quantified. Though a strong up-gradient flux of momentum by eddies was observed, measurements do not preclude the possibility that symmetric stresses play a critical role in maintaining the mean zonal circulation. Strong correlation between the observed meridional distribution of eddy-scale kinetic energy and available potential energy suggests coupling between the observed cloudtop turbulent motions and the upper tropospheric thermodynamics. An Oort energy budget for Jupiter's upper troposphere is formulated.

Impact of convection on stratospheric humidity and upper tropospheric clouds

NASA Astrophysics Data System (ADS)

Ueyama, R.; Schoeberl, M. R.; Jensen, E. J.; Pfister, L.; Avery, M. A.

2017-12-01

The role of convection on stratospheric water vapor and upper tropospheric cloud fraction is investigated using two sets of complementary transport and microphysical models driven by MERRA-2 and ERA-Interim meteorological analyses: (1) computationally efficient ensembles of forward trajectories with simplified cloud microphysics, and (2) one-dimensional simulations with detailed microphysics along back trajectories. Convective influence along the trajectories is diagnosed based on TRMM/GPM rainfall products and geostationary infrared satellite cloud-top measurements, with convective cloud-top height adjusted to match the CloudSat, CALIPSO, and CATS measurements. We evaluate and constrain the model results by comparison with satellite observations (e.g., Aura MLS, CALIPSO CALIOP) and high-altitude aircraft campaigns (e.g., ATTREX, POSIDON). Convection moistens the lower stratosphere by approximately 10-15% and increases the cloud fraction in the upper troposphere by 35-50%. Convective moistening is dominated by the saturating effect of parcels; convectively-lofted ice has a negligible impact on lower stratospheric humidity. We also find that the highest convective clouds have a disproportionately large impact on stratospheric water vapor because stratospheric relative humidity is low. Implications of these model results on the role of convection on present and future climate will be discussed.

Estimation of the global climate effect of brown carbon

NASA Astrophysics Data System (ADS)

Zhang, A.; Wang, Y.; Zhang, Y.; Weber, R. J.; Song, Y.

2017-12-01

Carbonaceous aerosols significantly affect global radiative forcing and climate through absorption and scattering of sunlight. Black carbon (BC) and brown carbon (BrC) are light-absorbing carbonaceous aerosols. The global distribution and climate effect of BrC is uncertain. A recent study suggests that BrC absorption is comparable to BC in the upper troposphere over biomass burning region and that the resulting heating tends to stabilize the atmosphere. Yet current climate models do not include proper treatments of BrC. In this study, we derived a BrC global biomass burning emission inventory from Global Fire Emissions Database 4 (GFED4) and developed a BrC module in the Community Atmosphere Model version 5 (CAM5) of Community Earth System Model (CESM) model. The model simulations compared well to BrC observations of the Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) and Deep Convective Clouds and Chemistry Project (DC-3) campaigns and includes BrC bleaching. Model results suggested that BrC in the upper troposphere due to convective transport is as important an absorber as BC globally. Upper tropospheric BrC radiative forcing is particularly significant over the tropics, affecting the atmosphere stability and Hadley circulation.

Comparing upper tropospheric humidity data from microwave satellite instruments and tropical radiosondes

NASA Astrophysics Data System (ADS)

Moradi, Isaac; Buehler, Stefan A.; John, Viju O.; Eliasson, Salomon

2010-12-01

Atmospheric humidity plays an important role in the Earth's climate. Microwave satellite data provide valuable humidity observations in the upper troposphere with global coverage. In this study, we compare upper tropospheric humidity (UTH) retrieved from the Advanced Microwave Sounding Unit and the Microwave Humidity Sounder against radiosonde data measured at four of the central facilities of the Atmospheric Radiation Measurement program. The Atmospheric Radiative Transfer Simulator (ARTS) was used to simulate satellite brightness temperatures from the radiosonde profiles. Strong ice clouds were filtered out, as their influence on microwave measurements leads to incorrect UTH values. Day and night radiosonde profiles were analyzed separately to take into account the radiosonde radiation bias. The comparison between radiosonde and satellite is most meaningful for data in cloud-free, nighttime conditions and with a time difference of less than 2 hr. We found good agreement between the two data sets. The satellite data were slightly moister than the radiosonde data, with a mean difference of 1%-2.3% relative humidity (RH), depending on the radiosonde site. Monthly gridded data were also compared and showed a slightly larger mean difference of up to 3.3% RH, which can be explained by sampling issues.

Correction Technique for Raman Water Vapor Lidar Signal-Dependent Bias and Suitability for Water Wapor Trend Monitoring in the Upper Troposphere

NASA Technical Reports Server (NTRS)

Whiteman, D. N.; Cadirola, M.; Venable, D.; Calhoun, M.; Miloshevich, L; Vermeesch, K.; Twigg, L.; Dirisu, A.; Hurst, D.; Hall, E.;

Characterization of Upper-Troposphere Water Vapor Measurements during AFWEX Using LASE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ferrare, Richard; Browell, E. V.; Ismail, S.

Water vapor profiles from NASA's Lidar Atmospheric Sensing Experiment (LASE) system acquired during the ARM/FIRE Water Vapor Experiment (AFWEX) are used to characterize upper troposphere water vapor (UTWV) measured by ground-based Raman lidars, radiosondes, and in situ aircraft sensors over the Department of Energy Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site in northern Oklahoma. LASE was deployed from the NASA DC-8 aircraft and measured water vapor over the ARM SGP Central Facility (CF) site during seven flights between November 27 and December 10, 2000. Initially, the DOE ARM SGP Cloud and Radiation Testbed (CART) Raman lidar (CARL) UTWVmore » profiles were about 5-7% wetter than LASE in the upper troposphere, and the Vaisala RS80-H radiosonde profiles were about 10% drier than LASE between 8-12 km. Scaling the Vaisala water vapor profiles to match the precipitable water vapor (PWV) measured by the ARM SGP microwave radiometer (MWR) did not change these results significantly. By accounting for an overlap correction of the CARL water vapor profiles and by employing schemes designed to correct the Vaisala RS80-H calibration method and account for the time response of the Vaisala RS80H water vapor sensor, the average differences between the CARL and Vaisala radiosonde upper troposphere water vapor profiles are reduced to about 5%, which is within the ARM goal of mean differences of less than 10%. The LASE and DC-8 in situ Diode Laser Hygrometer (DLH) UTWV measurements generally agreed to within about 3 to 4%. The DC-8 in situ frost point cryogenic hygrometer and Snow White chilled mirror measurements were drier than the LASE, Raman lidars, and corrected Vaisala RS80H measurements by about 10-25% and 10-15%, respectively. Sippican (formerly VIZ manufacturing) carbon hygristor radiosondes exhibited large variabilities and poor agreement with the other measurements. PWV derived from the LASE profiles agreed to within about 3% on average with PWV derived from the ARM SGP microwave radiometer. The agreement between the LASE and MWR PWV and the LASE and CARL UTWV measurements supports the hypotheses that MWR measurements of the 22 GHz water vapor line can accurately constrain the total water vapor amount and that the CART Raman lidar, when calibrated using the MWR PWV, can provide an accurate, stable reference for characterizing upper troposphere water vapor.« less

The life-cycle of upper-tropospheric jet streams identified with a novel data segmentation algorithm

NASA Astrophysics Data System (ADS)

Limbach, S.; Schömer, E.; Wernli, H.

2010-09-01

Jet streams are prominent features of the upper-tropospheric atmospheric flow. Through the thermal wind relationship these regions with intense horizontal wind speed (typically larger than 30 m/s) are associated with pronounced baroclinicity, i.e., with regions where extratropical cyclones develop due to baroclinic instability processes. Individual jet streams are non-stationary elongated features that can extend over more than 2000 km in the along-flow and 200-500 km in the across-flow direction, respectively. Their lifetime can vary between a few days and several weeks. In recent years, feature-based algorithms have been developed that allow compiling synoptic climatologies and typologies of upper-tropospheric jet streams based upon objective selection criteria and climatological reanalysis datasets. In this study a novel algorithm to efficiently identify jet streams using an extended region-growing segmentation approach is introduced. This algorithm iterates over a 4-dimensional field of horizontal wind speed from ECMWF analyses and decides at each grid point whether all prerequisites for a jet stream are met. In a single pass the algorithm keeps track of all adjacencies of these grid points and creates the 4-dimensional connected segments associated with each jet stream. In addition to the detection of these sets of connected grid points, the algorithm analyzes the development over time of the distinct 3-dimensional features each segment consists of. Important events in the development of these features, for example mergings and splittings, are detected and analyzed on a per-grid-point and per-feature basis. The output of the algorithm consists of the actual sets of grid-points augmented with information about the particular events, and of the so-called event graphs, which are an abstract representation of the distinct 3-dimensional features and events of each segment. This technique provides comprehensive information about the frequency of upper-tropospheric jet streams, their preferred regions of genesis, merging, splitting, and lysis, and statistical information about their size, amplitude and lifetime. The presentation will introduce the technique, provide example visualizations of the time evolution of the identified 3-dimensional jet stream features, and present results from a first multi-month "climatology" of upper-tropospheric jets. In the future, the technique can be applied to longer datasets, for instance reanalyses and output from global climate model simulations - and provide detailed information about key characteristics of jet stream life cycles.

Overview of the summer 2004 Intercontinental Chemical Transport Experiment-North America (INTEX-A)

NASA Astrophysics Data System (ADS)

Singh, H. B.; Brune, W. H.; Crawford, J. H.; Jacob, D. J.; Russell, P. B.

2006-12-01

The INTEX-A field mission was conducted in the summer of 2004 (1 July to 15 August 2004) over North America (NA) and the Atlantic in cooperation with multiple national and international partners as part of a consortium called ICARTT. The main goals of INTEX-A were to (1) characterize the composition of the troposphere over NA, (2) characterize the outflow of pollution from NA and determine its chemical evolution during transatlantic transport, (3) validate satellite observations of tropospheric composition, (4) quantitatively relate atmospheric concentrations of gases and aerosols with their sources and sinks, and (5) investigate aerosol properties and their radiative effects. INTEX-A primarily relied on instrumented DC-8 and J-31 aircraft platforms to achieve its objectives. The DC-8 was equipped to measure detailed gas and aerosol composition and provided sufficient range and altitude capability to coordinate activities with distant partners and to sample the entire midlatitude troposphere. The J-31 was specifically focused on radiative effects of clouds and aerosols and operated largely in the Gulf of Maine. Satellite products along with meteorological and 3-D chemical transport model forecasts were integrated into the flight planning process. Intercomparisons were performed to quantify the accuracy of data and to create a unified data set. Satellite validation activities principally focused on Terra (MOPITT, MODIS, and MISR), Aqua (AIRS and MODIS) and Envisat (SCIAMACHY) to validate observations of CO, NO2, HCHO, H2O, and aerosol. Persistent fires in Alaska and NW Canada offered opportunities to quantify emissions from fires and study the transport and evolution of biomass burning plumes. Contrary to expectations, several pollution plumes of Asian origin, frequently mixed with stratospheric air, were sampled over NA. Quasi-Lagrangian sampling was successfully carried out to study chemical aging of plumes during transport over the Atlantic. Lightning NOx source was found to be far larger than anticipated and provided a major source of error in model simulations. The composition of the upper troposphere was significantly perturbed by influences from surface pollution and lightning. Drawdown of CO2 was characterized over NA and its atmospheric abundance related to terrestrial sources and sinks. INTEX-A observations provide a comprehensive data set to test models and evaluate major pathways of pollution transport over NA and the Atlantic. This overview provides a context within which the present and future INTEX-A/ICARTT publications can be understood.

Role of atmospheric heating over the South China Sea and western Pacific regions in modulating Asian summer climate under the global warming background

NASA Astrophysics Data System (ADS)

He, Bian; Yang, Song; Li, Zhenning

2016-05-01

The response of monsoon precipitation to global warming, which is one of the most significant climate change signals at the earth's surface, exhibits very distinct regional features, especially over the South China Sea (SCS) and adjacent regions in boreal summer. To understand the possible atmospheric dynamics in these specific regions under the global warming background, changes in atmospheric heating and their possible influences on Asian summer climate are investigated by both observational diagnosis and numerical simulations. Results indicate that heating in the middle troposphere has intensified in the SCS and western Pacific regions in boreal summer, accompanied by increased precipitation, cloud cover, and lower-tropospheric convergence and decreased sea level pressure. Sensitivity experiments show that middle and upper tropospheric heating causes an east-west feedback pattern between SCS and western Pacific and continental South Asia, which strengthens the South Asian High in the upper troposphere and moist convergence in the lower troposphere, consequently forcing a descending motion and adiabatic warming over continental South Asia. When air-sea interaction is considered, the simulation results are overall more similar to observations, and in particular the bias of precipitation over the Indian Ocean simulated by AGCMs has been reduced. The result highlights the important role of air-sea interaction in understanding the changes in Asian climate.

Coordinated profiling of stratospheric intrusions and transported pollution by the Tropospheric Ozone Lidar Network (TOLNet) and NASA Alpha Jet experiment (AJAX): Observations and comparison to HYSPLIT, RAQMS, and FLEXPART

NASA Astrophysics Data System (ADS)

Langford, A. O.; Alvarez, R. J.; Brioude, J.; Evan, S.; Iraci, L. T.; Kirgis, G.; Kuang, S.; Leblanc, T.; Newchurch, M. J.; Pierce, R. B.; Senff, C. J.; Yates, E. L.

2018-02-01

Ground-based lidars and ozonesondes belonging to the NASA-supported Tropospheric Ozone Lidar Network (TOLNet) are used in conjunction with the NASA Alpha Jet Atmospheric eXperiment (AJAX) to investigate the transport of stratospheric ozone and entrained pollution into the lower troposphere above the United States on May 24-25, 2013. TOLNet and AJAX measurements made in California, Nevada, and Alabama are compared to tropospheric ozone retrievals from the Atmospheric Infrared Sounder (AIRS), to back trajectories from the NOAA Air Resources Laboratory (ARL) Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model, and to analyses from the NOAA/NESDIS Real-time Air Quality Modeling System (RAQMS) and FLEXPART particle dispersion model. The measurements and model analyses show much deeper descent of ozone-rich upper tropospheric/lower stratospheric air above the Desert Southwest than above the Southeast, and comparisons to surface measurements from regulatory monitors reporting to the U.S. EPA Air Quality System (AQS) suggest that there was a much greater surface impact in the Southwest including exceedances of the 2008 National Ambient Air Quality Standard (NAAQS) of 0.075 ppm in both Southern California and Nevada. Our analysis demonstrates the potential benefits to be gained by supplementing the existing surface ozone network with coordinated upper air observations by TOLNet.

On the variability of tropospheric ozone in the Tropical Eastern Pacific and its impact on the oxidizing capacity

NASA Astrophysics Data System (ADS)

Saiz-Lopez, A.; Gomez Martin, J.; Hay, T.; Mahajan, A.; Ordoñez, C.; Parrondo Sempere, M.; Gil, M. J.; Agama Reyes, M.; Paredes Mora, J.; Voemel, H.

2012-12-01

Observations of surface ozone, NOx and meteorological variables were made during two ground based field campaigns in the Eastern Pacific marine boundary layer (MBL). The first study was PIQUERO (Primera Investigación de la Química, Evolución y Reparto de Ozono), running from September 2000 to July 2001 in parallel to the Southern Hemisphere ADditional OZonesondes (SHADOZ) in the Galápagos Islands. The second study is the Climate and HAlogen Reactivity tropicaL EXperiment (CHARLEX), running from September 2010 to present. These long-term, high frequency, measurements enable a detailed description of the daily, monthly, seasonal and interannual variability of ozone and help to constrain the MBL and lower free troposphere (FT) ozone budget. In the Equatorial Eastern Pacific "cold season" (August - October), net ozone photochemical destruction of ~ 2 ppb day-1 occurs in the MBL (~30% due to halogens, and the rest to HOx). Ozone recovers by entrainment from aloft at night. The monthly baseline is set by the tropical instability waves (TIW), which also impact the ozone concentration in the lower FT. In the cold phase of the TIWs the MBL is stratified and, apart from higher surface ozone, it may also contain an upper drier layer with higher ozone between ~ 500 m and the main inversion at ~1 km. In the warm phase the buoyant MBL expands upwards (as much as 500 m) and poor ozone air reaches the FT. As the system shifts to the warm season (February- April), the TIWs stop and the sea becomes warmer, increasing evaporation and reducing ozone. The inversion is pushed upwards and finally disappears or becomes very weak. Surface ozone is so low that even at the low background NOx levels observed ozone production balances photochemical destruction, so the daily profile is flat (observed local effects in the populated areas of Galapagos are discussed). In February Galapagos is almost in the doldrums because the Inter-Tropical Convergence Zone (ITCZ) shifts south. In this situation, air convected at the ITZC is advected at different heights in the FT over Galapagos, so the entrainment of air from the FT does not replenish MBL ozone, explaining the low seasonal minimum. An important aspect of the marked ozone seasonal cycle is the impact on OH. levels. The consequences of this for the oxidizing capacity of the lower atmosphere are discussed.

The Relative Importance of Random Error and Observation Frequency in Detecting Trends in Upper Tropospheric Water Vapor

NASA Technical Reports Server (NTRS)

Whiteman, David N.; Vermeesch, Kevin C.; Oman, Luke D.; Weatherhead, Elizabeth C.

2011-01-01

Recent published work assessed the amount of time to detect trends in atmospheric water vapor over the coming century. We address the same question and conclude that under the most optimistic scenarios and assuming perfect data (i.e., observations with no measurement uncertainty) the time to detect trends will be at least 12 years at approximately 200 hPa in the upper troposphere. Our times to detect trends are therefore shorter than those recently reported and this difference is affected by data sources used, method of processing the data, geographic location and pressure level in the atmosphere where the analyses were performed. We then consider the question of how instrumental uncertainty plays into the assessment of time to detect trends. We conclude that due to the high natural variability in atmospheric water vapor, the amount of time to detect trends in the upper troposphere is relatively insensitive to instrumental random uncertainty and that it is much more important to increase the frequency of measurement than to decrease the random error in the measurement. This is put in the context of international networks such as the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) and the Network for the Detection of Atmospheric Composition Change (NDACC) that are tasked with developing time series of climate quality water vapor data.

The relative importance of random error and observation frequency in detecting trends in upper tropospheric water vapor

NASA Astrophysics Data System (ADS)

Whiteman, David N.; Vermeesch, Kevin C.; Oman, Luke D.; Weatherhead, Elizabeth C.

2011-11-01

Recent published work assessed the amount of time to detect trends in atmospheric water vapor over the coming century. We address the same question and conclude that under the most optimistic scenarios and assuming perfect data (i.e., observations with no measurement uncertainty) the time to detect trends will be at least 12 years at approximately 200 hPa in the upper troposphere. Our times to detect trends are therefore shorter than those recently reported and this difference is affected by data sources used, method of processing the data, geographic location and pressure level in the atmosphere where the analyses were performed. We then consider the question of how instrumental uncertainty plays into the assessment of time to detect trends. We conclude that due to the high natural variability in atmospheric water vapor, the amount of time to detect trends in the upper troposphere is relatively insensitive to instrumental random uncertainty and that it is much more important to increase the frequency of measurement than to decrease the random error in the measurement. This is put in the context of international networks such as the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) and the Network for the Detection of Atmospheric Composition Change (NDACC) that are tasked with developing time series of climate quality water vapor data.

The EOS Aura Mission

NASA Technical Reports Server (NTRS)

Schoeberl, Mark R.; Douglass, A. R.; Hilsenrath, E.; Luce, M.; Barnett, J.; Beer, R.; Waters, J.; Gille, J.; Levelt, P. F.; DeCola, P.;

Clouds and Water Vapor in the Climate System: Remotely Piloted Aircraft and Satellites

NASA Technical Reports Server (NTRS)

Anderson, James G.

1999-01-01

The objective of this work was to attack unanswered questions that lie at the intersection of radiation, dynamics, chemistry and climate. Considerable emphasis was placed on scientific collaboration and the innovative development of instruments required to address these scientific issues. The specific questions addressed include: Water vapor distribution in the Tropical Troposphere: An understanding of the mechanisms that dictate the distribution of water vapor in the middle-upper troposphere; Atmospheric Radiation: In the spectral region between 200 and 600/cm that encompasses the water vapor rotational and continuum structure, where most of the radiative cooling of the upper troposphere occurs, there is a critical need to test radiative transfer calculations using accurate, spectrally resolved radiance observations of the cold atmosphere obtained simultaneously with in situ species concentrations; Thin Cirrus: Cirrus clouds play a central role in the energy and water budgets of the tropical tropopause region; Stratosphere-Troposphere Exchange: Assessment of our ability to predict the behavior of the atmosphere to changes in the boundary conditions defined by thermal, chemical or biological variables; Correlative Science with Satellite Observations: Linking this research to the developing series of EOS observations is critical for scientific progress.

The Plunger Hypothesis: an overview of a new theory of stratosphere-troposphere dynamic coupling

NASA Astrophysics Data System (ADS)

Clark, S.; Baldwin, M. P.; Stephenson, D.

2015-12-01

I will demonstrate the advantages of a new method of quantifying polar stratosphere-troposphere coupling by considering large-scale movements of mass into and out of the polar stratosphere. This project aims to use these mass movements to explain pressure and temperature anomalies throughout the polar troposphere and lower stratosphere in the aftermath of extreme stratospheric events. We hypothesise that these mass movements are induced by deposition of momentum by breaking waves in the stratosphere, slowing the wintertime polar vortex, and so are associated with sudden stratospheric warmings (SSWs). Such a mass movement in the upper stratosphere acts to compress the polar atmosphere below it in the manner of a plunger. In this way the pressure anomaly in the upper polar stratosphere 'controls' the pressure and temperature anomalies below by adiabatic compression of the polar atmospheric column. Better understanding this method of control will allow us to use stratospheric data to improve medium-range forecasting ability in the troposphere. One of the key innovations featured in this project is considering pressure and temperature fields at fixed geopotential surfaces, allowing for the easy observation of mass movement into and out of a polar cap region (which we have defined as north of 65N) as a function of altitude. Reanalysis data considered in this manner demonstrates a relationship between tropospheric pressure anomalies and stratospheric anomalies in the polar cap, and so a way to predict tropospheric variability given stratospheric information. This work forms part of a three and a half year PhD project.

Simulations of the effect of a warmer climate on atmospheric humidity

NASA Technical Reports Server (NTRS)

Del Genio, Anthony D.; Lacis, Andrew A.; Ruedy, Reto A.

1991-01-01

Increases in the concentration of water vapor constitute the single largest positive feedback in models of global climate warming caused by greenhouse gases. It has been suggested that sinking air in the regions surrounding deep cumulus clouds will dry the upper troposphere and eliminate or reverse the direction of water vapor feedback. This hypothesis has been tested by performing an idealized simulation of climate change with two different versions of a climate model which both incorporate drying due to subsidence of clear air but differ in their parameterization of moist convection and stratiform clouds. Despite increased drying of the upper troposphere by cumulus clouds, upper-level humidity increases in the warmer climate because of enhanced upward moisture transport by the general circulation and increased accumulation of water vapor and ice at cumulus cloud tops.

Effects of Subsonic Aircraft on Aerosols and Cloudiness in the Upper Troposphere and Lower Stratosphere

NASA Technical Reports Server (NTRS)

Detwiler, Andrew G.

1997-01-01

This work was accomplished primarily by Allison G. Wozniak, a graduate research assistant who has completed the Master of Science in Meteorology program at the South Dakota School of Mines and Technology. Ms. Wozniak was guided and assisted in her work by L. R. Johnson and the principal investigator. Invaluable guidance was supplied by Dr. James Holdeman, NASA Lewis, the manager of the Global Atmospheric Sampling Program (GASP). Dr. Gregory Nastrom, St. Cloud (Minnesota) State University, who has used the GASP data set to provide unique views of the distribution of ozone, clouds, and atmospheric waves and turbulence, in the upper troposphere/lower stratosphere region, was also extremely helpful. Finally, Dr. Terry Deshler, University of Wyoming, supplied observations from the university's upper atmospheric monitoring program for comparison to GASP data.

Scientific issues in the design of metrics for inclusion of oxides of nitrogen in global climate agreements

PubMed Central

Shine, K. P.; Berntsen, T. K.; Fuglestvedt, J. S.; Sausen, R.

2005-01-01

The Kyoto Protocol seeks to limit emissions of various greenhouse gases but excludes short-lived species and their precursors even though they cause a significant climate forcing. We explore the difficulties that are faced when designing metrics to compare the climate impact of emissions of oxides of nitrogen (NOx) with other emissions. There are two dimensions to this difficulty. The first concerns the definition of a metric that satisfactorily accounts for its climate impact. NOx emissions increase tropospheric ozone, but this increase and the resulting climate forcing depend strongly on the location of the emissions, with low-latitude emissions having a larger impact. NOx emissions also decrease methane concentrations, causing a global-mean radiative forcing similar in size but opposite in sign to the ozone forcing. The second dimension of difficulty concerns the intermodel differences in the values of computed metrics. We explore the use of indicators that could lead to metrics that, instead of using global-mean inputs, are computed locally and then averaged globally. These local metrics may depend less on cancellation in the global mean; the possibilities presented here seem more robust to model uncertainty, although their applicability depends on the poorly known relationship between local climate change and its societal/ecological impact. If it becomes a political imperative to include NOx emissions in future climate agreements, policy makers will be faced with difficult choices in selecting an appropriate metric. PMID:16243971

Scientific issues in the design of metrics for inclusion of oxides of nitrogen in global climate agreements.

PubMed

Shine, K P; Berntsen, T K; Fuglestvedt, J S; Sausen, R

2005-11-01

The Kyoto Protocol seeks to limit emissions of various greenhouse gases but excludes short-lived species and their precursors even though they cause a significant climate forcing. We explore the difficulties that are faced when designing metrics to compare the climate impact of emissions of oxides of nitrogen (NO(x)) with other emissions. There are two dimensions to this difficulty. The first concerns the definition of a metric that satisfactorily accounts for its climate impact. NO(x) emissions increase tropospheric ozone, but this increase and the resulting climate forcing depend strongly on the location of the emissions, with low-latitude emissions having a larger impact. NO(x) emissions also decrease methane concentrations, causing a global-mean radiative forcing similar in size but opposite in sign to the ozone forcing. The second dimension of difficulty concerns the intermodel differences in the values of computed metrics. We explore the use of indicators that could lead to metrics that, instead of using global-mean inputs, are computed locally and then averaged globally. These local metrics may depend less on cancellation in the global mean; the possibilities presented here seem more robust to model uncertainty, although their applicability depends on the poorly known relationship between local climate change and its societal/ecological impact. If it becomes a political imperative to include NO(x) emissions in future climate agreements, policy makers will be faced with difficult choices in selecting an appropriate metric.

Secondary organic aerosol formation from isoprene photooxidation

NASA Astrophysics Data System (ADS)

Kroll, J. H.; Ng, N. L.; Murphy, S. M.; Flagan, R. C.; Seinfeld, J. H.

2005-12-01

We report chamber studies of the formation of secondary organic aerosol (SOA) from the oxidation of isoprene (2-methyl-1,3-butadiene). Isoprene is the most abundant non-methane hydrocarbon emitted into the troposphere (source strength of ~500 Tg/year), so even small SOA yields may have a large impact on global SOA production. Reactions are carried out in Caltech's dual 28 m3 Teflon chambers, and aerosol growth is monitored by a differential mobility analyzer (DMA) and an Aerodyne time-of-flight aerosol mass spectrometer (AMS). Isoprene oxidation is initiated by the UV irradiation of isoprene in the presence of hydrogen peroxide, with NO added for high-NOx experiments. These conditions ensure that isoprene oxidation is initiated by reaction with the OH radical, with negligible interference from other oxidants (ozone, nitrate radicals, and O atoms). Aerosol growth is observed under both high-NOx and low-NOx conditions, at isoprene concentrations lower than measured in previous studies (down to 8 ppb). SOA yields are found to be in the range of 1-2%. Yields exhibit a complex dependence on NOx concentration, likely a result of changes in the chemistry of organic peroxy radicals. It is shown that condensable compounds are formed from further reactions of first-generation isoprene oxidation products; the rates and products of such gas-phase reactions are at present poorly understood. Additionally, measurements of SOA composition indicate that these products undergo reactions in the aerosol phase, leading to the formation of low-volatility oligomeric products.

Emissions and transport of NOx over East Asia diagnosed by satellite and in-situ observations and chemical transport model results

NASA Astrophysics Data System (ADS)

Lee, H.; Kim, S.; Brioude, J.; Cooper, O. R.; Frost, G. J.; Trainer, M.; Kim, C.

2012-12-01

Nitrogen dioxide (NO2) columns observed from space have been useful in detecting the increase of NOx emissions over East Asia in accordance with rapid growth in its economy. In addition to emissions, transport can be an important factor to determine the observed satellite NO2 columns in this region. Satellite tropospheric NO2 columns showed maximum in winter and minimum in summer over the high emission areas in China, as lifetime of NO2 decreases with increase of sunlight. However, secondary peaks in the satellite NO2 columns were found in spring in both Korea and Japan, which may be influenced by transport of NOx within East Asia. Surface in-situ observations confirm the findings from the satellite measurements. The large-scale distribution of satellite NO2 columns over East Asia and the Pacific Ocean showed that the locations of NO2 column maxima coincided with wind convergence zones that change with seasons. In spring, the convergence zone is located over 30-40°N, leading to the most efficient transport of the emissions from southern China to downwind areas including Korea, Japan, and western coastal regions of the United States. We employed a Lagrangian particle dispersion model to identify the sources of the observed springtime maximum NO2. In order to understand chemical processing during the transport and quantify the roles of emissions and transport in local NOx budgets, we will also present the results from a regional chemical transport model.

Investigation of Isomer-specific Sinks of Isoprene Oxidation Products in varying NOx Environments

NASA Astrophysics Data System (ADS)

Vasquez, K.; Allen, H.; Xu, L.; Nölscher, A. C.; Praske, E.; Bates, K. H.; Crounse, J. D.; Wennberg, P. O.

2017-12-01

Isoprene is the dominant non-methane hydrocarbon emitted into the atmosphere. Its large emissions and rapid rate coefficient with OH leads to a large role in the oxidative chemistry of the atmosphere. This is primarily due to the formation of its six isomeric isoprene peroxy radicals (ISOPO2) whose individual fates are critical in controlling local and regional concentrations of important atmospheric species. Though much insight has been gained about ISOPO2 chemistry through the observation of isoprene's oxidation products, our inability to distinguish between the individual isomers of these compounds have limited our ability to diagnose the photochemistry and its impact on secondary organic aerosol, NOx and tropospheric ozone. We have developed a field-hardened high resolution chemical ionization mass spectrometer coupled with a low-pressure gas chromatograph (GC-CIMS) that is capable of observing in situ isomer distributions of a wide range of atmospheric species. Its first deployment during the PROPHET 2016 campaign yielded promising results, providing insights into the atmospheric fate of species such as the isoprene hydroxy nitrates (ISOPN) in a low NOx environment. During summer 2017, deployment of the GC-CIMS at the Caltech campus in Pasadena, CA provided a valuable contrast to the PROPHET data set, showing the isomeric distributions of oxidation products in a high NOx, urban environment. Together these two data sets allow us to better understand the drivers of isoprene chemistry and lead to more quantitative description of isoprene oxidative chemistry.

Tropospheric Diagnostic Modeling Studies of PEM-Tropics B Field Data: Investigation of the HOx/NOx/O3 Photochemical System and its Coupling to Sulfur Chemistry

NASA Technical Reports Server (NTRS)

Davis, Douglas D.

2001-01-01

Over the time period of this NASA grant the PI has helped plan and execute the PEM-Tropics B field program. He has also helped organize and co-chair two data workshops which have focused on the detailed analysis of PEM-Tropics B data. His direct participation in these analyses has led to his involvement in 13 manuscripts, nine of which are in print, two in press, and two submitted. A complete list of papers is given.

On the structure of climate variability near the tropopause and its relationship to equatorial planetary waves

NASA Astrophysics Data System (ADS)

Grise, Kevin M.

The tropopause is an important interface in the climate system, separating the unique dynamical, chemical, and radiative regimes of the troposphere and stratosphere. Previous studies have demonstrated that the long-term mean structure and variability of the tropopause results from a complex interaction of stratospheric and tropospheric processes. This project provides new insight into the processes involved in the global tropopause region through two perspectives: (1) a high vertical resolution climatology of static stability and (2) an observational analysis of equatorial planetary waves. High vertical resolution global positioning system radio occultation profiles are used to document fine-scale features of the global static stability field near the tropopause. Consistent with previous studies, a region of enhanced static stability, known as the tropopause inversion layer (TIL), exists in a narrow layer above the extratropical tropopause and is strongest over polar regions during summer. However, in the tropics, the TIL possesses a unique horizontally and vertically varying structure with maxima located at ˜17 and ˜19 km. The upper feature peaks during boreal winter and has its largest magnitude between 10º and 15º latitude in both hemispheres; the lower feature exhibits a weaker seasonal cycle and is centered at the Equator. The spatial structure of both features resembles the equatorial planetary wave response to the climatological distribution of deep convection. Equatorial planetary waves not only dominate the climatological-mean general circulation near the tropical tropopause but also play an important role in its intraseasonal and interannual variability. The structure of the equatorial planetary waves emerges as the leading pattern of variability of the zonally asymmetric tropical atmospheric circulation. Regressions on an index of the equatorial planetary waves reveal that they are associated with a distinct pattern of equatorially symmetric climate variability characterized by variations in: (1) the distribution of convection in the deep tropics; (2) the eddy momentum flux convergence and the zonal-mean zonal wind in the tropical upper troposphere; (3) the mean meridional circulation of the tropical and subtropical troposphere; (4) temperatures in the tropical upper troposphere, the tropical lower stratosphere, and the subtropical troposphere of both hemispheres; and (5) the amplitude of the upper tropospheric anticyclones that straddle the Equator over the western tropical Pacific Ocean. The pulsation of the equatorial planetary waves in time provides a framework for interpreting a broad range of climate phenomena. Variability in the equatorial planetary waves is associated with variability in the tropical TIL and is linked to both the El Nino-Southern Oscillation and the Madden-Julian Oscillation (MJO). Evidence is presented that suggests that the MJO can be viewed as the linear superposition of: (1) the pulsation of the equatorial planetary waves at a fixed location and (2) a propagating component. Variability in the equatorial planetary waves may also contribute to variability in troposphere/stratosphere exchange and the width of the tropical belt.

NOx emission estimates during the 2014 Youth Olympic Games in Nanjing

NASA Astrophysics Data System (ADS)

Ding, J.; van der A, R. J.; Mijling, B.; Levelt, P. F.; Hao, N.

2015-08-01

The Nanjing Government applied temporary environmental regulations to guarantee good air quality during the Youth Olympic Games (YOG) in 2014. We study the effect of those regulations by applying the emission estimate algorithm DECSO (Daily Emission estimates Constrained by Satellite Observations) to measurements of the Ozone Monitoring Instrument (OMI). We improved DECSO by updating the chemical transport model CHIMERE from v2006 to v2013 and by adding an Observation minus Forecast (OmF) criterion to filter outlying satellite retrievals due to high aerosol concentrations. The comparison of model results with both ground and satellite observations indicates that CHIMERE v2013 is better performing than CHIMERE v2006. After filtering the satellite observations with high aerosol loads that were leading to large OmF values, unrealistic jumps in the emission estimates are removed. Despite the cloudy conditions during the YOG we could still see a decrease of tropospheric NO2 column concentrations of about 32 % in the OMI observations when compared to the average NO2 columns from 2005 to 2012. The results of the improved DECSO algorithm for NOx emissions show a reduction of at least 25 % during the YOG period and afterwards. This indicates that air quality regulations taken by the local government have an effect in reducing NOx emissions. The algorithm is also able to detect an emission reduction of 10 % during the Chinese Spring Festival. This study demonstrates the capacity of the DECSO algorithm to capture the change of NOx emissions on a monthly scale. We also show that the observed NO2 columns and the derived emissions show different patterns that provide complimentary information. For example, the Nanjing smog episode in December 2013 led to a strong increase in NO2 concentrations without an increase in NOx emissions. Furthermore, DECSO gives us important information on the non-trivial seasonal relation between NOx emissions and NO2 concentrations on a local scale.

Measurements of PAN, PPN, and MPAN made during the 1994 and 1995 Nashville Intensives of the Southern Oxidant Study: Implications for regional ozone production from biogenic hydrocarbons

NASA Astrophysics Data System (ADS)

Roberts, James M.; Williams, Jonathan; Baumann, Karsten; Buhr, Martin P.; Goldan, Paul D.; Holloway, John; Hübler, Gerhard; Kuster, William C.; McKeen, Stuart A.; Ryerson, Thomas B.; Trainer, Michael; Williams, Eric J.; Fehsenfeld, Fredrick C.; Bertman, Steven B.; Nouaime, George; Seaver, Craig; Grodzinsky, Gil; Rodgers, Michael; Young, Valerie L.

1998-09-01

Isoprene and a variety of other reactive hydrocarbons are released in large quantities by vegetation in forested regions and are thought to participate in the NOx-catalyzed production of ozone, a serious air quality problem in North America and Europe [National Research Council, 1991]. The determination of the fraction of O3 formed from anthropogenic NOx and biogenic hydrocarbons (BHC) is a crucial step in the formulation of effective control strategies. Peroxymethacrylic nitric anhydride (MPAN, CH2C(CH3)C(O)OONO2) is formed almost entirely from the atmospheric oxidation of isoprene in the presence of NOx and is an excellent indicator of recent ozone production from isoprene and therefore biogenic hydrocarbons. Measurements are presented here of MPAN, peroxyacetic nitric anhydride (PAN, CH3C(O)OONO2), peroxypropionic nitric anhydride (PPN, CH3CH2C(O)OONO2) and ozone from separate data sets acquired during the 1994 and 1995 Nashville intensive studies of the Southern Oxidant Study. It was found that PAN, a general product of HC-NOx photochemistry, could be well represented as a simple linear combination of contributions from BHC and anthropogenic hydrocarbon (AHC) chemistries as indicated by MPAN and PPN, respectively. The PAN:MPAN ratios found to be characteristic of BHC-dominated chemistry ranged from 6 to 10. The PAN:PPN ratios found to be characteristic of AHC-dominated chemistry ranged from 5.8 to 7.4. These BHC and AHC attributions were used to estimate the contributions of anthropogenic and biogenic hydrocarbons to regional tropospheric ozone production, and substantial BHC-O3 (50-60 ppbv) was estimated in cases where high NOx from power plants was present in areas of high BHC emission. This estimation method provides direct evidence of significant photochemical ozone production from the oxidation of biogenic hydrocarbons in the presence of NOx.

Regional Attribution of Ozone Production and Associated Radiative Forcing: a Step to Crediting NOx Emission Reductions

NASA Astrophysics Data System (ADS)

Naik, V.; Mauzerall, D. L.; Horowitz, L.; Schwarzkopf, D.; Ramaswamy, V.; Oppenheimer, M.

2004-12-01

The global distribution of tropospheric ozone (O3) depends on the location of emissions of its precursors in addition to chemical and dynamical factors. The global picture of O3 forcing is, therefore, a sum of regional forcings arising from emissions of precursors from different sources. The Kyoto Protocol does not include ozone as a greenhouse gas, and emission reductions of ozone precursors made under Kyoto or any similar agreement would presently receive no credit. In this study, we quantitatively estimate the contribution of emissions of nitrogen oxides (NOx), the primary limiting O3 precursor in the non-urban atmosphere, from specific countries and regions of the world to global O3 concentration distributions. We then estimate radiative forcing resulting from the regional perturbations of NOx emissions. This analysis is intended as an early step towards incorporating O3 into the Kyoto Protocol or any successor agreement. Under such a system countries could obtain credit for improvements in local air quality that result in reductions of O3 concentrations because of the associated reductions in radiative forcing. We use the global chemistry transport model, MOZART-2, to simulate the global O3 distribution for base year 1990 and perturbations to this distribution caused by a 10% percent reduction in the base emissions of NOx from the United States, Europe, East Asia, India, South America, and Africa. We calculate the radiative forcing for the simulated base and perturbed O3 distributions using the GFDL radiative transfer model. The difference between the radiative forcing from O3 for the base and perturbed distributions provides an estimate of the marginal radiative forcing from a region's emissions of NOx. We will present a quantitative analysis of the magnitude, spatial, and temporal distribution of radiative forcing resulting from marginal changes in the NOx emissions from each region.

Thermodynamic constraint on the depth of the global tropospheric circulation.

PubMed

Thompson, David W J; Bony, Sandrine; Li, Ying

2017-08-01

The troposphere is the region of the atmosphere characterized by low static stability, vigorous diabatic mixing, and widespread condensational heating in clouds. Previous research has argued that in the tropics, the upper bound on tropospheric mixing and clouds is constrained by the rapid decrease with height of the saturation water vapor pressure and hence radiative cooling by water vapor in clear-sky regions. Here the authors contend that the same basic physics play a key role in constraining the vertical structure of tropospheric mixing, tropopause temperature, and cloud-top temperature throughout the globe. It is argued that radiative cooling by water vapor plays an important role in governing the depth and amplitude of large-scale dynamics at extratropical latitudes.

Simulated forecast error and climate drift resulting from the omission of the upper stratosphere in numerical models

NASA Technical Reports Server (NTRS)

Boville, Byron A.; Baumhefner, David P.

1990-01-01

Using an NCAR community climate model, Version I, the forecast error growth and the climate drift resulting from the omission of the upper stratosphere are investigated. In the experiment, the control simulation is a seasonal integration of a medium horizontal general circulation model with 30 levels extending from the surface to the upper mesosphere, while the main experiment uses an identical model, except that only the bottom 15 levels (below 10 mb) are retained. It is shown that both random and systematic errors develop rapidly in the lower stratosphere with some local propagation into the troposphere in the 10-30-day time range. The random growth rate in the troposphere in the case of the altered upper boundary was found to be slightly faster than that for the initial-condition uncertainty alone. However, this is not likely to make a significant impact in operational forecast models, because the initial-condition uncertainty is very large.

Future local and remote influences on Mediterranean ozone air quality and climate forcing

NASA Astrophysics Data System (ADS)

Arnold, S.; Val Martin, M.; Heald, C. L.; Lamarque, J.; Tilmes, S.; Emmons, L. K.

2012-12-01

The Mediterranean region is expected to display large increases in population over the coming decades, and to exhibit strong sensitivity to projected climate change, with increasing frequency of extreme summer temperatures and decreases in precipitation. Understanding of how these changes will affect atmospheric composition in the region is limited. The eastern Mediterranean basin has been shown to exhibit a pronounced summertime local maximum in tropospheric ozone, which impacts both local air quality and the atmospheric radiation balance. The Mediterranean troposphere is influenced by a diverse range of sources, including contributions from inter-continental import, in addition to local anthropogenic and biogenic sources. In summer, the region is subject to import of pollution from Northern Europe in the boundary layer and lower troposphere, from North American sources in the large-scale westerly flow of the free mid and upper-troposphere, as well as import of pollution lofted in the Asian monsoon and carried west to the eastern Mediterranean in anticyclonic flow in the upper troposphere over north Africa. Future atmospheric composition in the Mediterranean is likely to be sensitive to projected changes in emissions from these different sources, as well as changes in transport patterns and dry deposition fluxes under future climate conditions. We use the NCAR Community Earth System Model (CESM) to simulate climate and atmospheric composition for the 2050s, based on greenhouse gas abundances, trace gas and aerosol emissions and land cover and use from two representative concentration pathway (RCP) scenarios (RCP4.5 & RCP8.5), designed for use by the IPCC Coupled Model Intercomparison Project Phase 5 (CMIP5) experiments. By comparing these simulations with a present-day scenario, we investigate the effects of predicted changes in climate and emissions on air quality and climate forcing over the Mediterranean region. The simulations suggest decreases in boundary layer ozone and sulfate aerosol throughout the tropospheric column over the Mediterranean under both RCP scenarios, and an increase in ozone of up to 14 ppbv between 5-10km. This ozone increase is coincident with an increase in easterly import of ozone precursors in upper tropospheric outflow from Asian monsoon convection. We present a breakdown of contributions to the projected ozone changes from changes in emissions and from climate-driven changes. We estimate the implications of the predicted changes in tropospheric composition for Mediterranean air quality and climate in 2050, and the consequences for the effectiveness of European policies aimed at protecting the region's climate and public health.

Characterization of Transport Errors in Chemical Forecasts from a Global Tropospheric Chemical Transport Model

NASA Technical Reports Server (NTRS)

Bey, I.; Jacob, D. J.; Liu, H.; Yantosca, R. M.; Sachse, G. W.

2004-01-01

We propose a new methodology to characterize errors in the representation of transport processes in chemical transport models. We constrain the evaluation of a global three-dimensional chemical transport model (GEOS-CHEM) with an extended dataset of carbon monoxide (CO) concentrations obtained during the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft campaign. The TRACEP mission took place over the western Pacific, a region frequently impacted by continental outflow associated with different synoptic-scale weather systems (such as cold fronts) and deep convection, and thus provides a valuable dataset. for our analysis. Model simulations using both forecast and assimilated meteorology are examined. Background CO concentrations are computed as a function of latitude and altitude and subsequently subtracted from both the observed and the model datasets to focus on the ability of the model to simulate variability on a synoptic scale. Different sampling strategies (i.e., spatial displacement and smoothing) are applied along the flight tracks to search for systematic model biases. Statistical quantities such as correlation coefficient and centered root-mean-square difference are computed between the simulated and the observed fields and are further inter-compared using Taylor diagrams. We find no systematic bias in the model for the TRACE-P region when we consider the entire dataset (i.e., from the surface to 12 km ). This result indicates that the transport error in our model is globally unbiased, which has important implications for using the model to conduct inverse modeling studies. Using the First-Look assimilated meteorology only provides little improvement of the correlation, in comparison with the forecast meteorology. These general statements can be refined when the entire dataset is divided into different vertical domains, i.e., the lower troposphere (less than 2 km), the middle troposphere (2-6 km), and the upper troposphere (greater than 6 km). The best agreement between the observations and the model is found in the lower and middle troposphere. Downward displacements in the lower troposphere provide a better fit with the observed value, which could indicate a problem in the representation of boundary layer height in the model. Significant improvement is also found for downward and southward displacements in the upper troposphere. There are several potential sources of errors in our simulation of the continental outflow in the upper troposphere which could lead to such biases, including the location and/or the strength of deep convective cells as well as that of wildfires in Southeast Asia.

High levels of reactive gaseous mercury observed at a high elevation research laboratory in the Rocky Mountains

NASA Astrophysics Data System (ADS)

Faïn, X.; Obrist, D.; Hallar, A. G.; McCubbin, I.; Rahn, T.

2009-10-01

The chemical cycling and spatiotemporal distribution of mercury in the troposphere is poorly understood. We measured gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particulate mercury (HgP) along with carbon monoxide (CO), ozone (O3), aerosols, and meteorological variables at Storm Peak Laboratory at an elevation of 3200 m a.s.l., in Colorado, from 28 April to 1 July 2008. The mean mercury concentrations were 1.6 ng m-3 (GEM), 20 pg m-3 (RGM) and 9 pg m-3 (HgP). We observed eight events of strongly enhanced atmospheric RGM levels with maximum concentrations up to 137 pg m-3. RGM enhancement events lasted for long time periods of 2 to 6 days showing both enriched level during daytime and nighttime when other tracers (e.g., aerosols) showed different representations of boundary layer air and free tropospheric air. During seven of these events, RGM was inversely correlated to GEM (RGM/GEM regression slope ~-0.1), but did not exhibit correlations with ozone, carbon monoxide, or aerosol concentrations. Relative humidity was the dominant factor affecting RGM levels with high RGM levels always present whenever relative humidity was below 40 to 50%. We conclude that RGM enhancements observed at Storm Peak Laboratory were not induced by pollution events and were related to oxidation of tropospheric GEM. High RGM levels were not limited to upper tropospheric or stratospherically influenced air masses, indicating that entrainment processes and deep vertical mixing of free tropospheric air enriched in RGM may lead to high RGM levels throughout the troposphere and into the boundary layer over the Western United States. Based on backtrajectory analysis and a lack of mass balance between RGM and GEM, atmospheric production of RGM may also have occurred in some distance allowing for scavenging and/or deposition of RGM prior to reaching the laboratory. Our observations provide evidence that the tropospheric pool of mercury is frequently enriched in divalent mercury, that high RGM levels are not limited to upper tropospheric air masses, but that the build-up of high RGM in the troposphere is limited to the presence of dry air.

Dynamical Meteorology of the Equatorial and Extratropical Stratosphere

NASA Technical Reports Server (NTRS)

Dunkerton, Tomothy

1999-01-01

Observational studies were performed of westward propagating synoptic scale waves in the tropical troposphere, the structure of monsoon circulations in the upper troposphere and lower stratosphere, and zonally propagating features in deep tropical convection. The effect of the quasi-biennial oscillation (QBO) were investigated, and a numerical study of the QBO was performed using a two-dimensional model, highlighting the role of gravity waves in the momentum balance of the QBO. Vertical coupling of the troposphere and stratosphere was examined in polar regions on intraseasonal and interannual timescales. A deep circumpolar mode was discovered, now known as the Arctic Oscillation.

What controls the seasonal cycle of columnar methane observed by GOSAT over different regions in India?

NASA Astrophysics Data System (ADS)

Chandra, Naveen; Hayashida, Sachiko; Saeki, Tazu; Patra, Prabir K.

2017-10-01

Methane (CH4) is one of the most important short-lived climate forcers for its critical roles in greenhouse warming and air pollution chemistry in the troposphere, and the water vapor budget in the stratosphere. It is estimated that up to about 8 % of global CH4 emissions occur from South Asia, covering less than 1 % of the global land. With the availability of satellite observations from space, variability in CH4 has been captured for most parts of the global land with major emissions, which were otherwise not covered by the surface observation network. The satellite observation of the columnar dry-air mole fractions of methane (XCH4) is an integrated measure of CH4 densities at all altitudes from the surface to the top of the atmosphere. Here, we present an analysis of XCH4 variability over different parts of India and the surrounding cleaner oceanic regions as measured by the Greenhouse gases Observation SATellite (GOSAT) and simulated by an atmospheric chemistry-transport model (ACTM). Distinct seasonal variations of XCH4 have been observed over the northern (north of 15° N) and southern (south of 15° N) parts of India, corresponding to the peak during the southwestern monsoon (July-September) and early autumn (October-December) seasons, respectively. Analysis of the transport, emission, and chemistry contributions to XCH4 using ACTM suggests that a distinct XCH4 seasonal cycle over northern and southern regions of India is governed by both the heterogeneous distributions of surface emissions and a contribution of the partial CH4 column in the upper troposphere. Over most of the northern Indian Gangetic Plain regions, up to 40 % of the peak-to-trough amplitude during the southwestern (SW) monsoon season is attributed to the lower troposphere ( ˜ 1000-600 hPa), and ˜ 40 % to uplifted high-CH4 air masses in the upper troposphere ( ˜ 600-200 hPa). In contrast, the XCH4 seasonal enhancement over semi-arid western India is attributed mainly ( ˜ 70 %) to the upper troposphere. The lower tropospheric region contributes up to 60 % in the XCH4 seasonal enhancement over the Southern Peninsula and oceanic region. These differences arise due to the complex atmospheric transport mechanisms caused by the seasonally varying monsoon. The CH4 enriched air mass is uplifted from a high-emission region of the Gangetic Plain by the SW monsoon circulation and deep cumulus convection and then confined by anticyclonic wind in the upper tropospheric heights ( ˜ 200 hPa). The anticyclonic confinement of surface emission over a wider South Asia region leads to a strong contribution of the upper troposphere in the formation of the XCH4 peak over northern India, including the semi-arid regions with extremely low CH4 emissions. Based on this analysis, we suggest that a link between surface emissions and higher levels of XCH4 is not always valid over Asian monsoon regions, although there is often a fair correlation between surface emissions and XCH4. The overall validity of ACTM simulation for capturing GOSAT observed seasonal and spatial XCH4 variability will allow us to perform inverse modeling of XCH4 emissions in the future using XCH4 data.

Seasonal Variability in Tropospheric Ozone Distribution Over Qatar

NASA Astrophysics Data System (ADS)

Ayoub, Mohammed; Ackermann, Luis

2015-04-01

We report on the vertical distribution and seasonal variability in tropospheric ozone over the Middle East through one year of weekly ozonesondes launched from Doha, Qatar during 2014. A total of 49 2Z-V7 DMT/EN-SCI Electrochemical Concentration Cell (ECC) ozonesondes employing a 1% buffered potassium iodide solution (KI), coupled with iMet-1-RS GPS radiosondes were launched around 1300 local time. The authors used the SkySonde telemetry software (developed by CIRES and NOAA/ESRL) and developed robust in-house data quality assurance and validation methodologies. The average height of the thermal tropopause is between 15-17.5 km (125-85 hPa). Monthly average relative humidity around the tropopause shows an enhancement during the months of June through the beginning of October. Monthly average temperature profiles show the development of the subtropical subsidence inversion around 5-6 km (450-520 hPa) between the months of April through October. The subsidence inversion is strongest during the months of June and July and is accompanied by a sharp drop in relative humidity over a 100-300 m in the vertical. The monthly average ozone background concentration between the Planetary Boundary Layer (PBL) height and the subsidence inversion increases from 50 ppb in the winter to almost 80 ppb in the summer months. An enhancement of up to 50% in the average ozone in the mid-to-upper troposphere (above the subsidence inversion) is strongest during the summer months (June through September) and results in average concentrations between 80-100 ppb. In the upper troposphere (above 13 km/200 hPa) ozone concentrations are highest during the spring and summer months. This is coupled with a drop in the average height of the tropopause. HYSPLIT back-trajectory analysis shows the enhancement in mid-to-upper tropospheric ozone in the summer is due to persistent high pressure over the Middle East between the months of June through September. Evidence of Stratosphere-Troposphere Exchange (STE) in the winter and spring months and Monsoonal outflow observed in late summer are also reflected in the ozone profiles and HYSPLIT back-trajectories.

Evaluation of Near-Tropopause Ozone Distributions in the Global Modeling Initiative Combined Stratosphere/Troposphere Model with Ozonesonde Data

NASA Technical Reports Server (NTRS)

Considine, David B.; Logan, Jennifer A.; Olsen, Mark A.

2008-01-01

The NASA Global Modeling Initiative has developed a combined stratosphere/troposphere chemistry and transport model which fully represents the processes governing atmospheric composition near the tropopause. We evaluate model ozone distributions near the tropopause, using two high vertical resolution monthly mean ozone profile climatologies constructed with ozonesonde data, one by averaging on pressure levels and the other relative to the thermal tropopause. Model ozone is high biased at the SH tropical and NH midlatitude tropopause by approx. 45% in a 4 deg. latitude x 5 deg. longitude model simulation. Increasing the resolution to 2 deg. x 2.5 deg. increases the NH tropopause high bias to approx. 60%, but decreases the tropical tropopause bias to approx. 30%, an effect of a better-resolved residual circulation. The tropopause ozone biases appear not to be due to an overly vigorous residual circulation or excessive stratosphere/troposphere exchange, but are more likely due to insufficient vertical resolution or excessive vertical diffusion near the tropopause. In the upper troposphere and lower stratosphere, model/measurement intercomparisons are strongly affected by the averaging technique. NH and tropical mean model lower stratospheric biases are less than 20%. In the upper troposphere, the 2 deg. x 2.5 deg. simulation exhibits mean high biases of approx. 20% and approx. 35% during April in the tropics and NH midlatitudes, respectively, compared to the pressure averaged climatology. However, relative-to-tropopause averaging produces upper troposphere high biases of approx. 30% and 70% in the tropics and NH midlatitudes. This is because relative-to-tropopause averaging better preserves large cross-tropopause O3 gradients, which are seen in the daily sonde data, but not in daily model profiles. The relative annual cycle of ozone near the tropopause is reproduced very well in the model Northern Hemisphere midlatitudes. In the tropics, the model amplitude of the near tropopause annual cycle is weak. This is likely due to the annual amplitude of mean vertical upwelling near the tropopause, which analysis suggests is approx. 30% weaker than in the real atmosphere.

The Tropospheric cooling and the Stratospheric warming at Tirunelveli during the Annular Solar Eclipse of 15 January, 2010

NASA Astrophysics Data System (ADS)

Nelli, Narendra Reddy; Choudhary, Raj Kumar; Rao, Kusuma

The UTLS region, a transition region between the troposphere and the stratosphere is of concern to climate scientists as its temperature variations are crucial in determining the water vapour and the other trace gases transport between the two regions, which inturn determine the radiative warming and cooling of the troposphere and the stratosphere. To examine, the temperature variations from surface to lower stratosphere,a major experiment facility was set up for upper air and surface measurements during the Annular Solar Eclipse (ASE) of January 15, 2010 at Tirunelveli (8.72 N, 77.81 E) located in 94% eclipse path in the southern peninsular India. The instruments,namely, 1. high resolution GPS radiosonde system, 2. an instrumented 15 m high Mini Boundary Layer Mast, 3. an instrumented 1 m high Near Surface Mast (NSM), radiation and other ground sensors were operated during the period 14-19 Jan, 2010. The ASE of January 15, 2010 was unique being the longest in duration (9 min, 15.3 sec) among the similar ones that occurred in the past. The major inference from an analysis of surface and upper air measurements is the occurrence of troposphere cooling during the eclipse with the peak cooling of 5 K at 15 km height with respect to no-eclispe conditions. Also, intense warming in the stratosphere is observed with the peak warming of 7 K at 19 km height.Cooling of the Troposphere as the eclipse advanced and the revival to its normal temperature is clearly captured in upper air measurements. The downward vertical velocities observed at 100 hPa in NCEP Re-analyses, consistent with the tropospheric cooling during the ASE window, may be causing the stratospheric warming. Partly, these vertical velocities could be induced by the mesoscale circulation associated with the mesoscale convective system that prevailed parallel to the eclipse path as described in METEOSAT imageries of brightness temperatures from IR channel. Further analysis is being carried out to quantify the variations in turbulent parameters during ASE window using the high resolution GPS Radiosonde data.

Tropospheric Vertical Distribution of Tropical Atlantic Ozone Observed by TES during the Northern African Biomass Burning Season

NASA Technical Reports Server (NTRS)

Jourdain, L.; Worden, H. M.; Worden, J. R.; Bowman, K.; Li, Q.; Eldering, A.; Kulawik, S. S.; Osterman, G.; Boersma, K. F.; Fisher, B.;

Balloon Borne Soundings of Water Vapor, Ozone and Temperature in the Upper Tropospheric and Lower Stratosphere as Part of the Second SAGE III Ozone Loss and Validation Experiment (SOLVE-2)

NASA Technical Reports Server (NTRS)

Voemel, Holger

2004-01-01

The main goal of our work was to provide in situ water vapor and ozone profiles in the upper troposphere and lower stratosphere as reference measurements for the validation of SAGE III water vapor and ozone retrievals. We used the NOAA/CMDL frost point hygrometer and ECC ozone sondes on small research balloons to provide continuous profiles between the surface and the mid stratosphere. The NOAA/CMDL frost point hygrometer is currently the only lightweight balloon borne instrument capable of measuring water vapor between the lower troposphere and middle stratosphere. The validation measurements were based in the arctic region of Scandinavia for northern hemisphere observations and in New Zealand for southern hemisphere observations and timed to coincide with overpasses of the SAGE III instrument. In addition to SAGE III validation we also tried to coordinate launches with other instruments and studied dehydration and transport processes in the Arctic stratospheric vortex.

Stratospheric Aerosol and Gas Experiment (SAGE 3)

NASA Technical Reports Server (NTRS)

Mccormick, M. P.

1993-01-01

The proposed SAGE III instrument would be the principal source of data for global changes of stratospheric aerosols, stratospheric water vapor, and ozone profiles, and a contributing source of data for upper tropospheric water vapor, aerosols, and clouds. The ability to obtain such data has been demonstrated by the predecessor instrument, SAGE II, but SAGE III will be substantially more capable, as discussed below. The capabilities for monitoring the profiles of atmospheric constituents have been verified in detail, including ground-based validations, for aerosol, ozone, and water vapor. Indeed, because of its self-calibrating characteristics, SAGE II was an essential component of the international ozone trend assessments, and SAGE II is now proving to be invaluable in tracking the aerosols from Mt. Pinatubo. Although SAGE profiles generally terminate at the height of the first tropospheric cloud layer, it has been found that the measurements extend down to 3 km altitude more than 40 percent of the time at most latitudes. Thus, useful information can also be obtained on upper tropospheric aerosols, water vapor, and ozone.

Thermodynamic control of anvil cloud amount

PubMed Central

Bony, Sandrine; Stevens, Bjorn; Coppin, David; Becker, Tobias; Reed, Kevin A.; Voigt, Aiko

2016-01-01

General circulation models show that as the surface temperature increases, the convective anvil clouds shrink. By analyzing radiative–convective equilibrium simulations, we show that this behavior is rooted in basic energetic and thermodynamic properties of the atmosphere: As the climate warms, the clouds rise and remain at nearly the same temperature, but find themselves in a more stable atmosphere; this enhanced stability reduces the convective outflow in the upper troposphere and decreases the anvil cloud fraction. By warming the troposphere and increasing the upper-tropospheric stability, the clustering of deep convection also reduces the convective outflow and the anvil cloud fraction. When clouds are radiatively active, this robust coupling between temperature, high clouds, and circulation exerts a positive feedback on convective aggregation and favors the maintenance of strongly aggregated atmospheric states at high temperatures. This stability iris mechanism likely contributes to the narrowing of rainy areas as the climate warms. Whether or not it influences climate sensitivity requires further investigation. PMID:27412863

On the role of ozone feedback in the ENSO amplitude response under global warming.

PubMed

Nowack, Peer J; Braesicke, Peter; Luke Abraham, N; Pyle, John A

2017-04-28

The El Niño-Southern Oscillation (ENSO) in the tropical Pacific Ocean is of key importance to global climate and weather. However, state-of-the-art climate models still disagree on the ENSO's response under climate change. The potential role of atmospheric ozone changes in this context has not been explored before. Here we show that differences between typical model representations of ozone can have a first-order impact on ENSO amplitude projections in climate sensitivity simulations. The vertical temperature gradient of the tropical middle-to-upper troposphere adjusts to ozone changes in the upper troposphere and lower stratosphere, modifying the Walker circulation and consequently tropical Pacific surface temperature gradients. We show that neglecting ozone changes thus results in a significant increase in the number of extreme ENSO events in our model. Climate modeling studies of the ENSO often neglect changes in ozone. We therefore highlight the need to understand better the coupling between ozone, the tropospheric circulation, and climate variability.

Thermodynamic control of anvil cloud amount

DOE PAGES

Bony, Sandrine; Stevens, Bjorn; Coppin, David; ...

2016-07-13

General circulation models show that as the surface temperature increases, the convective anvil clouds shrink. By analyzing radiative–convective equilibrium simulations, our work shows that this behavior is rooted in basic energetic and thermodynamic properties of the atmosphere: As the climate warms, the clouds rise and remain at nearly the same temperature, but find themselves in a more stable atmosphere; this enhanced stability reduces the convective outflow in the upper troposphere and decreases the anvil cloud fraction. By warming the troposphere and increasing the upper-tropospheric stability, the clustering of deep convection also reduces the convective outflow and the anvil cloud fraction.more » When clouds are radiatively active, this robust coupling between temperature, high clouds, and circulation exerts a positive feedback on convective aggregation and favors the maintenance of strongly aggregated atmospheric states at high temperatures. This stability iris mechanism likely contributes to the narrowing of rainy areas as the climate warms. Whether or not it influences climate sensitivity requires further investigation.« less

Mesoscale aspects of jet streak coupling and implications for the short term forecasting of severe convective storms. [severe environmental storms and mesoscale experiment (SESAME)

NASA Technical Reports Server (NTRS)

Uccellini, L. W.; Kocin, P. J.

1981-01-01

An analysis of a tornado outbreak in Wichita Falls, Texas was analyzed. The coupling of upper and lower tropospheric jet streaks, leading to severe storm outbreaks is illustrated. The high resolution SESAME data sets indicate that mass and momentum adjustments which couple upper and lower tropospheric jets occur within a 3 to 6 hr time frame over a 100 to 500 km domain, and establish the role of isallobaric forcing in the storm development. It is suggested that the output rate of data from the existing 12 hr network be increased to provide better temporal resolution of wind, mass and moisture data.

Theoretical Investigations of Clouds and Aerosols in the Stratosphere and Upper Troposphere

NASA Technical Reports Server (NTRS)

Toon, Owen B.

2005-01-01

support of the Atmospheric Chemistry Modeling and Data Analysis Program. We investigated a wide variety of issues involving ambient stratospheric aerosols, polar stratospheric clouds or heterogeneous chemistry, analysis of laboratory data, and particles in the upper troposphere. The papers resulting from these studies are listed below. In addition, I participated in the 1999-2000 SOLVE mission as one of the project scientists and in the 2002 CRYSTAL field mission as one of the project scientists. Several CU graduate students and research associates also participated in these mission, under support from the ACMAP program, and worked to interpret data. During the past few years my group has completed a number of projects under the

Concentrations of carbonyl sulfide and hydrogen cyanide in the free upper troposphere and lower stratosphere deduced from ATMOS/Spacelab 3 infrared solar occultation spectra

NASA Technical Reports Server (NTRS)

Zander, R.; Rinsland, C. P.; Russell, J. M., III; Farmer, C. B.; Norton, R. H.

1988-01-01

This paper presents the results on the volume mixing ratio profiles of carbonyl sulfide and hydrogen cyanide, deduced from the spectroscopic analysis of IR solar absorption spectra obtained in the occultation mode with the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument during its mission aboard Spacelab 3. A comparison of the ATMOS measurements for both northern and southern latitudes with previous field investigations at low midlatitudes shows a relatively good agreement. Southern Hemisphere volume mixing ratio profiles for both molecules were obtained for the first time, as were the profiles for the Northern Hemisphere covering the upper troposphere and the lower stratosphere simultaneously.

Global CO emission estimates inferred from assimilation of MOPITT and IASI CO data, together with observations of O3, NO2, HNO3, and HCHO.

NASA Astrophysics Data System (ADS)

Zhang, X.; Jones, D. B. A.; Keller, M.; Jiang, Z.; Bourassa, A. E.; Degenstein, D. A.; Clerbaux, C.; Pierre-Francois, C.

2017-12-01

Atmospheric carbon monoxide (CO) emissions estimated from inverse modeling analyses exhibit large uncertainties, due, in part, to discrepancies in the tropospheric chemistry in atmospheric models. We attempt to reduce the uncertainties in CO emission estimates by constraining the modeled abundance of ozone (O3), nitrogen dioxide (NO2), nitric acid (HNO3), and formaldehyde (HCHO), which are constituents that play a key role in tropospheric chemistry. Using the GEOS-Chem four-dimensional variational (4D-Var) data assimilation system, we estimate CO emissions by assimilating observations of CO from the Measurement of Pollution In the Troposphere (MOPITT) and the Infrared Atmospheric Sounding Interferometer (IASI), together with observations of O3 from the Optical Spectrograph and InfraRed Imager System (OSIRIS) and IASI, NO2 and HCHO from the Ozone Monitoring Instrument (OMI), and HNO3 from the Microwave Limb Sounder (MLS). Our experiments evaluate the inferred CO emission estimates from major anthropogenic, biomass burning and biogenic sources. Moreover, we also infer surface emissions of nitrogen oxides (NOx = NO + NO2) and isoprene. Our results reveal that this multiple species chemical data assimilation produces a chemical consistent state that effectively adjusts the CO-O3-OH coupling in the model. The O3-induced changes in OH are particularly large in the tropics. Overall, our analysis results in a better constrained tropospheric chemical state.

Simulation of Aerosols and Chemistry with a Unified Global Model

NASA Technical Reports Server (NTRS)

Chin, Mian

2004-01-01

This project is to continue the development of the global simulation capabilities of tropospheric and stratospheric chemistry and aerosols in a unified global model. This is a part of our overall investigation of aerosol-chemistry-climate interaction. In the past year, we have enabled the tropospheric chemistry simulations based on the GEOS-CHEM model, and added stratospheric chemical reactions into the GEOS-CHEM such that a globally unified troposphere-stratosphere chemistry and transport can be simulated consistently without any simplifications. The tropospheric chemical mechanism in the GEOS-CHEM includes 80 species and 150 reactions. 24 tracers are transported, including O3, NOx, total nitrogen (NOy), H2O2, CO, and several types of hydrocarbon. The chemical solver used in the GEOS-CHEM model is a highly accurate sparse-matrix vectorized Gear solver (SMVGEAR). The stratospheric chemical mechanism includes an additional approximately 100 reactions and photolysis processes. Because of the large number of total chemical reactions and photolysis processes and very different photochemical regimes involved in the unified simulation, the model demands significant computer resources that are currently not practical. Therefore, several improvements will be taken, such as massive parallelization, code optimization, or selecting a faster solver. We have also continued aerosol simulation (including sulfate, dust, black carbon, organic carbon, and sea-salt) in the global model to cover most of year 2002. These results have been made available to many groups worldwide and accessible from the website http://code916.gsfc.nasa.gov/People/Chin/aot.html.

Simulations of Tropospheric NO2 by the Global Modeling Initiative (GMI) Model Utilizing Assimilated and Forecast Meteorological Fields: Comparison to Ozone Monitoring Instrument (OMI) Measurements

NASA Technical Reports Server (NTRS)

Rodriquez, J. M.; Yoshida, Y.; Duncan, B. N.; Bucsela, E. J.; Gleason, J. F.; Allen, D.; Pickering, K. E.

2007-01-01

We present simulations of the tropospheric composition for the years 2004 and 2005, carried out by the GMI Combined Stratosphere-Troposphere (Combo) model, at a resolution of 2degx2.5deg. The model includes a new parameterization of lightning sources of NO(x) which is coupled to the cloud mass fluxes in the adopted meteorological fields. These simulations use two different sets of input meteorological fields: a)late-look assimilated fields from the Global Modeling and Assimilation Office (GMAO), GEOS-4 system and b) 12-hour forecast fields initialized with the assimilated data. Comparison of the forecast to the assimilated fields indicates that the forecast fields exhibit less vigorous convection, and yield tropical precipitation fields in better agreement with observations. Since these simulations include a complete representation of the stratosphere, they provide realistic stratosphere-tropospheric fluxes of O3 and NO(y). Furthermore, the stratospheric contribution to total columns of different troposheric species can be subtracted in a consistent fashion, and the lightning production of NO(y) will depend on the adopted meteorological field. We concentrate here on the simulated tropospheric columns of NO2, and compare them to observations by the OM1 instrument for the years 2004 and 2005. The comparison is used to address these questions: a) is there a significant difference in the agreement/disagreement between simulations for these two different meteorological fields, and if so, what causes these differences?; b) how do the simulations compare to OMI observations, and does this comparison indicate an improvement in simulations with the forecast fields? c) what are the implications of these simulations for our understanding of the NO2 emissions over continental polluted regions?

The influence of synoptic weather regimes on UK air quality: regional model studies of tropospheric column NO2

NASA Astrophysics Data System (ADS)

Pope, R. J.; Savage, N. H.; Chipperfield, M. P.; Ordóñez, C.; Neal, L. S.

2015-10-01

Synoptic meteorology can have a significant influence on UK air quality. Cyclonic conditions lead to the dispersion of air pollutants away from source regions, while anticyclonic conditions lead to their accumulation over source regions. Meteorology also modifies atmospheric chemistry processes such as photolysis and wet deposition. Previous studies have shown a relationship between observed satellite tropospheric column NO2 and synoptic meteorology in different seasons. Here, we test whether the UK Met Office Air Quality in the Unified Model (AQUM) can reproduce these observations and then use the model to explore the relative importance of various factors. We show that AQUM successfully captures the observed relationships when sampled under the Lamb weather types, an objective classification of midday UK circulation patterns. By using a range of idealized NOx-like tracers with different e-folding lifetimes, we show that under different synoptic regimes the NO2 lifetime in AQUM is approximately 6 h in summer and 12 h in winter. The longer lifetime can explain why synoptic spatial tropospheric column NO2 variations are more significant in winter compared to summer, due to less NO2 photochemical loss. We also show that cyclonic conditions have more seasonality in tropospheric column NO2 than anticyclonic conditions as they result in more extreme spatial departures from the wintertime seasonal average. Within a season (summer or winter) under different synoptic regimes, a large proportion of the spatial pattern in the UK tropospheric column NO2 field can be explained by the idealized model tracers, showing that transport is an important factor in governing the variability of UK air quality on seasonal synoptic timescales.

Microbiome of the upper troposphere: species composition and prevalence, effects of tropical storms, and atmospheric implications.

PubMed

DeLeon-Rodriguez, Natasha; Lathem, Terry L; Rodriguez-R, Luis M; Barazesh, James M; Anderson, Bruce E; Beyersdorf, Andreas J; Ziemba, Luke D; Bergin, Michael; Nenes, Athanasios; Konstantinidis, Konstantinos T

2013-02-12

The composition and prevalence of microorganisms in the middle-to-upper troposphere (8-15 km altitude) and their role in aerosol-cloud-precipitation interactions represent important, unresolved questions for biological and atmospheric science. In particular, airborne microorganisms above the oceans remain essentially uncharacterized, as most work to date is restricted to samples taken near the Earth's surface. Here we report on the microbiome of low- and high-altitude air masses sampled onboard the National Aeronautics and Space Administration DC-8 platform during the 2010 Genesis and Rapid Intensification Processes campaign in the Caribbean Sea. The samples were collected in cloudy and cloud-free air masses before, during, and after two major tropical hurricanes, Earl and Karl. Quantitative PCR and microscopy revealed that viable bacterial cells represented on average around 20% of the total particles in the 0.25- to 1-μm diameter range and were at least an order of magnitude more abundant than fungal cells, suggesting that bacteria represent an important and underestimated fraction of micrometer-sized atmospheric aerosols. The samples from the two hurricanes were characterized by significantly different bacterial communities, revealing that hurricanes aerosolize a large amount of new cells. Nonetheless, 17 bacterial taxa, including taxa that are known to use C1-C4 carbon compounds present in the atmosphere, were found in all samples, indicating that these organisms possess traits that allow survival in the troposphere. The findings presented here suggest that the microbiome is a dynamic and underappreciated aspect of the upper troposphere with potentially important impacts on the hydrological cycle, clouds, and climate.

Water vapor changes under global warming and the linkage to present-day interannual variabilities in CMIP5 models

NASA Astrophysics Data System (ADS)

Takahashi, Hanii; Su, Hui; Jiang, Jonathan H.

2016-12-01

The fractional water vapor changes under global warming across 14 Coupled Model Intercomparison Project Phase 5 simulations are analyzed. We show that the mean fractional water vapor changes under global warming in the tropical upper troposphere between 300 and 100 hPa range from 12.4 to 28.0 %/K across all models while the fractional water vapor changes are about 5-8 %/K in other regions and at lower altitudes. The "upper-tropospheric amplification" of the water vapor change is primarily driven by a larger temperature increase in the upper troposphere than in the lower troposphere per degree of surface warming. The relative contributions of atmospheric temperature and relative humidity changes to the water vapor change in each model vary between 71.5 to 131.8 % and 24.8 to -20.1 %, respectively. The inter-model differences in the water vapor change is primarily caused by differences in temperature change, except over the inter-tropical convergence zone within 10°S-10°N where the model differences due to the relative humidity change are significant. Furthermore, we find that there is generally a positive correlation between the rates of water vapor change for long-tem surface warming and those on the interannual time scales. However, the rates of water vapor change under long-term warming have a systematic offset from those on the inter-annual time scales and the dominant contributor to the differences also differs for the two time scales, suggesting caution needs to be taken when inferring long-term water vapor changes from the observed interannual variations.

Impact of climate variability on tropospheric ozone.

PubMed

Grewe, Volker

2007-03-01

A simulation with the climate-chemistry model (CCM) E39/C is presented, which covers both the troposphere and stratosphere dynamics and chemistry during the period 1960 to 1999. Although the CCM, by its nature, is not exactly representing observed day-by-day meteorology, there is an overall model's tendency to correctly reproduce the variability pattern due to an inclusion of realistic external forcings, like observed sea surface temperatures (e.g. El Niño), major volcanic eruption, solar cycle, concentrations of greenhouse gases, and Quasi-Biennial Oscillation. Additionally, climate-chemistry interactions are included, like the impact of ozone, methane, and other species on radiation and dynamics, and the impact of dynamics on emissions (lightning). However, a number of important feedbacks are not yet included (e.g. feedbacks related to biogenic emissions and emissions due to biomass burning). The results show a good representation of the evolution of the stratospheric ozone layer, including the ozone hole, which plays an important role for the simulation of natural variability of tropospheric ozone. Anthropogenic NO(x) emissions are included with a step-wise linear trend for each sector, but no interannual variability is included. The application of a number of diagnostics (e.g. marked ozone tracers) allows the separation of the impact of various processes/emissions on tropospheric ozone and shows that the simulated Northern Hemisphere tropospheric ozone budget is not only dominated by nitrogen oxide emissions and other ozone pre-cursors, but also by changes of the stratospheric ozone budget and its flux into the troposphere, which tends to reduce the simulated positive trend in tropospheric ozone due to emissions from industry and traffic during the late 80s and early 90s. For tropical regions the variability in ozone is dominated by variability in lightning (related to ENSO) and stratosphere-troposphere exchange (related to Northern Hemisphere Stratospheric dynamics and solar activity). Since tropospheric background chemistry is regarded only, the results are quantitatively limited with respect to derived trends. However, the main results are regarded to be robust. Although the horizontal resolution is rather coarse in comparison to regional models, such kind of simulations provide useful and necessary information on the impact of large-scale processes and inter-annual/decadal variations on regional air quality.

Observation of isoprene hydroxynitrates in the Southeastern United States and implications for the fate of NOx

NASA Astrophysics Data System (ADS)

Xiong, F.; McAvey, K. M.; Pratt, K. A.; Groff, C. J.; Hostetler, M. A.; Lipton, M. A.; Starn, T. K.; Seeley, J. V.; Bertman, S. B.; Teng, A. P.; Crounse, J. D.; Nguyen, T. B.; Wennberg, P. O.; Misztal, P. K.; Goldstein, A. H.; Guenther, A. B.; Koss, A. R.; Olson, K. F.; de Gouw, J. A.; Baumann, K.; Edgerton, E. S.; Feiner, P. A.; Zhang, L.; Miller, D. O.; Brune, W. H.; Shepson, P. B.

2015-07-01

Isoprene hydroxynitrates (IN) are tracers of the photochemical oxidation of isoprene in high NOx environments. Production and loss of IN have a significant influence on the NOx cycle and tropospheric O3 chemistry. To better understand IN chemistry, a series of photochemical reaction chamber experiments were conducted to determine the IN yield from isoprene photooxidation at high NO concentrations (> 100 ppt). By combining experimental data and calculated isomer distributions, a total IN yield of 9(+4/-3) % was derived. The result was applied in a zero-dimensional model to simulate production and loss of ambient IN observed in a temperate forest atmosphere, during the Southern Oxidant and Aerosol Study (SOAS) field campaign, from 27 May to 11 July 2013. By comparing field observations with model simulations, we identified NO as the limiting factor for ambient IN production during SOAS, but vertical mixing at dawn might also contribute (~ 27 %) to IN dynamics. A close examination of isoprene's oxidation products indicates that its oxidation transitioned from a high-NO dominant chemical regime in the morning into a low-NO dominant regime in the afternoon. A significant amount of IN produced in the morning high NO regime could be oxidized in the low NO regime, and a possible reaction scheme was proposed.

Nitrogen oxides and methane treatment by non-thermal plasma

NASA Astrophysics Data System (ADS)

Alva, E.; Pacheco, M.; Colín, A.; Sánchez, V.; Pacheco, J.; Valdivia, R.; Soria, G.

2015-03-01

Non thermal plasma was used to treat nitrogen oxides (NOx) and methane (CH4), since they are important constituents of hydrocarbon combustion emissions processes and, both gases, play a key role in the formation of tropospheric ozone. These gases are involved in environmental problems like acid rain and some diseases such as bronchitis and pneumonia. In the case of methane is widely known its importance in the global climate change, and currently accounts for 30% of global warming. There is a growing concern for methane leaks, associated with a rapid expansion of unconventional oil and gas extraction techniques as well as a large-scale methane release from Arctic because of ice melting and the subsequent methane production of decaying organic matter. Therefore, methane mitigation is a key to avoid dangerous levels of global warming. The research, here reported, deals about the generation of non-thermal plasma with a double dielectric barrier (2DBD) at atmospheric pressure with alternating current (AC) for NOx and CH4 treatment. The degradation efficiencies and their respective power consumption for different reactor configurations (cylindrical and planar) are also reported. Qualitative and quantitative analysis of gases degradation are reported before and after treatment with cold plasma. Experimental and theoretical results are compared obtaining good removal efficiencies, superior to 90% and to 20% respectively for NOx and CH4.

Direct Measurements of the Local Ozone Production Rate in the Pollution Outflow from a Megacity

NASA Astrophysics Data System (ADS)

Crilley, L.; Kramer, L. J.; Woodward-Massey, R.; Cryer, D. R.; Whalley, L. K.; Heard, D. E.; Reeves, C.; Forster, G.; Oram, D.; Bandy, B.; Reed, C.; Lee, J. D.; Bloss, W.

2015-12-01

Tropospheric ozone (O3) is major secondary air pollutant that is formed in the atmosphere through the complex oxidation of volatile organic carbon compounds (VOCs) in the presence of nitrogen oxides (NOx) and sunlight. In order to effectively implement control measures to reduce O3 levels, it is necessary to understand the chemical processes that in part govern O3 concentration, and to disaggregate local chemical O3 production from transport. To address this issue, a major field campaign was organised at the Weybourne Atmospheric Observatory (WAO), a coastal site in the UK that is regularly within the pollution outflow from London and Western Europe. As part of this campaign, a novel approach to directly measure in situ the rate of local O3 production was employed along with a range of instrumentation to measure concentrations of different radical species as well as with detailed VOC and NOx speciation. We will present preliminary findings from a major O3 pollution event (~120 ppb) that occurred during the campaign as a case study for investigating the contributing factors influencing O3 formation at a NOx limited site. Direct measurements of local chemical O3 production rates are compared with those inferred from a range of indirect approaches.

Effects of diabatic heating on the ageostrophic circulation of an upper tropospheric jet streak

NASA Technical Reports Server (NTRS)

Keyser, D. A.; Johnson, D. R.

1982-01-01

Interaction between the mass circulation within a mesoscale convective complex (MCC) and a direct mass circulation in the entrance region of an upper tropospheric polar jet streak was examined within the isentropic structure to investigate mechanisms responsible for linking these two scales of motion. The results establish that latent heating in the MCC modifies the direct mass circulation in the jet streak entrance region through the diabatically induced components of ageostrophic motion analyzed within isentropic coordinates. Within the strong mesoscale mass circulation of each MCC, strong horizontal mass flux convergence into the MCC at low levels is balanced by strong horizontal mass flux divergence away from the convergence at upper levels. Locations of large diabatic heating rates correspond well to the MCC position for each case; diabatic heating forces the upward vertical branch for the mesoscale mass circulation.

Global view of the upper level outflow patterns associated with tropical cyclone intensity changes during FGGE

NASA Technical Reports Server (NTRS)

Chen, L.; Gray, W. M.

1985-01-01

The characteristics of the upper tropospheric outflow patterns which occur with tropical cyclone intensification and weakening over all of the global tropical cyclone basins during the year long period of the First GARP Global Experiment (FGGE) are discussed. By intensification is meant the change in the tropical cyclone's maximum wind or central pressure, not the change of the cyclone's outer 1 to 3 deg radius mean wind which we classify as cyclone strength. All the 80 tropical cyclones which existed during the FGGE year are studied. Two-hundred mb wind fields are derived from the analysis of the European Center for Medium Range Weather Forecasting (ECMWF) which makes extensive use of upper tropospheric satellite and aircraft winds. Corresponding satellite cloud pictures from the polar orbiting U.S. Defense Meteorological Satellite Program (DMSP) and other supplementary polar and geostationary satellite data are also used.

Preindustrial to Present-Day Changes in Tropospheric Hydroxyl Radical and Methane Lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

NASA Technical Reports Server (NTRS)

Naik, V.; Voulgarakis, A.; Fiore, A. M.; Horowitz, L. W.; Lamarque, J.-F.; Lin, M.; Prather, M. J.; Young, P. J.; Bergmann, D.; Cameron-Smith, P. J.;

Tropospheric temperature climatology and trends observed over the Middle East

NASA Astrophysics Data System (ADS)

Basha, Ghouse; Marpu, P. R.; Ouarda, T. B. M. J.

2015-10-01

In this study, we report for the first time, the upper air temperature climatology, and trends over the Middle East, which seem to be significantly affected by the changes associated with hot summer and low precipitation. Long term (1985-2012) radiosonde data from 12 stations are used to derive the mean temperature climatology and vertical trends. The study was performed by analyzing the data at different latitudes. The vertical profiles of air temperature show distinct behavior in terms of vertical and seasonal variability at different latitudes. The seasonal cycle of temperature at the 100 hPa, however, shows an opposite pattern compared to the 200 hPa levels. The temperature at 100 hPa shows a maximum during winter and minimum in summer. Spectral analysis shows that the annual cycle is dominant in comparison with the semiannual cycle. The time-series of temperature data was analyzed using the Bayesian change point analysis and cumulative sum method to investigate the changes in temperature trends. Temperature shows a clear change point during the year 1999 at all stations. Further, Modified Mann-Kendall test was applied to study the vertical trend, and analysis shows statistically significant lower tropospheric warming and cooling in upper troposphere after the year 1999. In general, the magnitude of the trend decreases with altitude in the troposphere. In all the latitude bands in lower troposphere, significant warming is observed, whereas at higher altitudes cooling is noticed based on 28 years temperature observations over the Middle East.

Upper-tropospheric inversion and easterly jet in the tropics

NASA Astrophysics Data System (ADS)

Fujiwara, M.; Xie, S.-P.; Shiotani, M.; Hashizume, H.; Hasebe, F.; VöMel, H.; Oltmans, S. J.; Watanabe, T.

2003-12-01

Shipboard radiosonde measurements revealed a persistent temperature inversion layer with a thickness of ˜200 m at 12-13 km in a nonconvective region over the tropical eastern Pacific, along 2°N, in September 1999. Simultaneous relative humidity measurements indicated that the thin inversion layer was located at the top of a very wet layer with a thickness of 3-4 km, which was found to originate from the intertropical convergence zone (ITCZ) to the north. Radiative transfer calculations suggested that this upper tropospheric inversion (UTI) was produced and maintained by strong longwave cooling in this wet layer. A strong easterly jet stream was also observed at 12-13 km, centered around 4°-5°N. This easterly jet was in the thermal wind balance, with meridional temperature gradients produced by the cloud and radiative processes in the ITCZ and the wet outflow. Furthermore, the jet, in turn, acted to spread inversions further downstream through the transport of radiatively active water vapor. This feedback mechanism may explain the omnipresence of temperature inversions and layering structures in trace gases in the tropical troposphere. Examination of high-resolution radiosonde data at other sites in the tropical Pacific indicates that similar UTIs often appear around 12-15 km. The UTI around 12-15 km may thus be characterized as one of the "climatological" inversions in the tropical troposphere, forming the lower boundary of the so-called tropical tropopause layer, where the tropospheric air is processed photochemically and microphysically before entering the stratosphere.

Tropical Convective Responses to Microphysical and Radiative Processes: A Sensitivity Study With a 2D Cloud Resolving Model

NASA Technical Reports Server (NTRS)

Li, Xiao-Fan; Sui, C.-H.; Lau, K.-M.; Tao, W.-K.

2004-01-01

Prognostic cloud schemes are increasingly used in weather and climate models in order to better treat cloud-radiation processes. Simplifications are often made in such schemes for computational efficiency, like the scheme being used in the National Centers for Environment Prediction models that excludes some microphysical processes and precipitation-radiation interaction. In this study, sensitivity tests with a 2D cloud resolving model are carried out to examine effects of the excluded microphysical processes and precipitation-radiation interaction on tropical thermodynamics and cloud properties. The model is integrated for 10 days with the imposed vertical velocity derived from the Tropical Ocean Global Atmosphere Coupled Ocean-Atmosphere Response Experiment. The experiment excluding the depositional growth of snow from cloud ice shows anomalous growth of cloud ice and more than 20% increase of fractional cloud cover, indicating that the lack of the depositional snow growth causes unrealistically large mixing ratio of cloud ice. The experiment excluding the precipitation-radiation interaction displays a significant cooling and drying bias. The analysis of heat and moisture budgets shows that the simulation without the interaction produces more stable upper troposphere and more unstable mid and lower troposphere than does the simulation with the interaction. Thus, the suppressed growth of ice clouds in upper troposphere and stronger radiative cooling in mid and lower troposphere are responsible for the cooling bias, and less evaporation of rain associated with the large-scale subsidence induces the drying in mid and lower troposphere.

MOZAIC-IAGOS program : 20 years of in-situ data in the UTLS

NASA Astrophysics Data System (ADS)

Thouret, Valérie; Sauvage, Bastien; Nédélec, Philippe; Petzold, Andreas; Volz-Thomas, Andreas

2014-05-01

The use of commercial aircraft allows the collection of highly relevant observations on a scale and in numbers impossible to achieve using research aircraft, and in regions where other measurement methods (e.g., satellites) have technical limitations. Since 1994, the MOZAIC program has been measuring ozone, water vapor and meteorological parameters (along with NOy for 2001-2005 and CO since 2001) on board 5 commercial aircraft. IAGOS (In-service Aircraft for a Global Observing System, http://www.iagos.org) was initiated in 2006 and combines the experience gained within the MOZAIC and CARIBIC programs. IAGOS is now one of the new European Research Infrastructures with the objective of establishing and operating a distributed infrastructure for long-term observations of atmospheric composition (O3, CO, CO2, NOy, NOx, H2O), aerosol and cloud particles on a global scale from a fleet of initially 10-20 long-range in-service aircraft of internationally operating airlines. Data are available in near real time for weather services and Copernicus service centres, as demonstrated in the MACC project (http://www.iagos.fr/macc). The IAGOS database is an essential part of the program and is still under development/improvement such as additional new value-added products (source-receptor link of observed pollutants) obtained by coupling the Lagrangian dispersion model FLEXPART to CO surface emissions from different inventories. Data access through http://www.iagos.fr is handled by an open access policy based on the submission of research requests. An overview of the most recent results focusing on UTLS data will be presented, including : - Five years of MOZAIC NOy observations that are used to characterize and describe large-scale plumes including lightning NOx emissions, in the upper troposphere between North America and Europe. - Characteristics of ozone and CO distributions over regions of interest never or poorly sampled by other platforms are measured: UTLS Northern mid-latitudes thanks to 5 aircraft based in Europe flying westbound and eastbound since 1994; Transects over the African continent thanks to daily Air Namibia flights between 2006 and 2013; South Atlantic area thanks to regular flights between Europe and South America; The Asian monsoon region thanks to regular flights between Europe and the Indian-South East Asia area sampling the UT under the influence of the Asian Monsoon Anticyclone (AMA). - Ten years of CO measurements which show an increase in concentration on moving from the Western to Eastern hemisphere. In the US, Atlantic and European sectors CO concentrations have fallen by about 2% per year. - Almost 20 years of Ozone measurements at northern mid-latitudes showing a leveling-off of the mixing ratios for the last 10-12 years over the Atlantic sector while ozone is still increasing over Asia. - Almost 20 years of relative humidity measurements showing that the upper troposphere (10 - 12 km altitude, which corresponds to the aircraft cruise level) is much wetter than reflected in the model analyses of the ECMWF (European Centre for Medium range Weather Forecast).

Signals of El Niño Modoki in the tropical tropopause layer and stratosphere

NASA Astrophysics Data System (ADS)

Xie, F.; Li, J.; Tian, W.; Feng, J.; Huo, Y.

2012-06-01

The effects of El Niño Modoki events on the tropical tropopause layer (TTL) and on the stratosphere were investigated using European Center for Medium Range Weather Forecasting (ECMWF) reanalysis data, oceanic El Niño indices, and general climate model outputs. El Niño Modoki events tend to depress convective activities in the western and eastern Pacific but enhance convective activities in the central and northern Pacific. Consequently, during El Niño Modoki events, negative water vapor anomalies occur in the western and eastern Pacific upper troposphere, whereas there are positive anomalies in the central and northern Pacific upper troposphere. The spatial patterns of the outgoing longwave radiation (OLR) and upper tropospheric water vapor anomalies exhibit a tripolar form. The empirical orthogonal function (EOF) analysis of the OLR and upper tropospheric water vapor anomalies reveals that canonical El Niño events are associated with the leading mode of the EOF, while El Niño Modoki events correspond to the second mode. The composite analysis based on ERA-interim data indicate that El Niño Modoki events have a reverse effect on middle-high latitudes stratosphere, as compared with the effect of typical El Niño events, i.e., the northern polar vortex is stronger and colder but the southern polar vortex is weaker and warmer during El Niño Modoki events. According to the simulation' results, we found that the reverse effect on the middle-high latitudes stratosphere is resulted from a complicated interaction between quasi-biennial oscillation (QBO) signal of east phase and El Niño Modoki signal. This interaction is not a simply linear overlay of QBO signal and El Niño Modoki signal in the stratosphere, it is El Niño Modoki that leads to different tropospheric zonal wind anomalies with QBO forcing from that caused by typical El Niño, thus, the planetary wave propagation from troposphere to the stratosphere during El Niño Modoki events is different from that during canonical El Niño events. However, when QBO is in its west phase, El Niño Modoki events have the same effect on middle-high latitudes stratosphere as the typical El Niño events. Our simulations also suggest that canonical El Niño and El Niño Modoki activities actually have the same influence on the middle-high latitudes stratosphere when in the absence of QBO forcing.

The Ozone Budget in the Upper Troposphere from Global Modeling Initiative (GMI)Simulations

NASA Technical Reports Server (NTRS)

Rodriquez, J.; Duncan, Bryan N.; Logan, Jennifer A.

2006-01-01

Ozone concentrations in the upper troposphere are influenced by in-situ production, long-range tropospheric transport, and influx of stratospheric ozone, as well as by photochemical removal. Since ozone is an important greenhouse gas in this region, it is particularly important to understand how it will respond to changes in anthropogenic emissions and changes in stratospheric ozone fluxes.. This response will be determined by the relative balance of the different production, loss and transport processes. Ozone concentrations calculated by models will differ depending on the adopted meteorological fields, their chemical scheme, anthropogenic emissions, and treatment of the stratospheric influx. We performed simulations using the chemical-transport model from the Global Modeling Initiative (GMI) with meteorological fields from (It)h e NASA Goddard Institute for Space Studies (GISS) general circulation model (GCM), (2) the atmospheric GCM from NASA's Global Modeling and Assimilation Office(GMAO), and (3) assimilated winds from GMAO . These simulations adopt the same chemical mechanism and emissions, and adopt the Synthetic Ozone (SYNOZ) approach for treating the influx of stratospheric ozone -. In addition, we also performed simulations for a coupled troposphere-stratosphere model with a subset of the same winds. Simulations were done for both 4degx5deg and 2degx2.5deg resolution. Model results are being tested through comparison with a suite of atmospheric observations. In this presentation, we diagnose the ozone budget in the upper troposphere utilizing the suite of GMI simulations, to address the sensitivity of this budget to: a) the different meteorological fields used; b) the adoption of the SYNOZ boundary condition versus inclusion of a full stratosphere; c) model horizontal resolution. Model results are compared to observations to determine biases in particular simulations; by examining these comparisons in conjunction with the derived budgets, we may pinpoint deficiencies in the representation of chemical/dynamical processes.

NASA's Upper Atmosphere Research Program (UARP) and Atmospheric Chemistry Modeling and Analysis Program (ACMAP): Research Summaries 1997-1999

NASA Technical Reports Server (NTRS)

Kurylo, M. J.; DeCola, P. L.; Kaye, J. A.

2000-01-01

Under the mandate contained in the FY 1976 NASA Authorization Act, the National Aeronautics and Space Administration (NASA) has developed and is implementing a comprehensive program of research, technology development, and monitoring of the Earth's upper atmosphere, with emphasis on the upper troposphere and stratosphere. This program aims at expanding our chemical and physical understanding to permit both the quantitative analysis of current perturbations as well as the assessment of possible future changes in this important region of our environment. It is carried out jointly by the Upper Atmosphere Research Program (UARP) and the Atmospheric Chemistry Modeling and Analysis Program (ACMAP), both managed within the Research Division in the Office of Earth Science at NASA. Significant contributions to this effort have also been provided by the Atmospheric Effects of Aviation Project (AEAP) of NASA's Office of Aero-Space Technology. The long-term objectives of the present program are to perform research to: understand the physics, chemistry, and transport processes of the upper troposphere and the stratosphere and their control on the distribution of atmospheric chemical species such as ozone; assess possible perturbations to the composition of the atmosphere caused by human activities and natural phenomena (with a specific emphasis on trace gas geographical distributions, sources, and sinks and the role of trace gases in defining the chemical composition of the upper atmosphere); understand the processes affecting the distributions of radiatively active species in the atmosphere, and the importance of chemical-radiative-dynamical feedbacks on the meteorology and climatology of the stratosphere and troposphere; and understand ozone production, loss, and recovery in an atmosphere with increasing abundances of greenhouse gases. The current report is composed of two parts. Part 1 summarizes the objectives, status, and accomplishments of the research tasks supported under NASA UARP and ACMAP in a document entitled, Research Summaries 1997- 1999. Part 2 is entitled Present State of Knowledge of the Upper Atmosphere 1999 An Assessment Report.

Wave Activity and Its Changes in the Troposphere and Stratosphere of the Northern Hemisphere in Winters of 1979-2016

NASA Astrophysics Data System (ADS)

Guryanov, V. V.; Eliseev, A. V.; Mokhov, I. I.; Perevedentsev, Yu. P.

2018-03-01

An analysis of spectra of wave disturbances with zonal wave numbers 1 ≤ k ≤ 10 is carried out using winter (November to March) ERA-Interim reanalysis geopotential data in the troposphere and stratosphere for 1979-2016. Contributions of eastward-traveling ( E), westward-traveling ( W), and stationary ( S) waves are estimated. The intensification of wave activity is observed in the tropical troposphere and stratosphere and in the upper stratosphere of the entire Northern Hemisphere. The intensification of wave activity in the tropics and subtropics is noted for waves of all types ( E, W, and S), while in the middle and higher latitudes it is related mainly to stationary and eastward waves. Near the subtropical tropopause, the energy of stationary waves has increased in recent decades. In addition, in the tropical and subtropical troposphere and in the subtropical lower stratosphere, the energy of the eastward-traveling waves in El Niño years may be one and a half times or twice the energy in La Niña years. The spectrally weighted zonal wave numbers for waves of all types ( E, W, and S) are the largest in the upper subtropical troposphere. The spectrally weighted zonal wave number for W and S waves is correlated with the Atlantic Multidecadal Oscillation index and varies by 15% in 1979-2016 (on an interdecadal time scale). The spectrally weighted wave period is larger in the stratosphere than in the troposphere. It is maximal in the middle extratropical stratosphere. The spectrally weighted wave periods correlate with the activity of sudden stratospheric warmings. The sign of this correlation depends on the latitude, atmospheric layer, and zonal wave number.

The environmental influence on tropical cyclone precipitation

NASA Technical Reports Server (NTRS)

Rodgers, Edward B.; Baik, Jong-Jin; Pierce, Harold F.

1994-01-01

The intensity, spatial, and temporal changes in precipitation were examined in three North Atlantic hurricanes during 1989 (Dean, Gabrielle, and Hugo) using precipitation estimates made from Special Sensor Microwave/Imager (SSM/I) measurements. In addition, analyses from a barotropic hurricane forecast model and the European Centre for Medium-Range Weather Forecast model were used to examine the relationship between the evolution of the precipitation in these tropical cyclones and external forcing. The external forcing parameters examined were (1) mean climatological sea surface temperatures, (2) vertical wind shear, (3) environmental tropospheric water vapor flux, and (4) upper-tropospheric eddy relative angular momentum flux convergence. The analyses revealed that (1) the SSM/I precipitation estimates were able to delineate and monitor convective ring cycles similar to those observed with land-based and aircraft radar and in situ measurements; (2) tropical cyclone intensification was observed to occur when these convective rings propagated into the inner core of these systems (within 111 km of the center) and when the precipitation rates increased; (3) tropical cyclone weakening was observed to occur when these inner-core convective rings dissipated; (4) the inward propagation of the outer convective rings coincided with the dissipation of the inner convective rings when they came within 55 km of each other; (5) in regions with the combined warm sea surface temperatures (above 26 C) and low vertical wind shear (less than 5 m/s), convective rings outside the region of strong lower-tropospheric inertial stability could be initiated by strong surges of tropospheric moisture, while convective rings inside the region of strong lower-tropospheric inertial stability could be enhanced by upper-tropospheric eddy relative angular momentum flux convergence.

The Environmental Influence on Tropical Cyclone Precipitation.

NASA Astrophysics Data System (ADS)

Rodgers, Edward B.; Baik, Jong-Jin; Pierce, Harold F.

1994-05-01

The intensity, spatial, and temporal changes in precipitation were examined in three North Atlantic hurricanes during 1989 (Dean, Gabrielle, and Hugo) using precipitation estimates made from Special Sensor Microwave/Imager (SSM/I) measurements. In addition, analyses from a barotropic hurricane forecast model and the European Centre for Medium-Range Weather Forecast model were used to examine the relationship between the evolution of the precipitation in these tropical cyclones and external forcing. The external forcing parameters examined were 1) mean climatological sea surface temperatures, 2) vertical wind shear, 3) environmental tropospheric water vapor flux, and 4) upper-tropospheric eddy relative angular momentum flux convergence.The analyses revealed that 1) the SSM/I precipitation estimates were able to delineate and monitor convective ring cycles similar to those observed with land-based and aircraft radar and in situ measurements; 2) tropical cyclone intensification was observed to occur when these convective rings propagated into the inner core of these systems (within 111 km of the center) and when the precipitation rates increased; 3) tropical cyclone weakening was observed to occur when these inner-core convective rings dissipated; 4) the inward propagation of the outer convective rings coincided with the dissipation of the inner convective rings when they came within 55 km of each other; 5) in regions with the combined warm sea surface temperatures (above 26°C) and low vertical wind shear (less than 5 m s1), convective rings outside the region of strong lower-tropospheric inertial stability could be initiated by strong surges of tropospheric moisture, while convective rings inside the region of strong lower-tropospheric inertial stability could be enhanced by upper-tropospheric eddy relative angular momentum flux convergence.

Radiative effects due to North American anthropogenic and lightning emissions: Global and regional modeling

NASA Astrophysics Data System (ADS)

Martini, Matus Novak

We analyze the contribution of North American (NA) lightning and anthropogenic emissions to summertime ozone concentrations, radiative forcing, and exports from North America using the global University of Maryland chemistry transport model (UMD-CTM) and the regional scale Weather Research and Forecasting model with chemistry (WRF-Chem). Lightning NO contributes by 15--20 ppbv to upper tropospheric ozone concentrations over the United States with the effects of NA lightning on ozone seen as far east as North Africa and Europe. Using the UMD-CTM, we compare changes in surface and column ozone amounts due to the NOx State Implementation Plan (SIP) Call with the natural variability in ozone due to changes in meteorology and lightning. Comparing early summer 2004 with 2002, surface ozone decreased by up to 5 ppbv due to the NO x SIP Call while changes in meteorology and lightning resulted in a 0.3--1.4 ppbv increase in surface ozone. Ozone column variability was driven primarily by changes in lightning NO emissions, especially over the North Atlantic. As part of our WRF-Chem analysis, we modify the radiation schemes to use model-calculated ozone (interactive ozone) instead of climatological ozone profiles and conduct multiple 4-day simulations of July 2007. We found that interactive ozone increased the outgoing longwave radiation (OLR) by 3 W m-2 decreasing the bias with respect to remotely sensed OLR. The improvement is due to a high bias in the climatological ozone profiles. The interactive ozone had a small impact on mean upper troposphere temperature (-0.15°C). The UMD-CTM simulations indicate that NA anthropogenic emissions are responsible for more ozone export but less ozone radiative forcing than lightning NO emissions. Over the North Atlantic, NA anthropogenic emissions contributed 0.15--0.30 W m-2 to the net downward radiative flux at the tropopause while NA lightning contributed 0.30--0.50 W m-2. The ozone export from anthropogenic emissions was almost twice as large as that from lightning emissions. The WRF-Chem simulations show that the export of reactive nitrogen was 23%--28% of the boundary layer emissions and 26%--38% of the total emissions including lightning NO.

Climatology 2011: An MLS and Sonde Derived Ozone Climatology for Satellite Retrieval Algorithms

NASA Technical Reports Server (NTRS)

McPeters, Richard D.; Labow, Gordon J.

2012-01-01

The ozone climatology used as the a priori for the version 8 Solar Backscatter Ultraviolet (SBUV) retrieval algorithms has been updated. The Microwave Limb Sounder (MLS) instrument on Aura has excellent latitude coverage and measures ozone daily from the upper troposphere to the lower mesosphere. The new climatology consists of monthly average ozone profiles for ten degree latitude zones covering pressure altitudes from 0 to 65 km. The climatology was formed by combining data from Aura MLS (2004-2010) with data from balloon sondes (1988-2010). Ozone below 8 km (below 12 km at high latitudes) is based on balloons sondes, while ozone above 16 km (21 km at high latitudes) is based on MLS measurements. Sonde and MLS data are blended in the transition region. Ozone accuracy in the upper troposphere is greatly improved because of the near uniform coverage by Aura MLS, while the addition of a large number of balloon sonde measurements improves the accuracy in the lower troposphere, in the tropics and southern hemisphere in particular. The addition of MLS data also improves the accuracy of climatology in the upper stratosphere and lower mesosphere. The revised climatology has been used for the latest reprocessing of SBUV and TOMS satellite ozone data.

Improved simulation of aerosol, cloud, and density measurements by shuttle lidar

NASA Technical Reports Server (NTRS)

Russell, P. B.; Morley, B. M.; Livingston, J. M.; Grams, G. W.; Patterson, E. W.

1981-01-01

Data retrievals are simulated for a Nd:YAG lidar suitable for early flight on the space shuttle. Maximum assumed vertical and horizontal resolutions are 0.1 and 100 km, respectively, in the boundary layer, increasing to 2 and 2000 km in the mesosphere. Aerosol and cloud retrievals are simulated using 1.06 and 0.53 microns wavelengths independently. Error sources include signal measurement, conventional density information, atmospheric transmission, and lidar calibration. By day, tenuous clouds and Saharan and boundary layer aerosols are retrieved at both wavelengths. By night, these constituents are retrieved, plus upper tropospheric, stratospheric, and mesospheric aerosols and noctilucent clouds. Density, temperature, and improved aerosol and cloud retrievals are simulated by combining signals at 0.35, 1.06, and 0.53 microns. Particlate contamination limits the technique to the cloud free upper troposphere and above. Error bars automatically show effect of this contamination, as well as errors in absolute density nonmalization, reference temperature or pressure, and the sources listed above. For nonvolcanic conditions, relative density profiles have rms errors of 0.54 to 2% in the upper troposphere and stratosphere. Temperature profiles have rms errors of 1.2 to 2.5 K and can define the tropopause to 0.5 km and higher wave structures to 1 or 2 km.

Vertical and meridional distributions of the atmospheric CO2 mixing ratio between northern midlatitudes and southern subtropics

NASA Astrophysics Data System (ADS)

Machida, T.; Kita, K.; Kondo, Y.; Blake, D.; Kawakami, S.; Inoue, G.; Ogawa, T.

2003-02-01

The atmospheric CO2 mixing ratio was measured using a continuous measurement system onboard a Gulfstream-II aircraft between the northern midlatitudes and the southern subtropics during the Biomass Burning and Lightning Experiment Phase A (BIBLE A) campaign in September-October 1998. The vertical distribution of CO2 over tropical regions was almost constant from the surface to an altitude of 13 km. CO2 enhancements from biomass burning and oceanic release were observed in the tropical boundary layer. Measurements in the upper troposphere indicate interhemispheric exchange was effectively suppressed between 2°N-7°N. Interhemispheric transport of air in the upper troposphere was suppressed effectively in this region. The CO2 mixing ratios in the Northern and Southern Hemispheres were almost constant, with an average value of about 365 parts per million (ppm) and 366 ppm, respectively. The correlation between the CO2 and NOy mixing ratios observed north of 7°N was apparently different from that obtained south of 2°N. This fact strongly supports the result that the north-south boundary in the upper troposphere during BIBLE A was located around 2°N-7°N as the boundary is not necessary a permanent feature.

Vertical and meridional distributions of the atmospheric CO2 mixing ratio between northern midlatitudes and southern subtropics

NASA Astrophysics Data System (ADS)

Machida, T.; Kita, K.; Kondo, Y.; Blake, D.; Kawakami, S.; Inoue, G.; Ogawa, T.

2002-02-01

The atmospheric CO2 mixing ratio was measured using a continuous measurement system onboard a Gulfstream-II aircraft between the northern midlatitudes and the southern subtropics during the Biomass Burning and Lightning Experiment Phase A (BIBLE A) campaign in September-October 1998. The vertical distribution of CO2 over tropical regions was almost constant from the surface to an altitude of 13 km. CO2 enhancements from biomass burning and oceanic release were observed in the tropical boundary layer. Measurements in the upper troposphere indicate interhemispheric exchange was effectively suppressed between 2°N-7°N. Interhemispheric transport of air in the upper troposphere was suppressed effectively in this region. The CO2 mixing ratios in the Northern and Southern Hemispheres were almost constant, with an average value of about 365 parts per million (ppm) and 366 ppm, respectively. The correlation between the CO2 and NOy mixing ratios observed north of 7°N was apparently different from that obtained south of 2°N. This fact strongly supports the result that the north-south boundary in the upper troposphere during BIBLE A was located around 2°N-7°N as the boundary is not necessary a permanent feature.

Influence of sudden stratospheric warming and quasi biennial oscillation on western disturbance over north India

NASA Astrophysics Data System (ADS)

Remya, R.; Kottayil, Ajil; Mohanakumar, K.

2017-07-01

This study demonstrates the variability in Western Disturbance during the sudden stratospheric warming (SSW) period and its eventual influence on the north Indian weather pattern. The modulations in the north Indian winter under the two phases of the Quasi-biennial oscillation (QBO) during SSW periods are also examined. The analysis has been carried out by using the ERA interim reanalysis dataset for different pressure levels in the stratosphere and upper troposphere during the time period of 1980-2010. The daily minimum surface temperature data published by India Meteorological Department from 1969 to 2013 has been used for the analysis of temperature anomaly over north India during SSW. The period of intense stratospheric warming witnesses a downward propagation and intensification of kinetic energy from stratosphere to upper troposphere over the Mediterranean and Caspian Sea. When QBO is in easterly phase, the cooling over north India is much larger when compared to the westerly phase during instances of SSW. SSW coincident with the easterly phase of QBO causes an intensified subtropical jet over the mid-latitude regions. The modulation in circulation pattern in stratosphere and upper troposphere when ENSO occurs during SSW period is also analysed separately. This study provides the link among SSW, Western Disturbances and the north Indian cooling during winter season.

Global budget of tropospheric ozone: Evaluating recent model advances with satellite (OMI), aircraft (IAGOS), and ozonesonde observations

NASA Astrophysics Data System (ADS)

Hu, Lu; Jacob, Daniel J.; Liu, Xiong; Zhang, Yi; Zhang, Lin; Kim, Patrick S.; Sulprizio, Melissa P.; Yantosca, Robert M.

2017-10-01

The global budget of tropospheric ozone is governed by a complicated ensemble of coupled chemical and dynamical processes. Simulation of tropospheric ozone has been a major focus of the GEOS-Chem chemical transport model (CTM) over the past 20 years, and many developments over the years have affected the model representation of the ozone budget. Here we conduct a comprehensive evaluation of the standard version of GEOS-Chem (v10-01) with ozone observations from ozonesondes, the OMI satellite instrument, and MOZAIC-IAGOS commercial aircraft for 2012-2013. Global validation of the OMI 700-400 hPa data with ozonesondes shows that OMI maintained persistent high quality and no significant drift over the 2006-2013 period. GEOS-Chem shows no significant seasonal or latitudinal bias relative to OMI and strong correlations in all seasons on the 2° × 2.5° horizontal scale (r = 0.88-0.95), improving on previous model versions. The most pronounced model bias revealed by ozonesondes and MOZAIC-IAGOS is at high northern latitudes in winter-spring where the model is 10-20 ppbv too low. This appears to be due to insufficient stratosphere-troposphere exchange (STE). Model updates to lightning NOx, Asian anthropogenic emissions, bromine chemistry, isoprene chemistry, and meteorological fields over the past decade have overall led to gradual increase in the simulated global tropospheric ozone burden and more active ozone production and loss. From simulations with different versions of GEOS meteorological fields we find that tropospheric ozone in GEOS-Chem v10-01 has a global production rate of 4960-5530 Tg a-1, lifetime of 20.9-24.2 days, burden of 345-357 Tg, and STE of 325-492 Tg a-1. Change in the intensity of tropical deep convection between these different meteorological fields is a major factor driving differences in the ozone budget.

Detection of Lightning-produced NOx by Air Quality Monitoring Stations in Israel

NASA Astrophysics Data System (ADS)

Yair, Y.; Shalev, S.; Saaroni, H.; Ziv, B.

2011-12-01

Lightning is the largest natural source for the production of nitrogen oxides (LtNOx) in the troposphere. Since NOx are greenhouse gases, it is important to know the global production rate of LtNOx for climate studies (present estimates range from 2 to 8 Tg per year) and to model its vertical distribution (Ott et al., 2010). One of the key factors for such an estimate is the yield of a single lightning flash, namely the number of molecules produced for each Joule of energy deposited along the lightning channel. We used lightning stroke data from the Israel Lightning Location System (ILLS) together with NOx data obtained from the national network of air quality monitoring stations operated by the Israeli Ministry of Environmental Protection. Looking for the fingerprints of LtNOx in the general ambient concentrations, usually most affected by pollution from urban sources, we looked only for CG strokes occurring within a radius of 3 km from the location of an air-quality monitoring station. This lowered the number of relevant cases from 605,413 strokes detected in the 2004/5 through 2009/10 seasons to 1,897 strokes. We applied a threshold of > 60kA reducing the number of events to 35. The results showed that there was no consistent rising trend in the NOx concentrations in the hour following the lightning (the lifetime near the ground is expected to be a few hours; Zhang et al., 2003). However, when considering only those events when the prevailing wind was in the direction from the stroke location toward the sensor (7 cases), a clear increase of few ppb following the stroke was observed in 5 cases [see Fig.]. This increase is well correlated with the wind speed, suggesting an effective transport from the stroke location to the sensor. Weaker winds allow dilution and result in smaller observed increases of LtNOx. Separate analysis of additional 17 cases in which the strokes were located < 500 m from the monitoring station (with any peak current above 7 kA) showed no consistent trend. When excluding the 7 events that occurred during rush hour traffic, we found 6 (of 10) cases with an average increase in NOx concentrations of 16 ppb in the hour following the lightning. These results suggest a contribution of CG lightning strokes to the ground level concentrations of NOx. L. E. Ott, K. E. Pickering, G. L. Stenchikov, D. J. Allen, A. J. DeCaria, B. Ridley, R.F. Lin, S. Lang, and W.K. Tao (2010), Production of lightning NOx and its vertical distribution calculated from three dimensional cloud scale chemical transport model simulations, J. Geophys. Res., 115, D04301, doi:10.1029/2009JD011880

Gravity Wave Variances and Propagation Derived from AIRS Radiances

DTIC Science & Technology

2011-04-15

synoptically warm condition and susequently affect ozone depletion (Hamill and Toon, 1991). The importance of gravity waves on climate and weather... troposphere to upper stratosphere can those GWs grow into significant strengths. Locations of high occurrence of convectively generated GWs are also...maximum comes in one month later. A close look at the vertical config- uration of the zonal wind reveals that tropospheric westerlies in the SH high

The Vertical Structure of Relative Humidity and Ozone in the Tropical Upper Troposphere: Intercomparisons Among In Situ Observations, A-Train Measurements and Large-Scale Models

NASA Technical Reports Server (NTRS)

Selkirk, Henry B.; Manyin, Michael; Douglass, Anne R.; Oman, Luke; Pawson, Steven; Ott, Lesley; Benson, Craig; Stolarski, Richard

2010-01-01

In situ measurements in the tropics have shown that in regions of active convection, relative humidity with respect to ice in the upper troposphere is typically close to saturation on average, and supersaturations greater than 20% are not uncommon. Balloon soundings with the cryogenic frost point hygrometer (CFH) at Costa Rica during northern summer, for example, show this tendency to be strongest between 11 and 15.5 km (345-360 K potential temperature, or approximately 250-120 hPa). this is the altitude range of deep convective detrainment. Additionally, simultaneous ozonesonde measurements show that stratospheric air (O3 greater than 150 ppbv) can be found as low as approximately 14 km (350 K/150 hPa). In contrast, results from northern winter show a much drier upper troposphere and little penetration of stratospheric air below the tropopause at 17.5 km (approximately 383 K). We show that these results are consistent with in situ measurements from the Measurement of Ozone and water vapor by Airbus In-service airCraft (MOZAIC) program which samples a wider, though still limited, range of tropical locations. To generalize to the tropics as a whole, we compare our insitu results to data from two A-Train satellite instruments, the Atmospheric Infrared Sounder (AIRS) and the Microwave Limb Sounder (MLS) on the Aqua and Aura satellites respectively. Finally, we examine the vertical structure of water vapor, relative humidity and ozone in the NASA Goddard MERRA analysis, an assimilation dataset, and a new version of the GEOS CCM, a free-running chemistry-climate model. We demonstrate that conditional probability distributions of relative humidity and ozone are a sensitive diagnostic for assessing the representation of deep convection and upper troposphere/lower stratosphere mixing processes in large-scale analyses and climate models.

A three-dimensional total odd nitrogen (NO y ) simulation during SONEX using a stretched-grid chemical transport model

NASA Astrophysics Data System (ADS)

Allen, Dale; Pickering, Kenneth; Stenchikov, Georgiy; Thompson, Anne; Kondo, Yutaka

2000-02-01

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 grid was chosen so that its maximum resolution is located over eastern North America and the North Atlantic; a region that includes most of the Subsonic Assessment (SASS) Ozone and Nitrogen Oxide Experiment (SONEX) flight paths. The SONEX period (October-November 1997) is simulated by driving the SG-GCTM with assimilated data from the Goddard Earth Observing System-Stratospheric Tracers of Atmospheric Transport Data Assimilation System (GEOS-STRAT DAS). A new algorithm is used to estimate the lightning flash rates needed to calculate NOy emission by lightning. This algorithm parameterizes the flash rate in terms of upper tropospheric convective mass flux. 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 peaks due to "stratospheric" NOy are occasionally too large. The lightning algorithm reproduces the temporally and spatially averaged total flash rate accurately; however, the use of emissions from observed lightning flashes significantly improves the simulation on a few days, especially November 3, 1997, showing that significant uncertainty remains in parameterizing lightning in chemistry and transport models. Aircraft emissions contributed ˜15% of the upper tropospheric NOy averaged along SONEX flight paths within the North Atlantic Flight Corridor with the contribution exceeding 40% during portions of some flights.