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Duncan, Bryan N.

Publications and source records attributed to Duncan, Bryan N..

33 records · Page 2

High-Frequency Measurements of Methane Ebullition Over a Growing Season at a Temperate Peatland Site

Bubbles can contribute a significant fraction of methane emissions fr om wetlands; however the range of reported fractions is very large an d accurate characterization of this pathway has proven difficult. Her e we show that continuous automated flux chambers combined with an in tegrated cavity output spectroscopy (ICOS) instrument allow us to qua ntify both CH4 ebullition rate and magnitude. For a temperate poor f en in 2009, ebullition rate varied on hourly to seasonal time scales. A diel pattern in ebullition was identified with peak release occurr ing between 20:00 and 06:00 local time, though steady fluxes (i.e., t hose with a linear increase in chamber headspace CH4 concentration) d id not exhibit diel variability. Seasonal mean ebullition rates peake d at 843.5 +/- 384.2 events m(exp -2)/d during the summer, with a me an magnitude of 0.19 mg CH4 released in each event.

Goodrich, Jordan P.↗

The Utility of the OMI HCHO and NO2 Data Products in Air Quality Decision- Making Activities

We will present three related air quality applications of the OMI HCHO (formaldehyde) and NO2 (nitrogen dioxide) data products, which we us to support mission planning of an OMI-like instrument for the proposed GEO-CAPE satellite that has as one of its objectives to study air quality from space. First, we will discuss a novel and practical application of the data products to the "weight of evidence" in the air quality decision-making process (e.g., State Implementation Plan (SIP)) for a city, region, or state to demonstrate that it is making progress toward attainment of the National Ambient Air Quality Standard (NAAQS) for ozone. Any trend, or lack thereof, in the observed OMI HCHO/NO2, which we use as an air quality indicator, may support that an emission control strategy implemented to reduce ozone is or is not occurring for a metropolitan area. Second, we will discuss how we use variations in the OMI HCHO product as a proxy for variability in the biogenic hydrocarbon, isoprene, which is an important player for the formation of high levels of ozone and the dominant source of HCHO in the eastern U.S. Third, we will discuss the variability of NO2 in the U.S. as indicated by the OMI NO2 product. In addition, we will show the impact of the 2005 hurricanes on pollutant emissions, including those associated with the intensive oil extraction and refining activities, in the Gulf of Mexico region using the OMI NO2 product. The variability of HCHO and NO2 as indicated by OMI helps us to understand changes in the OMI HCHO/NO2 and the implications for ozone formation.

Duncan, Bryan N.↗

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

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

Duncan, Bryan N.↗

Satellite Observation Highlights of the 2010 Russian Wildfires

From late-July through mid-August 2010, wildfires raged in western Russia. The resulting thick smoke and biomass burning products were transported over the highly populated Moscow city and surrounding regions, seriously impairing visibility and affecting human health. We demonstrate the uniqueness of the 2010 Russian wildfires by using satellite observations from NASA's Earth Observing System (EOS) platforms. Over Moscow and the region of major fire activity to the southeast, we calculate unprecedented increases in the MODIS fire count record of 178 %, an order of magnitude increase in the MODIS fire radiative power (308%) and OMI absorbing aerosols (255%), and a 58% increase in AIRS total carbon monoxide (CO). The exceptionally high levels of CO are shown to be of comparable strength to the 2006 El Nino wildfires over Indonesia. Both events record CO values exceeding 30x10(exp 7) molec/ square cm.

Witte, Jacquelyn C.↗

Sensitivity of Photolysis Frequencies and Key Tropospheric Oxidants in a Global Model to Cloud Vertical Distributions and Optical Properties

Clouds affect tropospheric photochemistry through modification of solar radiation that determines photolysis frequencies. As a follow-up study to our recent assessment of the radiative effects of clouds on tropospheric chemistry, this paper presents an analysis of the sensitivity of such effects to cloud vertical distributions and optical properties (cloud optical depths (CODs) and cloud single scattering albedo), in a global 3-D chemical transport model (GEOS-Chem). GEOS-Chem was driven with a series of meteorological archives (GEOS1- STRAT, GEOS-3 and GEOS-4) generated by the NASA Goddard Earth Observing System data assimilation system. Clouds in GEOS1-STRAT and GEOS-3 have more similar vertical distributions (with substantially smaller CODs in GEOS1-STRAT) while those in GEOS-4 are optically much thinner in the tropical upper troposphere. We find that the radiative impact of clouds on global photolysis frequencies and hydroxyl radical (OH) is more sensitive to the vertical distribution of clouds than to the magnitude of column CODs. With random vertical overlap for clouds, the model calculated changes in global mean OH (J(O1D), J(NO2)) due to the radiative effects of clouds in June are about 0.0% (0.4%, 0.9%), 0.8% (1.7%, 3.1%), and 7.3% (4.1%, 6.0%), for GEOS1-STRAT, GEOS-3 and GEOS-4, respectively; the geographic distributions of these quantities show much larger changes, with maximum decrease in OH concentrations of approx.15-35% near the midlatitude surface. The much larger global impact of clouds in GEOS-4 reflects the fact that more solar radiation is able to penetrate through the optically thin upper-tropospheric clouds, increasing backscattering from low-level clouds. Model simulations with each of the three cloud distributions all show that the change in the global burden of ozone due to clouds is less than 5%. Model perturbation experiments with GEOS-3, where the magnitude of 3-D CODs are progressively varied from -100% to 100%, predict only modest changes (<5%) in global mean OH concentrations. J(O1D), J(NO2) and OH3 concentrations show the strongest sensitivity for small CODs and become insensitive at large CODs due to saturation effects. Caution should be exercised not to use in photochemical models a value for cloud single scattering albedo lower than about 0.999 in order to be consistent with the current knowledge of cloud absorption at the ultraviolet wavelengths.

Liu, Hongyu↗

Temperature Dependence of Factors Controlling Isoprene Emissions

We investigated the relationship of variability in the formaldehyde (HCHO) columns measured by the Aura Ozone Monitoring Instrument (OMI) to isoprene emissions in the southeastern United States for 2005-2007. The data show that the inferred, regional-average isoprene emissions varied by about 22% during summer and are well correlated with temperature, which is known to influence emissions. Part of the correlation with temperature is likely associated with other causal factors that are temperature-dependent. We show that the variations in HCHO are convolved with the temperature dependence of surface ozone, which influences isoprene emissions, and the dependence of the HCHO column to mixed layer height as OMI's sensitivity to HCHO increases with altitude. Furthermore, we show that while there is an association of drought with the variation in HCHO, drought in the southeastern U.S. is convolved with temperature.

Duncan, Bryan N.↗

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

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

Duncan, Bryan N.↗

Performance of Versions 1,2 and 3 of the Goddard Earth Observing System (GEOS) Chemistry-Climate Model (CCM)

Version 1 of the Goddard Earth Observing System Chemistry-Climate Model (GEOS CCM) was used in the first CCMVa1 model evaluation and forms the basis for several studies of links between ozone and the circulation. That version of the CCM was based on the GEOS-4 GCM. Versions 2 and 3 of the GEOS CCM are based on the GEOS-5 GCM, which retains the "Lin-Rood" dynamical core but has a totally different set of physical parameterizatiOns to GEOS-4. In Version 2 of the GEOS CCM the Goddard stratospheric chemistry module is retained. Difference between Versions 1 and 2 thus reflect the physics changes of the underlying GCMs. Several comparisons between these two models are made, several of which reveal improvements in Version 2 (including a more realistic representation of the interannual variability of the Antarctic vortex). In Version 3 of the GEOS CCM, the stratospheric chemistry mechanism is replaced by the "GMI COMBO" code that includes tropospheric chemistry and different computational approaches. An advantage of this model version. is the reduction of high ozone biases that prevail at low chlorine loadings in Versions 1 and 2. This poster will compare and contrast various aspects of the three model versions that are relevant for understanding interactions between ozone and climate.

Pawson, Steven↗

Sensitivity of Photolysis Frequencies and Key Tropospheric Oxidants in a Global Model to Cloud Vertical Distributions and Optical Properties

As a follow-up study to our recent assessment of the radiative effects of clouds on tropospheric chemistry, this paper presents an analysis of the sensitivity of such effects to cloud vertical distributions and optical properties in a global 3-D chemical transport model (GEOS4-Chem CTM). GEOS-Chem was driven with a series of meteorological archives (GEOS1-STRAT, GEOS-3 and GEOS-4) generated by the NASA Goddard Earth Observing System data assimilation system, which have significantly different cloud optical depths (CODs) and vertical distributions. Clouds in GEOS1-STRAT and GEOS-3 have more similar vertical distributions while those in GEOS-4 are optically much thinner in the tropical upper troposphere. We find that the radiative impact of clouds on global photolysis frequencies and hydroxyl radical (OH) is more sensitive to the vertical distribution of clouds than to the magnitude of column CODs. Model simulations with each of the three cloud distributions all show that the change in the global burden of O3 due to clouds is less than 5%. Model perturbation experiments with GEOS-3, where the magnitude of 3-D CODs are progressively varied by -100% to 100%, predict only modest changes (<5%) in global mean OH concentrations. J(O1D), J(NO2) and OH concentrations show the strongest sensitivity for small CODs and become insensitive at large CODs due to saturation effects. Caution should be exercised not to use in photochemical models a value for cloud single scattering albedo lower than about 0.999 in order to be consistent with the current knowledge of cloud absorption at the UV wavelength. Our results have important implications for model intercomparisons and climate feedback on tropospheric photochemistry.

Liu, Hongyu↗

Compilation of a Global Emission Inventory from 1980 to 2000 for Global Model Simulations of the Long-term Trend of Tropospheric Aerosols

The approach to create a comprehensive emission inventory for the time period 1980 to 2000 is described in this paper. We have recently compiled an emission database, which we will use for a 21 year simulation of tropospheric aerosols with the GOCART model. Particular attention was paid to the time-dependent SO2, black carbon and organic carbon aerosol emissions. For the emission of SO2 from sporadically erupting volcanoes, we assembled emission data from the Global Volcanism Program of the Smithsonian Institution, using the VEI to derive the volcanic cloud height and the SO2 amount, and amended this dataset by the SO2 emission data from the TOMS instrument when available. 3-dimensional aircraft emission data was obtained for a number of years from the AEAP project, converted from burned fuel to SO2 and interpolated to each year, taking the sparsity of the flight patterns into account. Other anthropogenic SO2 emissions are based on gridded emissions from the EDGAR 2000 database (excluding sources from aircraft, biomass burning and international ship traffic), which were scaled to individual years with country/regional based emission inventories. Gridded SO2 emissions from international ship traffic for 2000 and the scaling factors for other years are from [Eyring et al., 2005]. We used gridded anthropogenic black and organic carbon emissions for 1996 [Bond et al., 2005], again excluding aircraft, biomass burning and ship sources. These emissions were scaled with regional based emission inventories from 1980 to 2000 to derive gridded emissions for each year. The biomass burning emissions are based on a climatology, which is scaled with regional scaling factors derived from the TOMS aerosol index and the AVHRR/ASTR fire counts to each year [Duncan et al., 2003]. Details on the integration of the information from the various sources will be provided and the distribution patterns and total emissions in the final product will be discussed.

Diehl, Thomas L.↗

The Ozone Budget in the Upper Troposphere from Global Modeling Initiative (GMI)Simulations

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.

Rodriquez, J.↗

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

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.

Martin, Randall V.↗

Transport Pathways for Asian Pollution Outflow Over the Pacific: Interannual and Seasonal Variations

The meteorological pathways contributing to Asian pollution outflow over the Pacific are examined with a global three-dimensional model analysis of CO observations from the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission (February-April 2001). The model is used also to place the TRACE-P observations in an interannual (1994-2001) and seasonal context. The major process driving Asian pollution outflow in spring is frontal lifting ahead of southeastward-moving cold fronts (the leading edge of cold surges) and transport in the boundary layer behind the cold fronts. Orographic lifting over central and eastern China combines with the cold fronts to promote the transport of Chinese pollution to the free troposphere. Outflow of seasonal biomass burning in Southeast Asia during spring takes place mostly by deep convection but also by northeastward transport and frontal lifting, mixing with the anthropogenic outflow. Boundary layer outflow over the western Pacific is largely devoid of biomass burning influence. European and African (biomass burning) plumes in Asian outflow during TRACE-P were weak (less than 60 ppbv and 20 ppbv CO, respectively) and were not detectable in the observations because of superposition of the much larger Asian pollution signal. Spring 2001 (La Nina) was characterized by unusually frequent cold surge events in the Asian Pacific rim and strong convection in Southeast Asia, leading to unusually strong boundary layer outflow of anthropogenic emissions and convective outflow of biomass burning emissions in the upper troposphere. The Asian outflow flux of CO to the Pacific is found to vary seasonally by a factor of 3-4 (maximum in March and minimum in summer). The March maximum results from frequent cold surge events and seasonal biomass burning emissions.

Liu, Hong-Yu↗

Interannual and Seasonal Variability of Biomass Burning Emissions Constrained by Satellite Observations

We present a methodology for estimating the seasonal and interannual variation of biomass burning designed for use in global chemical transport models. The average seasonal variation is estimated from 4 years of fire-count data from the Along Track Scanning Radiometer (ATSR) and 1-2 years of similar data from the Advanced Very High Resolution Radiometer (AVHRR) World Fire Atlases. We use the Total Ozone Mapping Spectrometer (TOMS) Aerosol Index (AI) data product as a surrogate to estimate interannual variability in biomass burning for six regions: Southeast Asia, Indonesia and Malaysia, Brazil, Central America and Mexico, Canada and Alaska, and Asiatic Russia. The AI data set is available from 1979 to the present with an interruption in satellite observations from mid-1993 to mid-1996; this data gap is filled where possible with estimates of area burned from the literature for different regions. Between August 1996 and July 2000, the ATSR fire-counts are used to provide specific locations of emissions and a record of interannual variability throughout the world. We use our methodology to estimate mean seasonal and interannual variations for emissions of carbon monoxide from biomass burning, and we find that no trend is apparent in these emissions over the last two decades, but that there is significant interannual variability.

Duncan, Bryan N.↗

Sources of Tropospheric Ozone along the Asian Pacific Rim: An Analysis of Ozonesonde Observations

The sources contributing to tropospheric ozone over the Asian Pacific Rim in different seasons are quantified by analysis of Hong Kong and Japanese ozonesonde observations with a global three-dimensional (3-D) chemical transport model (GEOS-CHEM) driven by assimilated meteorological observations. Particular focus is placed on the extensive observations available from Hong Kong in 1996. In the middle-upper troposphere (MT- UT), maximum Asian pollution influence along the Pacific Rim occurs in summer, reflecting rapid convective transport of surface pollution. In the lower troposphere (LT) the season of maximum Asian pollution influence shifts to summer at midlatitudes from fall at low latitudes due to monsoonal influence. The UT ozone minimum and high variability observed over Hong Kong in winter reflects frequent tropical intrusions alternating with stratospheric intrusions. Asian biomass burning makes a major contribution to ozone at less than 32 deg.N in spring. Maximum European pollution influence (less than 5 ppbv) occurs in spring in the LT. North American pollution influence exceeds European influence in the UT-MT, reflecting the uplift from convection and the warm conveyor belts over the eastern seaboard of North America. African outflow makes a major contribution to ozone in the low-latitude MT-UT over the Pacific Rim during November- April. Lightning influence over the Pacific Rim is minimum in summer due to westward UT transport at low latitudes associated with the Tibetan anticyclone. The Asian outflow flux of ozone to the Pacific is maximum in spring and fall and includes a major contribution from Asian anthropogenic sources year-round.

Liu, Hong-Yu↗