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  • 1
    Electronic Resource
    Electronic Resource
    Distribution of222Rn over the north Pacific: Implications for continental influences (1992)
    Springer
    Journal of atmospheric chemistry 14 (1992), S. 353-374 
    Details
    ISSN: 1573-0662
    Keywords: North Pacific ; global atmospheric chemistry ; modeling ; radon
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract The atmospheric distribution of222Rn over the north Pacific is simulated with a three-dimensional chemical tracer model using meteorological input from the NASA-GISS general circulation model (4°×5° resolution). Radon-222 (half-life 3.8 days) is a tracer of continental air. Model results are in good agreement with measurements from ships and aircraft. Strong Asian influence is found throughout the tropospheric column over the north Pacific in spring, reflecting a combination of frequent convection over the continent, strong westerly winds at altitude, and subsidence over the ocean. In summer, the upper troposphere over the north Pacific is heavily affected by deep convection over China; however, Asian influences at the surface are then at their yearly minimum. In winter, strong Asian influence is found near the surface but not at high altitudes. Transport of American air over the Pacific is important only at low latitudes. American sources account for 11% of total222Rn in the model at Midway, 30% at Mauna Loa and 59% at Oahu. Results for Hawaii indicate two seasonal peaks of American influence, one in summer and one in winter. The tropical western Pacific is particularly remote from continental influences year round.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1007/BF00115244
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  • 2
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    Global Modeling of Tropospheric Chemistry with Assimilated Meteorology: Model Description and Evaluation (2001)
    In:  Other Sources
    Details
    Publication Date: 2019-07-13
    Description: We present a first description and evaluation of GEOS-CHEM, a global three-dimensional (3-D) model of tropospheric chemistry driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS) of the NASA Data Assimilation Office (DAO). The model is applied to a 1-year simulation of tropospheric ozone-NOx-hydrocarbon chemistry for 1994, and is evaluated with observations both for 1994 and for other years. It reproduces usually to within 10 ppb the concentrations of ozone observed from the worldwide ozonesonde data network. It simulates correctly the seasonal phases and amplitudes of ozone concentrations for different regions and altitudes, but tends to underestimate the seasonal amplitude at northern midlatitudes. Observed concentrations of NO and peroxyacetylnitrate (PAN) observed in aircraft campaigns are generally reproduced to within a factor of 2 and often much better. Concentrations of HNO3 in the remote troposphere are overestimated typically by a factor of 2-3, a common problem in global models that may reflect a combination of insufficient precipitation scavenging and gas-aerosol partitioning not resolved by the model. The model yields an atmospheric lifetime of methylchloroform (proxy for global OH) of 5.1 years, as compared to a best estimate from observations of 5.5 plus or minus 0.8 years, and simulates H2O2 concentrations observed from aircraft with significant regional disagreements but no global bias. The OH concentrations are approximately 20% higher than in our previous global 3-D model which included an UV-absorbing aerosol. Concentrations of CO tend to be underestimated by the model, often by 10-30 ppb, which could reflect a combination of excessive OH (a 20% decrease in model OH could be accommodated by the methylchloroform constraint) and an underestimate of CO sources (particularly biogenic). The model underestimates observed acetone concentrations over the South Pacific in fall by a factor of 3; a missing source from the ocean may be implicated.
    Keywords: Meteorology and Climatology
    Type: Paper 2001JD000807 , (ISSN 0148-0227)
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  • 3
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    Interpretation of TOMS Observations of Tropical Tropospheric Ozone with a Global Model and In Situ Observations (2004)
    In:  CASI
    Details
    Publication Date: 2019-07-13
    Description: 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.
    Keywords: Meteorology and Climatology
    Type: Journal of Geophysical Research (ISSN 0148-0227); 107; D18; 4-1 - 4-19
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  • 4
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    Mapping Isoprene Emissions over North America using Formaldehyde Column Observations from Space (2004)
    In:  Other Sources
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    Publication Date: 2019-07-13
    Description: I] We present a methodology for deriving emissions of volatile organic compounds (VOC) using space-based column observations of formaldehyde (HCHO) and apply it to data from the Global Ozone Monitoring Experiment (GOME) satellite instrument over North America during July 1996. The HCHO column is related to local VOC emissions, with a spatial smearing that increases with the VOC lifetime. lsoprene is the dominant HCHO precursor over North America in summer, and its lifetime (approx. = 1 hour) is sufficiently short that the smearing can be neglected. We use the Goddard Earth Observing System global 3-D model of tropospheric chemistry (GEOS-CHEM) to derive the relationship between isoprene emissions and HCHO columns over North America and use these relationships to convert the GOME HCHO columns to isoprene emissions. We also use the GEOS-CHEM model as an intermediary to validate the GOME HCHO column measurements by comparison with in situ observations. The GEOS-CHEM model including the Global Emissions Inventory Activity (GEIA) isoprene emission inventory provides a good simulation of both the GOME data (r(sup 2) = 0.69, n = 756, bias = +l1 %) and the in situ summertime HCHO measurements over North America (r(sup 2) = 0.47, n = 10, bias = -3%). The GOME observations show high values over regions of known high isoprene emissions and a day-to-day variability that is consistent with the temperature dependence of isoprene emission. Isoprene emissions inferred from the GOME data are 20% less than GEIA on average over North America and twice those from the U S . EPA Biogenic Emissions Inventory System (BEIS2) inventory. The GOME isoprene inventory when implemented in the GEOS-CHEM model provides a better simulation of the HCHO in situ measurements thaneitherGEIAorBEIS2 (r(sup 2) = 0.71,n= 10, bias = -10 %).
    Keywords: Meteorology and Climatology
    Type: Journal of Geophysical Research; 108; D6; 2-1 - 2-9
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  • 5
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    The Role of Lightning in Controlling Interannual Variability of Tropical Tropospheric Ozone and OH and its Implications for Climate (2012)
    In:  CASI
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    Publication Date: 2019-07-19
    Description: Nitrogen oxides (NO(x) = NO + NO2) produced by lightning make a major contribution to the production of the dominant tropospheric oxidants (OH and ozone). These oxidants control the lifetime of many trace gases including long-lived greenhouse gases, and control the source-receptor relationship of inter-hemispheric pollutant transport. Lightning is affected by meteorological variability, and therefore represents a potentially important tropospheric chemistry-climate feedback. Understanding how interannual variability (IAV) in lightning affects IAV in ozone and OH in the recent past is important if we are to predict how oxidant levels may change in a future warmer climate. However, lightning parameterizations for chemical transport models (CTMs) show low skill in reproducing even climatological distributions of flash rates from the Lightning Imaging Sensor (LIS) and the Optical Transient Detector (OTD) satellite instruments. We present an optimized regional scaling algorithm for CTMs that enables sufficient sampling of spatiotemporally sparse satellite lightning data from LIS to constrain the spatial, seasonal, and interannual variability of tropical lightning. We construct a monthly time series of lightning flash rates for 1998-2010 and 35degS-35degN, and find a correlation of IAV in total tropical lightning with El Nino. We use the IAV-constraint to drive a 9-year hindcast (1998-2006) of the GEOS-Chem 3D chemical transport model, and find the increased IAV in LNO(x) drives increased IAV in ozone and OH, improving the model fs ability to simulate both. Although lightning contributes more than any other emission source to IAV in ozone, we find ozone more sensitive to meteorology, particularly convective transport. However, we find IAV in OH to be highly sensitive to lightning NO(x), and the constraint improves the ability of the model to capture the temporal behavior of OH anomalies inferred from observations of methyl chloroform and other gases. The sensitivity of OH is explained using photochemical reaction rates which show a "magnification" effect of the initial lightning NO perturbation on OH primary production, HO(x) recycling, and OH loss frequencies. This influence on OH may represent a negative feedback, if lightning increases in a warming world..
    Keywords: Meteorology and Climatology
    Type: M12-2030 , American Geophysical Union (AGU) 45th Annual Fall Meeting; Dec 03, 2012 - Dec 07, 2012; San Francisco, CA; United States
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  • 6
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    Errors and Improvements in the Use of Archived Meteorological Data for Chemical Transport Modeling: An Analysis Using GEOS-Chem V11-01 Driven by GEOS-5 Meteorology (2018)
    In:  CASI
    Details
    Publication Date: 2019-07-13
    Description: Global simulations of atmospheric chemistry are commonly conducted with off-line chemical transport models (CTMs) driven by archived meteorological data from general circulation models (GCMs). The off-line approach has the advantages of simplicity and expediency, but it incurs errors due to temporal averaging in the meteorological archive and the inability to reproduce the GCM transport algorithms exactly. The CTM simulation is also often conducted at coarser grid resolution than the parent GCM. Here we investigate this cascade of CTM errors by using (exp 222)Rn(exp 210)Pb(exp 7)Be chemical tracer simulations off-line in the GEOS-Chem CTM at rectilinear 0.250.3125 (25km) and 22.5 (200km) resolutions and online in the parent GEOS-5 GCM at cubed-sphere c360 (25km) and c48 (200km) horizontal resolutions. The c360 GEOS-5 GCM meteorological archive, updated every 3h and remapped to 0.250.3125, is the standard operational product generated by the NASA Global Modeling and Assimilation Office (GMAO) and used as input by GEOS-Chem. We find that the GEOS-Chem (exp 222)Rn simulation at native 0.250.3125 resolution is affected by vertical transport errors of up to 20% relative to the GEOS-5 c360 online simulation, in part due to loss of transient organized vertical motions in the GCM (resolved convection) that are temporally averaged out in the 3h meteorological archive. There is also significant error caused by operational remapping of the meteorological archive from a cubed-sphere to a rectilinear grid. Decreasing the GEOS-Chem resolution from 0.250.3125 to 22.5 induces further weakening of vertical transport as transient vertical motions are averaged out spatially and temporally. The resulting (exp 222)Rn concentrations simulated by the coarse-resolution GEOS-Chem are overestimated by up to 40% in surface air relative to the online c360 simulations and underestimated by up to 40% in the upper troposphere, while the tropospheric lifetimes of (exp 210)Pb and (exp 7)Be against aerosol deposition are affected by 510%. The lost vertical transport in the coarse-resolution GEOS-Chem simulation can be partly restored by recomputing the convective mass fluxes at the appropriate resolution to replace the archived convective mass fluxes and by correcting for bias in the spatial averaging of boundary layer mixing depths.
    Keywords: Meteorology and Climatology
    Type: GSFC-E-DAA-TN52078 , Geoscientific Model Development (ISSN 1991-959X) (e-ISSN 1991-9603); 11; 1; 305-319
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  • 7
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    Constraints Pb-210 and Be-7 on Wet Deposition and Transport in a Global Three-Dimensional Chemical Tracer Model Driven by Assimilated Meteorological Fields (2001)
    In:  Other Sources
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    Publication Date: 2019-07-13
    Description: The atmospheric distributions of the aerosol tracers Pb-210 and Be-7 are simulated with a global three-dimensional model driven by assimilated meteorological observations for 1991-1996 from the NASA Goddard Earth Observing System (GEOSl). The combination of terrigenic Pb-210 and cosmogenic Be-7 provides a sensitive test of wet deposition and vertical transport in the model. Our simulation of moist transport and removal includes scavenging in wet convective updrafts (40% scavenging efficiency per kilometer of updraft), midlevel entrainment and detrainment, first-order rainout and washout from both convective anvils and large-scale precipitation, and cirrus precipitation. Observations from surface sites in specific years are compared to model results for the corresponding meteorological years, and observations from aircraft missions over the Pacific are compared to model results for the days of the flights. Initial simulation of Be-7 showed that cross-tropopause transport in the GEOSl meteorological fields is too fast by a factor of 3-4. We adjusted the stratospheric Be-7 source to correct the tropospheric simulation. Including this correction, we find that the model gives a good simulation of observed Pb-210 and Be-7 concentrations and deposition fluxes at surface sites worldwide, with no significant global bias and with significant success in reproducing the observed latitudinal and seasonal distributions. We achieve several improvements over previous models; in particular, we reproduce the observed Be-7 minimum in the tropics and show that its simulation is sensitive to rainout from convective anvils. Comparisons with aircraft observations up to 12-km altitude suggest that cirrus precipitation could be important for explaining the low concentrations in the middle and upper troposphere.
    Keywords: Meteorology and Climatology
    Type: Paper 2000JD900839 , Journal of Geophysical Research (ISSN 0148-0227); 106; D11; 12109-12128
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  • 8
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    Why do Models Overestimate Surface Ozone in the Southeastern United States? (2016)
    In:  CASI
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    Publication Date: 2019-07-13
    Description: 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 deg. x 0.3125 deg. 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 15 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.
    Keywords: Meteorology and Climatology
    Type: GSFC-E-DAA-TN41263 , Atmospheric Chemistry and Physics (ISSN 1680-7316) (e-ISSN 1680-7324); 16; 21; 13561-13577
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  • 9
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    First Directly Retrieved Global Distribution of Tropospheric Column Ozone from GOME: Comparison with the GEOS-CHEM Model (2006)
    In:  Other Sources
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    Publication Date: 2019-07-13
    Description: We present the first directly retrieved global distribution of tropospheric column ozone from Global Ozone Monitoring Experiment (GOME) ultraviolet measurements during December 1996 to November 1997. The retrievals clearly show signals due to convection, biomass burning, stratospheric influence, pollution, and transport. They are capable of capturing the spatiotemporal evolution of tropospheric column ozone in response to regional or short time-scale events such as the 1997-1998 El Nino event and a 10-20 DU change within a few days. The global distribution of tropospheric column ozone displays the well-known wave-1 pattern in the tropics, nearly zonal bands of enhanced tropospheric column ozone of 36-48 DU at 20degS-30degS during the austral spring and at 25degN-45degN during the boreal spring and summer, low tropospheric column ozone of 〈30 DU uniformly distributed south of 35 S during all seasons, and relatively high tropospheric column ozone of 〉33 DU at some northern high-latitudes during the spring. Simulation from a chemical transport model corroborates most of the above structures, with small biases of 〈+/-5 DU and consistent seasonal cycles in most regions, especially in the southern hemisphere. However, significant positive biases of 5-20 DU occur in some northern tropical and subtropical regions such as the Middle East during summer. Comparison of GOME with monthly-averaged Measurement of Ozone and Water Vapor by Airbus in-service Aircraft (MOZAIC) tropospheric column ozone for these regions usually shows good consistency within 1 a standard deviations and retrieval uncertainties. Some biases can be accounted for by inadequate sensitivity to lower tropospheric ozone, the different spatiotemporal sampling and the spatiotemporal variations in tropospheric column ozone.
    Keywords: Meteorology and Climatology
    Type: Journal of Geophysical Research: Atmospheres; 111
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