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Martin, Randall V.

Publications and source records attributed to Martin, Randall V..

32 records · Page 2

Remote Sensing of Tropospheric Pollution from Space

We review the progress of tropospheric trace gas observations and address the need for additional measurement capabilities as recommended by the National Academy of Science (NAS, 2007). Tropospheric measurements from current and earlier instruments show pollution in the Northern Hemisphere as a result of fossil fuel burning and a strong seasonal dependence with the largest amounts of photochemically-generated ozone in summer. At low latitudes, where photon flux is stronger throughout the year, trace gas concentrations are driven by the abundance of the emissions, where the largest source, biomass burning, is readily seen in carbon monoxide measurements, but lightning and biogenic trace gases may also contribute to trace gas variability. Although substantive progress has been achieved in seasonal and global mapping of a few tropospheric trace gases, satellite trace-gas observations with considerably better temporal and spatial resolution are essential to forecasting air quality at scales required by policy-makers. The concurrent use of atmospheric composition measurements for both scientific and operational purposes is a new paradigm for the atmospheric chemistry community. The examples presented illustrate both the promise and challenge of merging satellite information with in situ observations in state-of-the-art data assimilation models.

Fishman, Jack↗

Space-Based Constraints on the Production of Nitric Oxide by Lightning

.We interpret observations of trace-gases from three satellite platforms to provide top-down constraints on the production of NO by lightning. The space-based observations are tropospheric NO2 columns from SCIAMACHY, tropospheric O3 columns from OMI and MLS, and upper tropospheric HNO3 from ACE-FTS. A global chemical transport model (GEOS-Chem) is used to identify locations and time periods in which lightning would be expected to dominate the trace gas observations. The satellite observations are sampled at those locations and time periods. All three observations exhibit a maximum in the tropical Atlantic region and a minimum in the tropical Pacific. This wave-1 pattern is driven by injection of lightning NO into the upper troposphere over the tropical continents, followed by photochemical production of NO2, HNO3, and O3 during transport. Lightning produces a broad enhancement over the tropical Atlantic and Africa of 2-6 x 10(exp 14) molecules NO2/sq cm, 4 x 10(exp 17) molecules O3/sq cm (15 Dobson Units), and 125 pptv of upper tropospheric HNO3. The lightning background is 25-50% weaker over the tropical Pacific. A global source of 6+/-2 Tg N/yr from lightning in the model best represents the satellite observations of tropospheric NO2, O3, and HNO3.

Martin, Randall V.↗

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

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).

Martin, Randall V.↗

First Directly Retrieved Global Distribution of Tropospheric Column Ozone from GOME: Comparison with the GEOS-CHEM Model

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.

Liu, Xiong↗

Global Partitioning of NOx Sources Using Satellite Observations: Relative Roles of Fossil Fuel Combustion, Biomass Burning and Soil Emissions

This document contains the following abstract for the paper "Global partitioning of NOx sources using satellite observations: Relative roles of fossil fuel combustion, biomass burning and soil emissions." Satellite observations have been used to provide important new information about emissions of nitrogen oxides. Nitrogen oxides (NOx) are significant in atmospheric chemistry, having a role in ozone air pollution, acid deposition and climate change. We know that human activities have led to a three- to six-fold increase in NOx emissions since pre-industrial times, and that there are three main surface sources of NOx: fuel combustion, large-scale fires, and microbial soil processes. How each of these sources contributes to the total NOx emissions is subject to some doubt, however. The problem is that current NOx emission inventories rely on bottom-up approaches, compiling large quantities of statistical information from diverse sources such as fuel and land use, agricultural data, and estimates of burned areas. This results in inherently large uncertainties. To overcome this, Lyatt Jaegle and colleagues from the University of Washington, USA, used new satellite observations from the Global Ozone Monitoring Experiment (GOME) instrument. As the spatial and seasonal distribution of each of the sources of NOx can be clearly mapped from space, the team could provide independent topdown constraints on the individual strengths of NOx sources, and thus help resolve discrepancies in existing inventories. Jaegle's analysis of the satellite observations, presented at the recent Faraday Discussion on "Atmospheric Chemistry", shows that fuel combustion dominates emissions at northern mid-latitudes, while fires are a significant source in the Tropics. Additionally, she discovered a larger than expected role for soil emissions, especially over agricultural regions with heavy fertilizer use. Additional information is included in the original extended abstract.

Jaegle, Lyatt↗

Analysis of Satellite and Sub-Orbital Measurements

The objective of this project is to support the INTEX aircraft mission by developing experience in the integrated analysis of existing sub-orbital observations and satellite observations with numerical models. Specific tasks include providing guidance to INTEX by identifying discrepancies in satellite observations with (1) in situ measurements, (2) bottom-up emission inventories of nitrogen oxides and volatile organic compounds, and (3) model calculations of the export of pollution from North America to the global atmosphere. An important focus area is developing and improving bottom-up emission inventories by combining top-down and bottom-up information.

Gleason, James↗

Space-Based Diagnosis of Surface Ozone Sensitivity to Anthropogenic Emissions

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.

Martin, Randall V.↗

Air Mass Factor Formulation for Spectroscopic Measurements from Satellites: Application to Formaldehyde Retrievals from the Global Ozone Monitoring Experiment

We present a new formulation for the air mass factor (AMF) to convert slant column measurements of optically thin atmospheric species from space into total vertical columns. Because of atmospheric scattering, the AMF depends on the vertical distribution of the species. We formulate the AMF as the integral of the relative vertical distribution (shape factor) of the species over the depth of the atmosphere, weighted by altitude-dependent coefficients (scattering weights) computed independently from a radiative transfer model. The scattering weights are readily tabulated, and one can then obtain the AMF for any observation scene by using shape factors from a three dimensional (3-D) atmospheric chemistry model for the period of observation. This approach subsequently allows objective evaluation of the 3-D model with the observed vertical columns, since the shape factor and the vertical column in the model represent two independent pieces of information. We demonstrate the AMF method by using slant column measurements of formaldehyde at 346 nm from the Global Ozone Monitoring Experiment satellite instrument over North America during July 1996. Shape factors are cumputed with the Global Earth Observing System CHEMistry (GEOS-CHEM) global 3-D model and are checked for consistency with the few available aircraft measurements. Scattering weights increase by an order of magnitude from the surface to the upper troposphere. The AMFs are typically 20-40% less over continents than over the oceans and are approximately half the values calculated in the absence of scattering. Model-induced errors in the AMF are estimated to be approximately 10%. The GEOS-CHEM model captures 50% and 60% of the variances in the observed slant and vertical columns, respectively. Comparison of the simulated and observed vertical columns allows assessment of model bias.

Palmer, Paul I.↗

Mapping Isoprene Emissions over North America using Formaldehyde Column Observations from Space

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 %).

Palmer, Paul I.↗

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.↗

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.↗

Global and Regional Decreases in Tropospheric Oxidants from Photochemical Effects of Aerosols

We evaluate the sensitivity of tropospheric OH, O3, and O3 precursors to photochemical effects of aerosols not usually included in global models: (1) aerosol scattering and absorption of ultraviolet radiation and (2) reactive uptake of HO', NO2, and NO3. Our approach is to couple a global 3-D model of tropospheric chemistry (GEOS- CHEM) with aerosol fields from a global 3-D aerosol model (GOCART). Reactive uptake by aerosols is computed using reaction probabilities from a recent review (gamma(sub HO2) = 0.2, gamma(sub NO2) = 10(exp -4), gamma(sub NO3) = l0(exp -3). Aerosols decrease the O3 - O((sup 1)D) photolysis frequency by 5-20% at the surface throughout the Northern Hemisphere (largely due to mineral dust) and by a factor of 2 in biomass burning regions (largely due to black carbon). Aerosol uptake of HO2 accounts for 10-40% of total HOx radical ((triple bonds)OH + peroxy) loss in the boundary layer over polluted continental regions (largely due to sulfate and organic carbon) and for more than 70% over tropical biomass burning regions (largely due to organic carbon). Uptake of NO2 and NO3 accounts for 10-20% of total HNO3 production over biomass burning regions and less elsewhere. Annual mean OH concentrations decrease by 9% globally and by 5-35% in the boundary layer over the Northern Hemisphere. Simulated CO increases by 5- 15 ppbv in the remote Northern Hemisphere, improving agreement with observations. Simulated boundary layer O3 decreases by 15- 45 ppbv over India during the biomass burning season in March and by 5-9 ppbv over northern Europe in August, again improving comparison with observations. We find that particulate matter controls would increase surface O3 over Europe and other industrial regions.

Martin, Randall V.↗

An Improved Retrieval of Tropospheric Nitrogen Dioxide from GOME

We present a retrieval of tropospheric nitrogen dioxide (NO2) columns from the Global Ozone Monitoring Experiment (GOME) satellite instrument that improves in several ways over previous retrievals, especially in the accounting of Rayleigh and cloud scattering. Slant columns, which are directly fitted without low-pass filtering or spectral smoothing, are corrected for an artificial offset likely induced by spectral structure on the diffuser plate of the GOME instrument. The stratospheric column is determined from NO2 columns over the remote Pacific Ocean to minimize contamination from tropospheric NO2. The air mass factor (AMF) used to convert slant columns to vertical columns is calculated from the integral of the relative vertical NO2 distribution from a global 3-D model of tropospheric chemistry driven by assimilated meteorological data (Global Earth Observing System (GEOS)-CHEM), weighted by altitude dependent scattering weights computed with a radiative transfer model (Linearized Discrete Ordinate Radiative Transfer), using local surface albedos determined from GOME observations at NO2 wavelengths. The AMF calculation accounts for cloud scattering using cloud fraction, cloud top pressure, and cloud optical thickness from a cloud retrieval algorithm (GOME Cloud Retrieval Algorithm). Over continental regions with high surface emissions, clouds decrease the AMT by 20- 30% relative to clear sky. GOME is almost twice as sensitive to tropospheric NO2 columns over ocean than over land. Comparison of the retrieved tropospheric NO2 columns for July 1996 with GEOS-CHEM values tests both the retrieval and the nitrogen oxide radical (NOx) emissions inventories used in GEOS-CHEM. Retrieved tropospheric NO2 columns over the United States, where NOx emissions are particularly well known, are within 18% of GEOS-CHEM columns and are strongly spatially correlated (r = 0.78, n = 288, p less than 0.005). Retrieved columns show more NO2 than GEOS-CHEM columns over the Transvaal region of South Africa and industrial regions of the northeast United States and Europe. They are lower over Houston, India, eastern Asia, and the biomass burning region of central Africa, possibly because of biases from absorbing aerosols.

Martin, Randall V.↗

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↗