Engineering topics

Crawford, James H.

Publications and source records attributed to Crawford, James H..

At least 19 records

DOE OSTI2020

Understanding and improving model representation of aerosol optical properties for a Chinese haze event measured during KORUS-AQ

KORUS-AQ was an international cooperative air quality field study in South Korea that measured local and remote sources of air pollution affecting the Korean Peninsula during May–June 2016. Some of the largest aerosol mass concentrations were measured during a Chinese haze transport event (24 May). Air quality forecasts using the WRF-Chem model with aerosol optical depth (AOD) data assimilation captured AOD during this pollution episode but overpredicted surface particulate matter concentrations in South Korea, especially PM 2.5 , often by a factor of 2 or larger. Analysis revealed multiple sources of model deficiency related to the calculation of optical properties from aerosol mass that explain these discrepancies. Using in situ observations of aerosol size and composition as inputs to the optical properties calculations showed that using a low-resolution size bin representation (four bins) underestimates the efficiency with which aerosols scatter and absorb light (mass extinction efficiency). Besides using finer-resolution size bins (8–16 bins), it was also necessary to increase the refractive indices and hygroscopicity of select aerosol species within the range of values reported in the literature to achieve better consistency with measured values of the mass extinction efficiency (6.7 m 2 g –1 observed average) and light-scattering enhancement factor (ƒ(RH)) due to aerosol hygroscopic growth (2.2 observed average). Furthermore, an evaluation of the optical properties obtained using modeled aerosol properties revealed the inability of sectional and modal aerosol representations in WRF-Chem to properly reproduce the observed size distribution, with the models displaying a much wider accumulation mode. Other model deficiencies included an underestimate of organic aerosol density (1.0 g cm –3 in the model vs. observed average of 1.5 g cm –3 ) and an overprediction of the fractional contribution of submicron inorganic aerosols other than sulfate, ammonium, nitrate, chloride, and sodium corresponding to mostly dust (17 %–28 % modeled vs. 12 % estimated from observations). These results illustrate the complexity of achieving an accurate model representation of optical properties and provide potential solutions that are relevant to multiple disciplines and applications such as air quality forecasts, health impact assessments, climate projections, solar power forecasts, and aerosol data assimilation.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2018

An Overview of Mesoscale Aerosol Processes, Comparisons, and Validation Studies from DRAGON Networks

Over the past 24 years, the AErosol RObotic NETwork (AERONET) program has provided highly accurate remote-sensing characterization of aerosol optical and physical properties for an increasingly extensive geographic distribution including all continents and many oceanic island and coastal sites. The measurements and retrievals from the AERONET global network have addressed satellite and model validation needs very well, but there have been challenges in making comparisons to similar parameters from in situ surface and airborne measurements. Additionally, with improved spatial and temporal satellite remote sensing of aerosols, there is a need for higher spatial-resolution ground-based remote-sensing networks. An effort to address these needs resulted in a number of field campaign networks called Distributed Regional Aerosol Gridded Observation Networks (DRAGONs) that were designed to provide a database for in situ and remote-sensing comparison and analysis of local to mesoscale variability in aerosol properties. This paper describes the DRAGON deployments that will continue to contribute to the growing body of research related to meso- and microscale aerosol features and processes. The research presented in this special issue illustrates the diversity of topics that has resulted from the application of data from these networks.

Holben, Brent N.↗

NASA NTRS2016

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

To determine the role of clouds in driving inter-annual and inter-seasonal variability of trace gases in the troposphere and lower stratosphere with a particular focus on the importance of cloud modification of photolysis. To evaluate the cloud fields and their vertical distribution in the HadGEM3 model utilizing 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.

Varma, Sunil↗

NASA NTRS2016

Constraints from Airborne (210)Pb Observations on Aerosol Scavenging and Lifetime in a Global Chemical Transport Model

Lead-210 distribution and lifetime in the atmosphere are not sensitive to ice in-cloud scavenging in convective updraft. Ice in-cloud scavenging in stratiform clouds reduce tropospheric (210)Pb lifetime by approximately 1 day and results in better agreements with observed surface observations and aircraft measured profiles. However, the process results in significant underestimate of (210)Pb in UT/LS.

Zhang, Bo↗

NASA NTRS2014

Impact of Bay-Breeze Circulations on Surface Air Quality and Boundary Layer Export

Meteorological and air-quality model simulations are analyzed alongside observations to investigate the role of the Chesapeake Bay breeze on surface air quality, pollutant transport, and boundary layer venting. A case study was conducted to understand why a particular day was the only one during an 11-day ship-based field campaign on which surface ozone was not elevated in concentration over the Chesapeake Bay relative to the closest upwind site and why high ozone concentrations were observed aloft by in situ aircraft observations. Results show that southerly winds during the overnight and early-morning hours prevented the advection of air pollutants from the Washington, D.C., and Baltimore, Maryland, metropolitan areas over the surface waters of the bay. A strong and prolonged bay breeze developed during the late morning and early afternoon along the western coastline of the bay. The strength and duration of the bay breeze allowed pollutants to converge, resulting in high concentrations locally near the bay-breeze front within the Baltimore metropolitan area, where they were then lofted to the top of the planetary boundary layer (PBL). Near the top of the PBL, these pollutants were horizontally advected to a region with lower PBL heights, resulting in pollution transport out of the boundary layer and into the free troposphere. This elevated layer of air pollution aloft was transported downwind into New England by early the following morning where it likely mixed down to the surface, affecting air quality as the boundary layer grew.

bay breeze↗

NASA NTRS2014

Relationship Between Column-Density and Surface Mixing Ratio: Statistical Analysis of O3 and NO2 Data from the July 2011 Maryland DISCOVER-AQ Mission

To investigate the ability of column (or partial column) information to represent surface air quality, results of linear regression analyses between surface mixing ratio data and column abundances for O3 and NO2 are presented for the July 2011 Maryland deployment of the DISCOVER-AQ mission. Data collected by the P-3B aircraft, ground-based Pandora spectrometers, Aura/OMI satellite instrument, and simulations for July 2011 from the CMAQ air quality model during this deployment provide a large and varied data set, allowing this problem to be approached from multiple perspectives. O3 columns typically exhibited a statistically significant and high degree of correlation with surface data (R(sup 2) > 0.64) in the P- 3B data set, a moderate degree of correlation (0.16 < R(sup 2) < 0.64) in the CMAQ data set, and a low degree of correlation (R(sup 2) < 0.16) in the Pandora and OMI data sets. NO2 columns typically exhibited a low to moderate degree of correlation with surface data in each data set. The results of linear regression analyses for O3 exhibited smaller errors relative to the observations than NO2 regressions. These results suggest that O3 partial column observations from future satellite instruments with sufficient sensitivity to the lower troposphere can be meaningful for surface air quality analysis.

nitrogen dioxide↗

NASA NTRS2013

An Elevated Reservoir of Air Pollutants over the Mid-Atlantic States During the 2011 DISCOVER-AQ Campaign: Airborne Measurements and Numerical Simulations

During a classic heat wave with record high temperatures and poor air quality from July 18 to 23, 2011, an elevated reservoir of air pollutants was observed over and downwind of Baltimore, MD, with relatively clean conditions near the surface. Aircraft and ozonesonde measurements detected approximately 120 parts per billion by volume ozone at 800 meters altitude, but approximately 80 parts per billion by volume ozone near the surface. High concentrations of other pollutants were also observed around the ozone peak: approximately 300 parts per billion by volume CO at 1200 meters, approximately 2 parts per billion by volume NO2 at 800 meters, approximately 5 parts per billion by volume SO2 at 600 meters, and strong aerosol optical scattering (2 x 10 (sup 4) per meter) at 600 meters. These results suggest that the elevated reservoir is a mixture of automobile exhaust (high concentrations of O3, CO, and NO2) and power plant emissions (high SO2 and aerosols). Back trajectory calculations show a local stagnation event before the formation of this elevated reservoir. Forward trajectories suggest an influence on downwind air quality, supported by surface ozone observations on the next day over the downwind PA, NJ and NY area. Meteorological observations from aircraft and ozonesondes show a dramatic veering of wind direction from south to north within the lowest 5000 meters, implying that the development of the elevated reservoir was caused in part by the Chesapeake Bay breeze. Based on in situ observations, Community Air Quality Multi-scale Model (CMAQ) forecast simulations with 12 kilometers resolution overestimated surface ozone concentrations and failed to predict this elevated reservoir; however, CMAQ research simulations with 4 kilometers and 1.33 kilometers resolution more successfully reproduced this event. These results show that high resolution is essential for resolving coastal effects and predicting air quality for cities near major bodies of water such as Baltimore on the Chesapeake Bay and downwind areas in the Northeast.

ozone↗

NASA NTRS2011

NASA's Earth Venture-1 (EV-1) Airborne Science Investigations

In 2010, NASA announced the first Earth Venture (EV-1) selections in response to a recommendation made by the National Research Council for low-cost investigations fostering innovation in Earth science. The five EV-1 investigations span the Earth science focus areas of atmosphere, weather, climate, water and energy and, carbon and represent earth science researchers from NASA as well as other government agencies, academia and industry from around the world. The EV-1 missions are: 1) Airborne Microwave Observatory of Subcanopy and Subsurface (AirMOSS), 2) Airborne Tropical Tropopause Experiment (ATTREX), 3) Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE), 4) Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ), and 5) Hurricane And Severe Storm Sentinel (HS3). The Earth Venture missions are managed out of the Earth System Science Pathfinder (ESSP) Program Office (Allen, et. al. 2010b)

Guillory, A.↗

NASA NTRS2011

An Overview of Measurement Comparisons from the INTEX-B/MILAGRO Airborne Field Campaign

As part of the NASA's INTEX-B mission, the NASA DC-8 and NSF C-130 conducted three wing-tip to wing-tip comparison flights. The intercomparison flights sampled a variety of atmospheric conditions (polluted urban, non-polluted, marine boundary layer, clean and polluted free troposphere). These comparisons form a basis to establish data consistency, but also should also be viewed as a continuation of efforts aiming to better understand and reduce measurement differences as identified in earlier field intercomparison exercises. This paper provides a comprehensive overview of 140 intercomparisons of data collected as well as a record of the measurement consistency demonstrated during INTEX-B. It is the primary goal to provide necessary information for the future research to determine if the observations from different INTEX-B platforms/instrument are consistent within the PI reported uncertainties and used in integrated analysis. This paper may also contribute to the formulation strategy for future instrument developments. For interpretation and most effective use of these results, the reader is strongly urged to consult with the instrument principle investigator.

Kleb, Mary M.↗

NASA NTRS2010

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.↗

NASA NTRS2009

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↗

NASA NTRS2008

An Overview of the NASA Spring/Summer 2008 Arctic Campaign - ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites)

ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) is a major NASA led airborne field campaign being performed in the spring and summer of 2008 at high latitudes (http://cloud1.arc.nasa.gov/arctas/). ARCTAS is a part of the International Polar Year program and its activities are closely coordinated with multiple U. S. (NOAA, DOE), Canadian, and European partners. Observational data from an ensemble of aircraft, surface, and satellite sensors are closely integrated with models of atmospheric chemistry and transport in this experiment. Principal NASA airborne platforms include a DC-8 for detailed atmospheric composition studies, a P-3 that focuses on aerosols and radiation, and a B-200 that is dedicated to remote sensing of aerosols. Satellite validation is a central activity in all these platforms and is mainly focused on CALIPSO, Aura, and Aqua satellites. Major ARCTAS themes are: (1) Long-range transport of pollution to the Arctic including arctic haze, tropospheric ozone, and persistent pollutants such as mercury; (2) Boreal forest fires and their implications for atmospheric composition and climate; (3) Aerosol radiative forcing from arctic haze, boreal fires, surface-deposited black carbon, and other perturbations; and (4) Chemical processes with focus on ozone, aerosols, mercury, and halogens. The spring deployment (April) is presently underway and is targeting plumes of anthropogenic and biomass burning pollution and dust from Asia and North America, arctic haze, stratosphere-troposphere exchange, and ozone photochemistry involving HOx and halogen radicals. The summer deployment (July) will target boreal forest fires and summertime photochemistry. The ARCTAS mission is providing a critical link to enhance the value of NASA satellite observations for Earth science. In this talk we will discuss the implementation of this campaign and some preliminary results.

Jacob, Daniel J.↗

NASA NTRS2008

An Instrument to Enable Identification of Anthropogenic CO2 Emissions Using Concurrent CO Measurements

We have developed an instrument concept that will enable the measurement of CO from the top of the atmosphere to the Earth's surface with very high sensitivity and at the high spatial and temporal resolutions required by the NRC Decadal Survey mission Active Sensing of Carbon Dioxide (CO2) over Nights, Days and Seasons (ASCENDS). We are developing an innovative CO sensor that will enable the ASCENDS mission to differentiate between anthropogenic and natural sources and sinks of global carbon. The NRC Decadal Survey places particular emphasis on retrieving CO information for the planetary boundary layer. Measurement made using both the 2.3 micron and 4.7 micron channels are needed to achieve the sensitivity required in the lower atmosphere where the degree of CO - CO2 correlation is indicative of anthropogenic sources of CO2. Measurements made using only the 4.7 micron channel cannot provide sufficient sensitivity to CO in the very lowest layers of the atmosphere. The fundamental method we use is Gas Filter Correlation Radiometry (GFCR), a highly successful technique used in other airborne and space-based missions for detecting trace species in the Earth's atmosphere. Our version of GFCR overcomes many of the limitations encountered by prior and existing instruments, allowing us to measure weak signals from small targets very quickly and with extremely high specificity by employing a new dual beam radiometer concept using a focal plane array. Our design will provide a means to make the desired CO measurements for the ASCENDS mission. A simple change in gas filter cell contents would allow the same hardware to measure CH4 with high precision under the nominal ASCENDS mission spatial and temporal constraints. All critical components in the sensor design are mature, many subsystems tested, and the system has been extensively modeled, bringing it to a present Technology Readiness Level (TRL) of 3 (though some individual components are at TRLs 6-9). We are presently developing critical components for the new spectrometer and advancing our understanding of the measurement requirements for both CO and CH4. This new GFCR technique/sensor will enable measurements of trace gases with high sensitivity while maintaining the inherent robustness and simplicity of the more traditional radiometer hardware. Initial estimates of cost/risk of a spacebased 2-channel GFCR indicate that our design is extremely cost effective and will fit within existing ASCENDS mission budget constraints as determined by the NRC Decadal Survey and a NASA-sponsored mission study.

Cook, William B.↗

NASA NTRS2008

HOx Observation and Model Comparison During INTEX-A 2004

OH and HO2 were measured with the Airborne Tropospheric Hydrogen Oxides Sensor (ATHOS) as part of a large measurement suite from the NASA DC-8 aircraft during the Intercontinental Chemical Transport Experiment - A (INTEX-A). This mission, which was conducted mainly over North America and the western Atlantic Ocean in summer 2004, was an excellent test of atmospheric oxidation chemistry. Throughout the troposphere, observed OH was generally 0.60 of the modeled OH; below 8 km, observed HO2 was generally 0.78 of modeled HO2. If the over-prediction of tropospheric OH is not due to an instrument calibration error, then it implied less global tropospheric oxidation capacity and longer lifetimes for gases like methane and methyl chloroform than currently thought. This discrepancy falls well outside uncertainties in both the OH measurement and rate coefficients for known reactions and points to a large unknown OH loss. If the modeled OH is forced to agree with observed values by introducing of an undefined OH loss that removed HOx (HOx=OH+HO2), the observed and modeled HO2 and HO2/OH ratios are largely reconciled within the measurement uncertainty. HO2 behavior above 8 km was markedly different. The observed-to-modeled ratio correlating with NO. The observed-to-modeled HO2 ratio increased from approximately 1 at 8 km to more than approximately 2.5 at 11 km with the observed-to-modeled ratio correlating with NO. The observed-to-modeled HO2 and NO were both considerably greater than observations from previous campaigns. In addition, the observed-to-modeled HO2/OH, which is sensitive to cycling reactions between OH and HO2, increased from approximately 1.2 at 8 km to almost 4 above 11 km. In contrast to the lower atmosphere, these discrepancies above 8 km suggest a large unknown HOx source and additional reactants that cycle HOx from OH to HO2. In the continental planetary boundary layer, the OH observed-to-modeled ratio increased from 0.6 when isoprene was less than 0.1 ppbv to over 3 when isoprene was greater than 2 ppbv, suggesting that forests throughout the United States are emitting unknown HOx sources. Progress in resolving these discrepancies requires further examinations of possible unknown OH sinks and HOx sources and a focused research activity devoted to ascertaining the accuracy of the OH and HO2 measurements.

Ren, Xinrong↗

NASA NTRS2008

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↗

NASA NTRS2007

Direct Measurements of the Convective Recycling of the Upper Troposphere

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

Bertram, Timothy H.↗

NASA NTRS2007

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

Global ozone analyses, based on assimilation of stratospheric profile and ozone column measurements, and NOy predictions from the Real-time Air Quality Modeling System (RAQMS) are used to estimate the ozone and NOy budget over the Continental US during the July-August 2004 Intercontinental Chemical Transport Experiment-North America (INTEX-A). Comparison with aircraft, satellite, surface, and ozonesonde measurements collected during the INTEX-A show that RAQMS captures the main features of the global and Continental US distribution of tropospheric ozone, carbon monoxide, and NOy with reasonable fidelity. Assimilation of stratospheric profile and column ozone measurements is shown to have a positive impact on the RAQMS upper tropospheric/lower stratosphere ozone analyses, particularly during the period when SAGE III limb scattering measurements were available. Eulerian ozone and NOy budgets during INTEX-A show that the majority of the Continental US export occurs in the upper troposphere/lower stratosphere poleward of the tropopause break, a consequence of convergence of tropospheric and stratospheric air in this region. Continental US photochemically produced ozone was found to be a minor component of the total ozone export, which was dominated by stratospheric ozone during INTEX-A. The unusually low photochemical ozone export is attributed to anomalously cold surface temperatures during the latter half of the INTEX-A mission, which resulted in net ozone loss during the first 2 weeks of August. Eulerian NOy budgets are shown to be very consistent with previously published estimates. The NOy export efficiency was estimated to be 24 percent, with NOx+PAN accounting for 54 percent of the total NOy export during INTEX-A.

Pierce, Robert B.↗

NASA NTRS2006

Radiative Effect of Clouds on Tropospheric Chemistry in a Global Three-Dimensional Chemical Transport Model

Clouds exert an important influence on tropospheric photochemistry through modification of solar radiation that determines photolysis frequencies (J-values). We assess the radiative effect of clouds on photolysis frequencies and key oxidants in the troposphere with a global three-dimensional (3-D) chemical transport model (GEOS-CHEM) driven by assimilated meteorological observations from the Goddard Earth Observing System data assimilation system (GEOS DAS) at the NASA Global Modeling and Assimilation Office (GMAO). We focus on the year of 2001 with the GEOS-3 meteorological observations. Photolysis frequencies are calculated using the Fast-J radiative transfer algorithm. The GEOS-3 global cloud optical depth and cloud fraction are evaluated and generally consistent with the satellite retrieval products from the Moderate Resolution Imaging Spectroradiometer (MODIS) and the International Satellite Cloud Climatology Project (ISCCP). Results using the linear assumption, which assumes linear scaling of cloud optical depth with cloud fraction in a grid box, show global mean OH concentrations generally increase by less than 6% because of the radiative effect of clouds. The OH distribution shows much larger changes (with maximum decrease of approx.20% near the surface), reflecting the opposite effects of enhanced (weakened) photochemistry above (below) clouds. The global mean photolysis frequencies for J[O1D] and J[NO2] in the troposphere change by less than 5% because of clouds; global mean O3 concentrations in the troposphere increase by less than 5%. This study shows tropical upper tropospheric O3 to be less sensitive to the radiative effect of clouds than previously reported (approx.5% versus approx.20-30%). These results emphasize that the dominant effect of clouds is to influence the vertical redistribution of the intensity of photochemical activity while global average effects remain modest, again contrasting with previous studies. Differing vertical distributions of clouds may explain part, but not the majority, of these discrepancies between models. Using an approximate random overlap or a maximum-random overlap scheme to take account of the effect of cloud overlap in the vertical reduces the impact of clouds on photochemistry but does not significantly change our results with respect to the modest global average effect.

Liu, Hongyu↗