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NASA NTRS2002

The Influence of Tropospheric Processes in Modeling the Middle Atmosphere with Gravity Waves

Our Numerical Spectral Model (NSM) extends from the ground up into the thermosphere and has a vertical grid point resolution of about 0.5 km to resolve the interactions of gravity waves (GWs) described with Hines' Doppler Spread Parameterization (DSP). This model produces in the stratosphere and mesosphere the major features of QBO, SAO, tides, and planetary waves. The purpose of this paper is to discuss results from an initial study with our 3D model that shows how certain tropospheric processes can affect the dynamics of the middle atmosphere. Under the influence of tropospheric heating, and augmented by GW interactions, two distinct but related processes can be identified. (1) A meridional circulation develops in the stratosphere, with rising motions at low latitudes that are in magnitude comparable to the downward propagation of the QBO. As Dunkerton pointed out, a larger GW source is then required to reproduce the observed QBO, which tends to move us closer to the values recommended for the DSP. This has significant consequences for our model results that describe the upper mesosphere, considering the general importance of GWs for this region and in influencing planetary waves (e.g., 2-day wave) and tides in particular. (2) Tropospheric heating produces zonal jets near the tropopause that are related to latitudinal variations in pressure and reversing temperature variations (resembling the dynamical conditions near the mesopause), which in turn is conducive to generate baroclinic instability. Modeling results show that our ability to generate the QBO critically depends on the magnitude of the temperature reversal that is a measure of this instability. Planetary waves are generated in this process, which can apparently interfere with or augment the GW interactions. As originally demonstrated by Lindzen and Holton, the eastward propagating Kelvin waves and westward propagating Rossby gravity waves (generated by tropospheric convection) can in principle provide the acceleration to influence the QBO, and we were able to confirm this with our 3D model.

Mayr, H. G.↗
NASA NTRS2002

Insights into Tropical Tropospheric Ozone from the SHADOZ Network

The first view of lower stratospheric and upper tropospheric structure from sondes is provided by a 3-year, 10-site record from the Southern Hemisphere ADditional OZonesondes (SHADOZ) network: http://code9 16.gsfc.nasa.gov/Data_services/shadoz. Observations covering 1998-2000 were made over Ascension Island; Nairobi, Kenya; Irene, South Africa; La Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil. Taking the UT/LS (upper troposphere-lower stratosphere) as the region between 12 and 17 km, we examine ozone variability in this region on a week-to- week and seasonal basis. The tropopause is lower in September-October-November than in March-April-May, when ozone is a minimum at most SHADOZ stations. A zonal wave-one pattern (referring to ozone mixing ratios greater over the Atlantic and adjacent continents than over the Pacific and eastern Indian Ocean), persists all year. The wave, predominantly in the troposphere and with variable magnitude, appears to be due to general circulation - with subsidence over the Atlantic and frequent deep convection over the Pacific and Indian Ocean. The variability of deep convection - most prominent at Java, Fiji, Samoa and Natal - is explored in time-vs-altitude ozone curtains. Stratospheric incursions into the troposphere are most prominent in soundings at Irene and Reunion Island.

Thompson, A. M.↗
NASA NTRS2004

Extratropical Stratosphere-Troposphere Mass Exchange

Understanding the exchange of gases between the stratosphere and the troposphere is important for determining how pollutants enter the stratosphere and how they leave. This study does a global analysis of that the exchange of mass between the stratosphere and the troposphere. While the exchange of mass is not the same as the exchange of constituents, you can t get the constituent exchange right if you have the mass exchange wrong. Thus this kind of calculation is an important test for models which also compute trace gas transport. In this study I computed the mass exchange for two assimilated data sets and a GCM. The models all agree that amount of mass descending from the stratosphere to the troposphere in the Northern Hemisphere extra tropics is approx. 10(exp 10) kg/s averaged over a year. The value for the Southern Hemisphere by about a factor of two. ( 10(exp 10) kg of air is the amount of air in 100 km x 100 km area with a depth of 100 m - roughly the size of the D.C. metro area to a depth of 300 feet.) Most people have the idea that most of the mass enters the stratosphere through the tropics. But this study shows that almost 5 times more mass enters the stratosphere through the extra-tropics. This mass, however, is quickly recycled out again. Thus the lower most stratosphere is a mixture of upper stratospheric air and tropospheric air. This is an important result for understanding the chemistry of the lower stratosphere.

Schoeberl, Mark R.↗
NASA NTRS2004

Tropical Tropospheric Ozone Climatology: Approaches Based on SHADOZ Observations

The SHADOZ (Southern Hemisphere Additional Ozonesondes) ozone sounding network was initiated in 1998 to improve the coverage of tropical in-situ ozone measurements for satellite validation, algorithm development and related process studies. Over 2000 soundings have been archived at the central website, , for 12 stations that span the entire equatorial zone [Thompson et al., JGR, 108,8238, 2003]. The most striking features of tropospheric ozone profiles in SHADOZ are: (1) persistent longitudinal variability in tropospheric ozone profiles, with a 10-15 DU column-integrated difference between Atlantic and Pacific sites; (2) intense short-term variability triggered by changing meteorological conditions and advection of pollution. The implications of these results for profile climatologies and trends are described along with several approaches to classifying ozone profiles: 1) Seasonal means during MAM (March-April-May) and SON (September-October-November); 2) Maxima and minima, identified through correlation of TOMS-derived TTO (tropical tropospheric ozone) column depth with the sonde integrated tropospheric ozone column; and 3) Meteorological regimes, a technique that is effective in the subtropics where tropical and mid-latitude conditions alternate.

Thompson, Anne M.↗
NASA NTRS2004

Discoveries about Tropospheric Ozone Pollution from Satellite and Soundings

We have been producing near-red time tropospheric ozone satellite maps from the TOMS (Total Ozone Mapping Spectrometer) sensor since 1997. Maps for 1996-2000 for the operational Earth-Probe instrument are at: . Pollution in the tropics is influenced by biomass burning and by transport patterns that favor recirculation and in other cases reflect climate variability like the El-Nino-Southern Oscillation [Thompson et al., 2001]. The satellite view of chemical-dynamical interactions in tropospheric ozone is not adequate to capture vertical gradients in pollution. Thus, in 1998, NASA's Goddard Space Flight Center and a team of international sponsors established the SHADOZ (Southern Hemisphere ADditional OZonesondes) project to address the gap in tropical ozone soundings. SHADOZ augments launches and provides a public archive of ozonesonde data from twelve tropical stations at http://croc.gsfc.nasa.gov/shadoz. Further insights into the role of chemical and dynamical influences have emerged from the first 4-5 years of SHADOZ data (more than 2000 ozone profiles). Highly variable tropospheric ozone and a zonal wave-one pattern in tropospheric ozone suggest that dynamics is as important as pollution in determining tropical ozone distributions.

Thompson, Anne M.↗
NASA NTRS2004

IVS Tropospheric Parameters: Comparison with DORIS and GPS for CONT02

In April 2002 the IVS (International VLBI Service for Geodesy and Astrometry) set up the Pilot Project - Tropospheric Parameters, and the Institute of Geodesy and Geophysics (IGG), Vienna, was put in charge of coordinating the project. Seven IVS Analysis Centers have joined the project and regularly submitted their estimates of tropospheric parameters (wet and total zenith delays, horizontal gradients) for all IVS-R1 mid IVS-R4 sessions since January 1st, 2002. The individual submissions are combined by a two-step procedure to obtain stable, robust and highly accurate tropospheric parameter time series with one hour resolution (internal accuracy: 2-4 ram). Starting with July 2003, the combined tropospheric estimates became operational IVS products. In the second half of October 2002 the VLBI campaign CONT02 was observed with 8 stations participating around the globe. At four of them (Gilmore Creek, U.S.A.; Hartebeesthoek, South Africa; Kokee Park, U.S.A.; Ny-Alesund, Norway) also total zenith delays from DORIS (Doppler Orbitography and Radiopositioning Integrated by Satellite) are available and these estimates are compared with those from the IGS (International GPS Service) and the IVS. The distance from the DORIS beacons to the co-located GPS and VLBI stations is around 2 km or less for the four sites mentioned above.

Schuh, Harald↗
NASA NTRS2003

Ozone Profiles and Tropospheric Ozone from Global Ozone Monitoring Experiment

Ozone profiles are derived from backscattered radiances in the ultraviolet spectra (290-340 nm) measured by the nadir-viewing Global Ozone Monitoring Experiment using optimal estimation. Tropospheric O3 is directly retrieved with the tropopause as one of the retrieval levels. To optimize the retrieval and improve the fitting precision needed for tropospheric O3, we perform extensive wavelength and radiometric calibrations and improve forward model inputs. Retrieved O3 profiles and tropospheric O3 agree well with coincident ozonesonde measurements, and the integrated total O3 agrees very well with Earth Probe TOMS and Dobson/Brewer total O3. The global distribution of tropospheric O3 clearly shows the influences of biomass burning, convection, and air pollution, and is generally consistent with our current understanding.

Liu, X.↗
NASA NTRS2005

Modeling of Isotope Fractionation in Stratospheric CO2, N2O, CH4, and O3: Investigations of Stratospheric Chemistry and Transport, Stratosphere-Troposphere Exchange, and Their Influence on Global Isotope Budgets

Until recently, the stable isotopic composition of chemically and datively important stratospheric species, such as ozone (O3), carbon dioxide (CO2), nitrous oxide (N2O), and methane (CH4), was largely unexplored, despite indications from the few measurements available and theoretical studies that global-scale isotopic variations will provide a unique tool for quantifying rates of global-scale mass transport into, within, and out of the stratosphere and for understanding the mechanisms of chemical reactions involved in ozone production. The number and geographical extent of observations are beginning to increase rapidly, however, as access to the stratosphere, both directly and by remote-sensing, has increased over the last 10 years and as new analytical techniques have been developed that make global-scale isotope measurements by whole-air sampling more feasible. The objective of this study, begun in April 1999, is to incorporate into the Livermore 2D model the likely photochemical fractionation processes that determine the isotopic compositions of stratospheric CO2, N2O, CH4, and O3, and to use the model results and new observations from NASA field campaigns in 1996 and 1997 to investigate stratospheric chemistry and mass transport. Additionally, since isotopic signatures from the stratosphere are transferred to the troposphere by downward transport at middle and high latitudes, the isotopic compositions may also serve as sensitive tracers of stratosphere-totroposphere transport. Comparisons of model results with stratospheric and upper tropospheric observations from these campaigns, as well as with ground-based observations from new NOAA and NSF-sponsored studies, will help determine whether the magnitudes of the stratospheric fractionation processes are large enough to use as global-scale tracers of transport into the troposphere and, if so, will be used to help constrain the degree of coupling between the troposphere and the stratosphere.

Boering, Kristie A.↗
NASA NTRS2003

Tropospheric Carbon Monoxide Measurements from the Scanning High-resolution Interferometer Sounder on 7 September 2000 in Southern Africa during SAFARI 2000

Retrieved tropospheric carbon monoxide (CO) column densities are presented for more than 9000 spectra obtained by the University of Wisconsin-Madison (UWis) Scanning High-Resolution Interferometer Sounder (SHIS) during a flight on the NASA ER-2 on 7 September 2000 as part of the Southern African Regional Science Initiative (SAFARI 2000) dry season field campaign. Enhancements in tropospheric column CO were detected in the vicinity of a controlled biomass burn in the Timbavati Game Reserve in northeastern South Africa and over the edge of the river of smoke in south central Mozambique. Relatively clean air was observed over the far southern coast of Mozambique. Quantitative comparisons are presented with in situ measurements from five different instruments flying on two other aircraft: the University of Washington Convair-580 (CV) and the South African Aerocommander JRB in the vicinity of the Timbavati fire. Measured tropospheric CO columns (extrapolated from 337 to 100 mb) of 2.1 x 10(exp 18) per square centimeter in background air and up to 1.5 x 10(exp 19) per square centimeter in the smoke plume agree well with SHIS retrieved tropospheric CO columns of (2.3 plus or minus 0.25) x 10(exp 18) per square centimeter over background air near the fire and (1.5 plus or minus 0.35) x 10(exp 19) per square centimeter over the smoke plume. Qualitative comparisons are presented with three other in situ CO profiles obtained by the South African JRA aircraft over Mozambique and northern South Africa showing the influence of the river of smoke.

McMillan, W. W.↗
NASA NTRS2006

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.↗
NASA NTRS2006

Investigations of Stratosphere-Troposphere Exchange of Ozone Derived From MLS Observations

Daily high-resolution maps of stratospheric ozone have been constructed using observations by MLS combined with trajectory information. These fields are used to determine the extratropical stratosphere-troposphere exchange (STE) of ozone for the year 2005 using two diagnostic methods. The resulting two annual estimates compare well with past model- and observational-based estimates. Initial analyses of the seasonal characteristics indicate that significant STE of ozone in the polar regions occurs only during spring and early summer. We also examine evidence that the Antarctic ozone hole is responsible for a rapid decrease in the rate of ozone STE during the SH spring. Subtracting the high-resolution stratospheric ozone fiom OMI total column measurements creates a high-resolution tropospheric ozone residual (HTOR) product. The HTOR fields are compared to the spatial distribution of the ozone STE. We show that the mean tropospheric ozone maxima tend to occur near locations of significant ozone STE. This suggests that STE may be responsible for a significant fraction of many mean tropospheric ozone anomalies.

Olsen, Mark A.↗
NASA NTRS2006

The Tropospheric Wind Lidar Technology Experiment (TWiLiTE): An Airborne Direct Detection Doppler Lidar Instrument Development Program

Global measurement of tropospheric winds is a key measurement for understanding atmospheric dynamics and improving numerical weather prediction. Global wind profiles remain a high priority for the operational weather community and also for a variety of research applications including studies of the global hydrologic cycle and transport studies of aerosols and trace species. In addition to space based winds, a high altitude airborne system flown on UAV or other advanced platforms would be of great interest for studying mesoscale dynamics and hurricanes. The Tropospheric Wind Lidar Technology Experiment (TWiLiTE) project was selected in 2005 by the NASA Earth Sun Technology Office as part of the Instrument Incubator Program. TWiLiTE will leverage significant research and development investments in key technologies made in the past several years. The primary focus will be on integrating these sub-systems into a complete molecular direct detection Doppler wind lidar system designed for autonomous operation on a high altitude aircraft, such as the NASA WB57, so that the nadir viewing lidar will be able to profile winds through the full troposphere. TWiLiTE is a collaboration involving scientists and technologists from NASA Goddard, NOAA ESRL, Utah State University Space Dynamics Lab and industry partners Michigan Aerospace Corporation and Sigma Space Corporation. NASA Goddard and it's partners have been at the forefront in the development of key lidar technologies (lasers, telescopes, scanning systems, detectors and receivers) required to enable spaceborne global wind lidar measurement. The TWiLiTE integrated airborne Doppler lidar instrument will be the first demonstration of a airborne scanning direct detection Doppler lidar and will serve as a critical milestone on the path to a fixture spaceborne tropospheric wind system. The completed system will have the capability to profile winds in clear air from the aircraft altitude of 18 h to the surface with 250 m vertical resolution and less than 2 meters per second velocity accuracy. The instrument design, technologies and predicted performance will be presented.

Gentry, Bruce↗
NASA NTRS2006

The High Resolution Tropospheric Ozone Residual

The co-flight of the MLS stratospheric limb sounder and the Ozone Monitoring Instrument (OMI) provides the capability of computing the Tropospheric Ozone Residual (TOR) in much greater detail [Ziemke et al., 2006]. Using forward trajectory calculations of MLS ozone measurements combined with OMI column ozone we have developed a high horizontal resolution tropospheric ozone residual (HTOR) which can provide even more detail than the standard TOR product. HTOR is especially useful for extra-tropical studies of tropospheric ozone transport. We find that both the Pacific pollution corridor (East Asia to Alaska) and the Atlantic pollution corridor (North America east coast to Europe) are also preferred locations for strat-trop folds leading to systematic overestimates of pollution amounts. In fact, fold events appear to dominate extra-tropical Northern Hemisphere day-to-day maps of HTOR. Model estimates of the tropospheric column are in reasonable agreement with the HTOR amounts when offsets due to different tropopause height calculations are taken into consideration.

Schoeberl, Mark R.↗
NASA NTRS2007

DIAL Measurements of Free-Tropospheric Ozone Profiles in Huntsville, AL

A tropospheric ozone Differential Absorption Lidar (DIAL) system, developed jointly by NASA and the University of Alabama at Huntsville (UAH), measures free-tropospheric ozone profiles between 4-10 km. Located at 192 meters altitude in the Regional Atmospheric Profiling Laboratory for Discovery (RAPCD) on the UAH campus in Huntsville, AL, USA, this tropospheric ozone lidar operates under both daytime and nighttime conditions. Frequent coincident ozonesonde flights and theoretical calculations provide evidence to indicate the retrieval accuracy ranges from better than 8% at 4km to 40%-60% at 10 kin with 750-m vertical resolution and 30-minute integration. With anticipated improvements to allow retrievals at both higher and lower altitudes, this ozone lidar, along with co-located aerosol and Doppler Wind Lidars, will provide a unique 18 dataset for investigations of PBL and free-tropospheric chemical and dynamic processes.

Kuang, Shi↗
NASA NTRS2008

Global Radiative Forcing of Coupled Tropospheric Ozone and Aerosols in a Unified General Circulation Model

Global simulations of sea salt and mineral dust aerosols are integrated into a previously developed unified general circulation model (GCM), the Goddard Institute for Space Studies (GISS) GCM II', that simulates coupled tropospheric ozone-NOx-hydrocarbon chemistry and sulfate, nitrate, ammonium, black carbon, primary organic carbon, and secondary organic carbon aerosols. The fully coupled gas-aerosol unified GCM allows one to evaluate the extent to which global burdens, radiative forcing, and eventually climate feedbacks of ozone and aerosols are influenced by gas-aerosol chemical interactions. Estimated present-day global burdens of sea salt and mineral dust are 6.93 and 18.1 Tg with lifetimes of 0.4 and 3.9 days, respectively. The GCM is applied to estimate current top of atmosphere (TOA) and surface radiative forcing by tropospheric ozone and all natural and anthropogenic aerosol components. The global annual mean value of the radiative forcing by tropospheric ozone is estimated to be +0.53 W m(sup -2) at TOA and +0.07 W m(sup -2) at the Earth's surface. Global, annual average TOA and surface radiative forcing by all aerosols are estimated as -0.72 and -4.04 W m(sup -2), respectively. While the predicted highest aerosol cooling and heating at TOA are -10 and +12 W m(sup -2) respectively, surface forcing can reach values as high as -30 W m(sup -2), mainly caused by the absorption by black carbon, mineral dust, and OC. We also estimate the effects of chemistry-aerosol coupling on forcing estimates based on currently available understanding of heterogeneous reactions on aerosols. Through altering the burdens of sulfate, nitrate, and ozone, heterogeneous reactions are predicted to change the global mean TOA forcing of aerosols by 17% and influence global mean TOA forcing of tropospheric ozone by 15%.

Liao, Hong↗
NASA NTRS2007

Simulations of Tropospheric NO2 by the Global Modeling Initiative (GMI) Model Utilizing Assimilated and Forecast Meteorological Fields: Comparison to Ozone Monitoring Instrument (OMI) Measurements

We present simulations of the tropospheric composition for the years 2004 and 2005, carried out by the GMI Combined Stratosphere-Troposphere (Combo) model, at a resolution of 2degx2.5deg. The model includes a new parameterization of lightning sources of NO(x) which is coupled to the cloud mass fluxes in the adopted meteorological fields. These simulations use two different sets of input meteorological fields: a)late-look assimilated fields from the Global Modeling and Assimilation Office (GMAO), GEOS-4 system and b) 12-hour forecast fields initialized with the assimilated data. Comparison of the forecast to the assimilated fields indicates that the forecast fields exhibit less vigorous convection, and yield tropical precipitation fields in better agreement with observations. Since these simulations include a complete representation of the stratosphere, they provide realistic stratosphere-tropospheric fluxes of O3 and NO(y). Furthermore, the stratospheric contribution to total columns of different troposheric species can be subtracted in a consistent fashion, and the lightning production of NO(y) will depend on the adopted meteorological field. We concentrate here on the simulated tropospheric columns of NO2, and compare them to observations by the OM1 instrument for the years 2004 and 2005. The comparison is used to address these questions: a) is there a significant difference in the agreement/disagreement between simulations for these two different meteorological fields, and if so, what causes these differences?; b) how do the simulations compare to OMI observations, and does this comparison indicate an improvement in simulations with the forecast fields? c) what are the implications of these simulations for our understanding of the NO2 emissions over continental polluted regions?

Rodriquez, J. M.↗
NASA NTRS2007

Tropospheric Vertical Distribution of Tropical Atlantic Ozone Observed by TES during the Northern African Biomass Burning Season

We present vertical distributions of ozone from the Tropospheric Emission Spectrometer (TES) over the tropical Atlantic Ocean during January 2005. Between 10N and 20S, TES ozone retrievals have Degrees of Freedom for signal (DOF) around 0.7 - 0.8 each for tropospheric altitudes above and below 500 hPa. As a result, TES is able to capture for the first time from space a distribution characterized by two maxima: one in the lower troposphere north of the ITCZ and one in the middle and upper troposphere south of the ITCZ. We focus our analysis on the north tropical Atlantic Ocean, where most of previous satellite observations showed discrepancies with in-situ ozone observations and models. Trajectory analyses and a sensitivity study using the GEOS-Chem model confirm the influence of northern Africa biomass burning on the elevated ozone mixing ratios observed by TES over this region.

satellite observations↗
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↗