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Statistical Analyses of Satellite Cloud Object Data from CERES: Comparison with Cloud-Resolving Model Simulations of Tropical Convective Clouds - Part III

The present study evaluates the ability of a cloud-resolving model (CRM) to simulate the physical properties of tropical deep convective cloud objects identified from a Clouds and the Earth s Radiant Energy System (CERES) data product. The emphasis of this study is the comparisons among the small-, medium- and large-size categories of cloud objects observed during March 1998 and between the large-size categories of cloud objects observed during March 1998 (strong El Ni o) and March 2000 (weak La Ni a). Results from the CRM simulations are analyzed in a way that is consistent with the CERES retrieval algorithm and they are averaged to match the scale of the CERES satellite footprints. Cloud physical properties are analyzed in terms of their summary histograms for each category. It is found that there is a general agreement in the overall shapes of all cloud physical properties between the simulated and observed distributions. Each cloud physical property produced by the CRM also exhibits different degrees of disagreement with observations over different ranges of the property. The simulated cloud tops are generally too high and cloud top temperatures are too low except for the large-size category of March 1998. The probability densities of the simulated top-of-the-atmosphere (TOA) albedos for all four categories are underestimated for high albedos, while those of cloud optical depth are overestimated at its lowest bin. These disagreements are mainly related to uncertainties in the cloud microphysics parameterization and inputs such as cloud ice effective size to the radiation calculation. Summary histograms of cloud optical depth and TOA albedo from the CRM simulations of the large-size category of cloud objects do not differ significantly between the March 1998 and 2000 periods, consistent with the CERES observations. However, the CRM is unable to reproduce the significant differences in the observed cloud top height while it overestimates the differences in the observed outgoing longwave radiation and cloud top temperature between the two periods. Comparisons between the CRM results and the observations for most parameters in March 1998 consistently show that both the simulations and observations have larger differences between the large- and small-size categories than between the large- and medium-size, or between the medium- and small-size categories. However, the simulated cloud properties do not change as much with size as observed. These disagreements are likely related to the spatial averaging of the forcing data and the mismatch in time and in space between the numerical weather prediction model from which the forcing data are produced and the CERES observed cloud systems.

Luo, Yali

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

Uncertainties in CERES Top-of-Atmosphere Fluxes Caused by Changes in Accompanying Imager

The Clouds and the Earth’s Radiant Energy System (CERES) project provides observations of Earth’s radiation budget using measurements from CERES instruments on board the Terra, Aqua, Suomi National Polar-orbiting Partnership (S-NPP), and NOAA-20 satellites. The CERES top-of-atmosphere (TOA) fluxes are produced by converting radiance measurements using empirical angular distribution models, which are functions of cloud properties that are retrieved from imagers flying with the CERES instruments. As the objective is to create a long-term climate data record, not only calibration consistency of the six CERES instruments needs to be maintained for the entire time period, it is also important to maintain the consistency of other input data sets used to produce this climate data record. In this paper, we address aspects that could potentially affect the CERES TOA flux data quality. Discontinuities in imager calibration can affect cloud retrieval which can lead to erroneous flux trends. When imposing an artificial 0.6 per decade decreasing trend to cloud optical depth, which is similar to the trend difference between CERES Edition 2 and Edition 4 cloud retrievals, the decadal SW flux trend changed from −0.3 5 ± 0.18 Wm −2 to 0.61 ± 0.18 Wm −2 . This indicates that a 13% change in cloud optical depth results in about 1% change in the SW flux. Furthermore, different CERES instruments provide valid fluxes at different viewing zenith angle ranges, and including fluxes derived at the most oblique angels unique to S-NPP (>66 ∘ ) can lead to differences of 0.8 Wm −2 and 0.3 Wm −2 in global monthly mean instantaneous SW flux and LW flux. To ensure continuity, the viewing zenith angle ranges common to all CERES instruments (<66 ∘ ) are used to produce the long-term Earth’s radiation budget climate data record. The consistency of cloud properties retrieved from different imagers also needs to be maintained to ensure the TOA flux consistency.

Wenying Su

Marine and continental stratocumulus cloud microphysical properties obtained from routine ARM Cimel sunphotometer observations

This study investigates marine and continental stratocumulus (Sc) cloud properties obtained from an automated implementation of a multispectral photometer retrieval. Photometer methods simultaneously retrieve cloud optical depth (τ) and cloud droplet effective radius (r e ), with estimates for liquid water path (LWP) calculated on the availability of those quantities. These applied methods evaluate retrieved cloud properties for Sc identified during a recent 6 year period over the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) program sites in Oklahoma, USA (SGP) and in the Azores, Portugal (ENA). Modest agreement in key quantity retrievals is found between the routine photometer products and multisensor collocated profiling references. Cumulative breakdowns contingent on cloud thickness indicate increases in all retrieved quantities in thicker clouds, with larger discrepancies in the relative performance between the retrievals collected in the presence of drizzle. Under continental cloud conditions, the clouds of a similar thickness and r e to those sampled under marine conditions report a factor of 1.5 larger τ and LWP. An r 2 ≅0.65 is found between photometer τ retrievals and shadowband radiometer measurements, with photometer retrievals reporting a high (relative) bias. The τ intercomparisons indicate that variability between retrievals is a factor of three larger than errors reported from individual retrieval input perturbation tests. Photometer r e retrievals suggest a low r 2 (< 0.1) having a standard deviation ≅ 3 µm when compared to ARM baseline multi-sensor radar/radiometer references (accounting for offsets in the cloud droplet number concentration assumptions of the latter). However, photometer LWP calculations remain relatively unbiased in non-drizzling conditions, with errors O (50 g m −2 ) and r 2 ≅0.5 to collocated radiometer and interferometer references. Additional sensitivity tests for island influences on marine Sc properties suggest that while island-influenced winds may promote larger cloud LWP or thickness, the influence could be within retrieval method uncertainty and/or collocated instrument variability.

54 ENVIRONMENTAL SCIENCES

Cloud-Vegetation Interaction: Use of Normalized Difference Cloud Index for Estimation of Cloud Optical Thickness

A new technique to retrieve cloud optical depth for broken clouds above green vegetation using ground-based zenith radiance measurements is developed. By analogy with the Normalized Difference Vegetation Index NDVI), the Normalized Difference Cloud Index (NDCI) is defined as a ratio between the difference and the sum of two zenith radiances measured for two narrow spectral bands in the visible and near-IR regions. The very different spectral behavior of cloud liquid water drops and green vegetation is the key physics behind the NDCI. It provides extra tools to remove the radiative effects of the 3D cloud structure. Numerical calculations based on fractal clouds and real measurements of NDCI and cloud liquid water path confirm the improvements.

Marshak, A.

Application of the CERES Flux-by-Cloud Type Simulator to GCM Output

The CERES Flux By CloudType data product produces CERES top-of-atmosphere (TOA) fluxes by region and cloud type. Here, the cloud types are defined by cloud optical depth (t) and cloud top pressure (pc), with bins similar to those used by ISCCP (International Satellite Cloud Climatology Project). This data product has the potential to be a powerful tool for the evaluation of the clouds produced by climate models by helping to identify which physical parameterizations have problems (e.g., boundary-layer parameterizations, convective clouds, processes that affect surface albedo). Also, when the flux-by-cloud type and frequency of cloud types are simultaneously used to evaluate a model, the results can determine whether an unrealistically large or small occurrence of a given cloud type has an important radiative impact for a given region. A simulator of the flux-by-cloud type product has been applied to three-hourly data from the year 2008 from the UK Met Office HadGEM2-A model using the Langley Fu-Lour radiative transfer model to obtain TOA SW and LW fluxes.

Eitzen, Zachary

Cloud-Vegetation Radiative Interaction: What Can We Learn from it about Cloud Optical Properties?

Because of their radiative interactions, the vegetation canopy and the atmosphere are coupled together; each serves as a boundary condition to the radative transfer equations in the adjacent medium. To better understand radiative processes in these media we need an accurate description of their interactions. This presentation outlines a technique needed to describe interactions between vegetation and clouds and exploits it to retrieve cloud optical depth from ground-based radiance measurements. measurements of zenith radiance in the RED and NIR spectral regions. In addition to an algebraic combinations of spectral radiances such as Normalized Difference Cloud Index (NDCI) that can result in poor retrievals due to its insensitivity to cloud fraction, both RED and NIR radiances as points on the "RED vs. NIR" plane are proposed to be used for retrieval. The proposed method is applied to a multi-channel sunphotometer (as a part of AERONET) measurements at the ARM site in Oklahoma. In addition to cloud optical depth, the new method also infers a "radiatively effective" cloud fraction.

Marshak, Alexander

Monte Carlo Bayesian Inference on a Statistical Model of Sub-gridcolumn Moisture Variability Using High-resolution Cloud Observations : Sensitivity Tests and Results - Part II

Part I presented a Monte Carlo Bayesian method for constraining a complex statistical model of GCM sub-gridcolumn moisture variability using high-resolution MODIS cloud data, thereby permitting large-scale model parameter estimation and cloud data assimilation. This part performs some basic testing of this new approach, verifying that it does indeed significantly reduce mean and standard deviation biases with respect to the assimilated MODIS cloud optical depth, brightness temperature and cloud top pressure, and that it also improves the simulated rotational-Ramman scattering cloud optical centroid pressure (OCP) against independent (non-assimilated) retrievals from the OMI instrument. Of particular interest, the Monte Carlo method does show skill in the especially difficult case where the background state is clear but cloudy observations exist. In traditional linearized data assimilation methods, a subsaturated background cannot produce clouds via any infinitesimal equilibrium perturbation, but the Monte Carlo approach allows finite jumps into regions of non-zero cloud probability. In the example provided, the method is able to restore marine stratocumulus near the Californian coast where the background state has a clear swath. This paper also examines a number of algorithmic and physical sensitivities of the new method and provides guidance for its cost-effective implementation. One obvious difficulty for the method, and other cloud data assimilation methods as well, is the lack of information content in the cloud observables on cloud vertical structure, beyond cloud top pressure and optical thickness, thus necessitating strong dependence on the background vertical moisture structure. It is found that a simple flow-dependent correlation modification due to Riishojgaard (1998) provides some help in this respect, by better honoring inversion structures in the background state.

Monte Carlo Bayesian inference

The Use of Vegetation For Estimating Broken-Cloud Optical Properties From Surface Measurements

It is known that because of complex three-dimensional (3D) radiative effects of broken clouds, the retrieval of cloud optical properties from upward measurements based on a one-dimensional (1D) inversion technique almost surely fails. To remove radiative effects of 3D cloud structure, we have developed a new technique that retrieves cloud optical thickness for broken clouds above green vegetation from simultaneous surface measurements in the VIS and Near Infrared (NIR) spectral regions. The theoretical basis of the method is the very different spectral behavior of cloud liquid water drops and green vegetation. For example, cloud optical properties, and hence cloud reflectivities, change little between 650 and 860 nm, while the vegetated surface albedo changes from 0.05 to 0.5 between the same two wavelengths. This spectral contrast in surface albedo suggests using ground measurements at both wavelengths not independently, but as an algebraic combination (a spectral index). For a spectral band in the NIR region, the green vegetation acts as a powerful reflector that "illuminates" horizontally inhomogeneous clouds from below. This provides the extra information needed to largely remove the 3D radiative effects, especially in the case of broken clouds; this in turn allows the retrieval of cloud optical depth using traditional 1D radiative transfer theory. This approach is similar to the so-called Green's function problem for radiative transfer where a laser beam illuminates clouds and the resulting "spot-size" of the reflected light around the beam characterizes cloud properties. We generalize Green's function theory to surf ace-cloud interaction and develop new spectral indices from which broken-cloud optical depth can be retrieved.

Marshak, A.

Cloud and aerosol optical depths

An airborne Sun photometer was used to measure optical depths in clear atmospheres between the appearances of broken stratus clouds, and the optical depths in the vicinity of smokes. Results show that (human) activities can alter the chemical and optical properties of background atmospheres to affect their spectral optical depths. Effects of water vapor adsorption on aerosol optical depths are apparent, based on data of the water vapor absorption band centered around 940 nm. Smoke optical depths show increases above the background atmosphere by up to two orders of magnitude. When the total optical depths measured through clouds were corrected for molecular scattering and gaseous absorption by subtracting the total optical depths measured through the background atmosphere, the resultant values are lower than those of the background aerosol at short wavelengths. The spectral dependence of these cloud optical depths is neutral, however, in contrast to that of the background aerosol or the molecular atmosphere.

Pueschel, R. F.

Improvements in CALIOP Smoke Optical Depth over Clouds

Smoke over marine stratocumulus is ubiquitous off the southwest coast of Africa during biomass burning season. Past studies have shown that CALIOP overestimates the base altitudes of strongly attenuating smoke layers. This is because CALIOP layer detection operates on the 532 nm attenuated backscatter signal. Smoke strongly attenuates light at this wavelength, so CALIOP feature detection at times assigns a base altitude that is higher than the true layer base for optically thick layers. In order to improve the AOD for smoke over clouds, a new algorithm has been implemented in for an upcoming CALIOP level 2 data release that will extend the base altitudes of smoke layers over clouds. This poster summarizes the new smoke base extension algorithm and its performance.

Jason L. Tackett

An Evaluation of the Liquid Cloud Droplet Effective Radius Derived from MODIS, Airborne Remote Sensing, and in Situ Measurements from CAMP2Ex

The cloud drop effective radius (Re) of the drop size distribution derived from passive satellite sensors is a key variable used in climate research. Validation of these satellite products has often taken place under stratiform cloud conditions that favor the assumption of cloud horizontal homogeneity used by the retrieval techniques. However, many studies have noted concerns with respect to significant biases in retrieved Re arising from cloud heterogeneity, for example, in cumulus cloud fields. Here, we examine data collected during the 2019 “Cloud, Aerosol and Monsoon Processes Philippines Experiment” (CAMP2Ex), which, in part, targeted the objective of providing the first detailed evaluation of Re retrieved across multiple platforms and techniques in a cumulus and congestus cloud region. Our evaluation consists of cross-comparisons of Re between the Moderate Resolution Imaging Spectroradiometer (MODIS) onboard the Terra satellite, the Research Scanning Polarimeter (RSP) onboard the NASA P-3 aircraft, and in situ measurements from both the NASA P-3 and Learjet aircraft that are all taken in close spatiotemporal proximity to the same cloud fields. A particular advantage of our approach lies in the capability of the RSP to retrieve Re using a bi-spectral MODIS approach and a polarimetric approach, which allows for the evaluation of bi-spectral and polarimetric Re retrievals from an airborne perspective using the same samples. Averaged over all P-3 flight segments examined here for warm clouds, the RSP polarimetric method, the in situ method, and the bias-adjusted MODIS method of Fu et al. (2019) show a comparable median (mean ± standard deviation) for the Re samples of 9.6 (10.2 ± 4.0) µm, 11.0 (13.6 ± 11.3) µm, and 10.4 (10.8 ± 3.8) µm, respectively. These values are far lower than the values of 15.1 (16.2 ± 5.5) µm and 17.2 (17.7 ± 5.7) µm from the bi-spectral retrievals of RSP and MODIS, respectively. Similar results are observed when Re is segregated by cloud-top height and in detailed case studies. The clouds sampled during CAMP2Ex consist of mostly small (mean transect length ∼ 1.4 km) and low clouds (mean cloud-top height ∼ 1 km), which had more numerous small clouds than the trade wind cumuli sampled in past field campaigns such as Rain in Shallow Cumulus over the Ocean (RICO) and the Indian Ocean Experiment (INDOEX). The overestimates of Re from the RSP bi-spectral technique compared with the polarimetric technique increased as cloud size and cloud optical depth decreased. Drizzle, cloud-top bumpiness, and solar zenith angle, however, are not closely correlated with the overestimate of bi-spectral Re. For shallow clouds that dominated the liquid cloud cover for the CAMP2Ex region and period, we show that 3-D radiative transfer and cloud heterogeneity, particularly for the optically thin and small clouds, appear to be the leading cause of the large positive biases in bi-spectral retrievals. Because this bias varies with the underlying structure of the cloud field, caution continues to be warranted in studies that use bi-spectral Re retrievals in cumulus cloud fields.

Cloud microphysics

Improvements in CALIOP Smoke Optical Depth over Clouds

Smoke over marine stratocumulus is ubiquitous off the south west coast of Africa during biomass burning season. The vertical profile measurements provided by the CALIOP lidar are successfully able to distinguish between smoke and underlying clouds. With over 14 years of observations, the CALIOP data set is a valuable asset for quantifying the radiative impact of smoke over clouds in this region. However past studies have shown that CALIOP overestimates the base altitudes of strongly attenuating smoke layers. This is because CALIOP layer detection operates on the 532 nm attenuated backscatter signal. Smoke strongly attenuates light at this wavelength, so CALIOP feature detection at times assigns a base altitude that is higher than the true layer base for optically thick layers. This can be confirmed by the 1064 nm attenuated backscatter signal, also measured by CALIOP. In order to improve the AOD for smoke over clouds, a new algorithm has been implemented in for an upcoming CALIOP level 2 data release that will extend the base altitudes of smoke layers over clouds. Tunable restrictions are put in place to ensure that smoke bases are only extended within a reasonable smoke-to-cloud gap distance and only when there is strong reason to believe that smoke exists within the gap. This presentation will summarize the new smoke base extension algorithm and summarize its performance. We will demonstrate that base extension is primarily invoked off the south west coast of Africa as expected. We will also quantify the increase in smoke AOD that will be reported in the upcoming level 2 data release.

Jason L Tackett

Detecting Thin Cirrus in Multiangle Imaging Spectroradiometer Aerosol Retrievals

Thin cirrus clouds (optical depth (OD) < 03) are often undetected by standard cloud masking in satellite aerosol retrieval algorithms. However, the Mu]tiangle Imaging Spectroradiometer (MISR) aerosol retrieval has the potential to discriminate between the scattering phase functions of cirrus and aerosols, thus separating these components. Theoretical tests show that MISR is sensitive to cirrus OD within Max{0.05 1 20%l, similar to MISR's sensitivity to aerosol OD, and MISR can distinguish between small and large crystals, even at low latitudes, where the range of scattering angles observed by MISR is smallest. Including just two cirrus components in the aerosol retrieval algorithm would capture typical MISR sensitivity to the natural range of cinus properties; in situations where cirrus is present but the retrieval comparison space lacks these components, the retrieval tends to underestimate OD. Generally, MISR can also distinguish between cirrus and common aerosol types when the proper cirrus and aerosol optical models are included in the retrieval comparison space and total column OD is >-0.2. However, in some cases, especially at low latitudes, cirrus can be mistaken for some combinations of dust and large nonabsorbing spherical aerosols, raising a caution about retrievals in dusty marine regions when cirrus is present. Comparisons of MISR with lidar and Aerosol Robotic Network show good agreement in a majority of the cases, but situations where cirrus clouds have optical depths >0.15 and are horizontally inhomogeneous on spatial scales shorter than 50 km pose difficulties for cirrus retrieval using the MISR standard aerosol algorithm..

Pierce, Jeffrey R.

Three-Channel Sunphotometer Cloud Mode Value-Added Product Report

A primary source of uncertainty in Earth system model (ESM) predictions is the representation of cloud processes and associated cloud feedback. Several fundamental cloud properties critical to the understanding of aerosol-cloud interactions are poorly constrained by observations, with key deficiencies in our observations of cloud and precipitation droplet sizes and cloud optical depth. Observations of these cloud properties are often challenging to estimate from remote-sensing platforms and costly to obtain from in situ aircraft. Nevertheless, observations of boundary-layer clouds, and improved knowledge of stratocumulus cloud (Sc) processes, are especially important to ESM advancement. This is because these clouds have extensive coverage and exert controls on boundary-layer dynamics and the global radiative energy balance.

54 ENVIRONMENTAL SCIENCES

The Experimental Cloud Lidar Pilot Study (ECLIPS) for cloud-radiation research

The Experimental Cloud Lidar Pilot Study (ECLIPS) was initiated to obtain statistics on cloud-base height, extinction, optical depth, cloud brokenness, and surface fluxes. Two observational phases have taken place, in October-December 1989 and April-July 1991, with intensive 30-day periods being selected within the two time intervals. Data are being archived at NASA Langley Research Center and, once there, are readily available to the international scientific community. This article describes the scale of the study in terms of its international involvement and in the range of data being recorded. Lidar observations of cloud height and backscatter coefficient have been taken from a number of ground-based stations spread around the globe. Solar shortwave and infrared longwave fluxes and infrared beam radiance have been measured at the surface wherever possible. The observations have been tailored to occur around the overpass times of the NOAA weather satellites. This article describes in some detail the various retrieval methods used to obtain results on cloud-base height, extinction coefficient, and infrared emittance, paying particular attention to the uncertainties involved.

Platt, C. M.

Comparison of Cloud Resolving Model Simulations to Remote Sensing Data

The purpose of this research was to evaluate the ability of a cloud-resolving model (CRM) to simulate the dynamical, radiative, and microphysical properties of deep convective cloud objects identified using CERES (Clouds and the Earth s Radiant Energy System) on board the Tropical Rainfall Measuring Mission (TRMM) satellite platform, for many cases. A deep convective cloud object is a contiguous region that is composed of satellite footprints that fulfill the following selection criteria: 100% cloud fraction, cloud optical depth > 10, and a cloud top height of at least 10 km. Selection criteria have also been formed for different types of boundary-layer clouds, as described in Xu et al. (2005). The purpose of the cloud object approach is to identify specific areas of where the cloud properties simulated by the CRM systematically differ from the observed cloud properties. Where these systematic differences exist, concrete steps can be made to improve the CRM s simulation of an entire class of clouds, rather than by tuning the model to correctly simulate a single case study, as is often done. Additional information regarding detailed approaches and findings are presented.

Randall, David A.

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