ALBERT

Description: This paper describes the retrievals algorithm used to determine temperature and height from radiance measurements by the Microwave Limb Sounder on EOS Aura. MLS is a "limbscanning" instrument, meaning that it views the atmosphere along paths that do not intersect the surface - it actually looks forwards from the Aura satellite. This means that the temperature retrievals are for a "profile" of the atmosphere somewhat ahead of the satellite. Because of the need to view a finite sample of the atmosphere, the sample spans a box about 1.5km deep and several tens of kilometers in width; the optical characteristics of the atmosphere mean that the sample is representative of a tube about 200-300km long in the direction of view. The retrievals use temperature analyses from NASA's Goddard Earth Observing System, Version 5 (GEOS-5) data assimilation system as a priori states. The temperature retrievals are somewhat deperrde~zt on these a priori states, especially in the lower stratosphere. An important part of the validation of any new dataset involves comparison with other, independent datasets. A large part of this study is concerned with such comparisons, using a number of independent space-based measurements obtained using different techniques, and with meteorological analyses. The MLS temperature data are shown to have biases that vary with height, but also depend on the validation dataset. MLS data are apparently biased slightly cold relative to correlative data in the upper troposphere and slightly warm in the middle stratosphere. A warm MLS bias in the upper stratosphere may be due to a cold bias in GEOS-5 temperatures.

Description: A comprehensive group of reactive nitrogen species (NO, NO2, HNO3, HO2NO2, PANs, alkyl nitrates, and aerosol-NO3) were measured in the troposphere and lowermost stratosphere over North America and the Atlantic during July/August 2004 (INTEX-A) from the NASA DC-8 platform (0.1-12 km). Less reactive nitrogen species (HCN and CH3CN), that are also unique tracers of biomass combustion, were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, and stratosphere was sampled both over continental U. S., Atlantic and Pacific. The North American upper troposphere was found to be greatly influenced by both lightning NO(x) and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO(x). Under polluted conditions PAN was a dominant carrier of reactive nitrogen in the upper troposphere while nitric acid dominated in the lower troposphere. Peroxynitric acid (HO2NO2) was present in sizable concentrations always peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the lower troposphere. Plumes from Alaskan fires contained large amounts of PAN and very little enhancement in ozone. Observational data suggest that lightning was a far greater contributor to NO(x) in the upper troposphere than previously believed. NO(x) and NO(y) reservoir appeared to be in steady state only in the middle troposphere where NO(x)/NO(y) was independent of air mass age. A first comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. These uncertainties likely propagate themselves in satellites derived NOx data. Observed data are interpreted to suggest that soil sinks of HCN/CH3CN are at best very small. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation.

Description: We present a global chemical data assimilation system using a global atmosphere model, the Community Atmosphere Model (CAM3) with simplified chemistry and the Data Assimilation Research Testbed (DART) assimilation package. DART is a community software facility for assimilation studies using the ensemble Kalman filter approach. Here, we apply the assimilation system to constrain global tropospheric carbon monoxide (CO) by assimilating meteorological observations of temperature and horizontal wind velocity and satellite CO retrievals from the Measurement of Pollution in the Troposphere (MOPITT) satellite instrument. We verify the system performance using independent CO observations taken on board the NSFINCAR C-130 and NASA DC-8 aircrafts during the April 2006 part of the Intercontinental Chemical Transport Experiment (INTEX-B). Our evaluations show that MOPITT data assimilation provides significant improvements in terms of capturing the observed CO variability relative to no MOPITT assimilation (i.e. the correlation improves from 0.62 to 0.71, significant at 99% confidence). The assimilation provides evidence of median CO loading of about 150 ppbv at 700 hPa over the NE Pacific during April 2006. This is marginally higher than the modeled CO with no MOPITT assimilation (-140 ppbv). Our ensemble-based estimates of model uncertainty also show model overprediction over the source region (i.e. China) and underprediction over the NE Pacific, suggesting model errors that cannot be readily explained by emissions alone. These results have important implications for improving regional chemical forecasts and for inverse modeling of CO sources and further demonstrate the utility of the assimilation system in comparing non-coincident measurements, e.g. comparing satellite retrievals of CO with in-situ aircraft measurements. The work described above also brought to light several short-comings of the data assimilation approach for CO profiles. Because of the limited vertical resolution of the measurement, the retrievals at different altitudes are correlated which can lead to problems with numerical error and overall efficiency. This has resulted in a manuscript that is about to be submitted to JGR:

Description: Vertical profiles of stratospheric HOCl calculated with a diurnal steady-state photochemical model that uses currently recommended reaction rates and photolysis cross sections underestimate observed profiles of HOCl obtained by two balloon-borne instruments, FIRS-2 (a far-infrared emission spectrometer) and MkIV (a mid-infrared, solar absorption spectrometer). Considerable uncertainty (a factor of two) persists in laboratory measurements of the rate constant (k(sub 1)) for the reaction ClO + HO2 yields HOCl + O2. Agreement between modeled and measured HOCl can be attained using a value of k(sub 1) from Stimpfle et al. (1979) that is about a factor-of-two faster than the currently recommended rate constant. Comparison of modeled and measured HOCl suggests that models using the currently recommended value for k(sub 1) may underestimate the role of the HOCl catalytic cycle for ozone depletion, important in the midlatitude lower stratosphere.

Description: Derived Meteorological Products (DMPs, including potential temperature (theta), potential vorticity, equivalent latitude (EqL), horizontal winds and tropopause locations) have been produced for the locations and times of measurements by several solar occultation (SO) instruments and the Aura Microwave Limb Sounder (MLS). DMPs are calculated from several meteorological analyses for the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer, Stratospheric Aerosol and Gas Experiment II and III, Halogen Occultation Experiment, and Polar Ozone and Aerosol Measurement II and III SO instruments and MLS. Time-series comparisons of MLS version 1.5 and SO data using DMPs show good qualitative agreement in time evolution of O3, N2O, H20, CO, HNO3, HCl and temperature; quantitative agreement is good in most cases. EqL-coordinate comparisons of MLS version 2.2 and SO data show good quantitative agreement throughout the stratosphere for most of these species, with significant biases for a few species in localized regions. Comparisons in EqL coordinates of MLS and SO data, and of SO data with geographically coincident MLS data provide insight into where and how sampling effects are important in interpretation of the sparse SO data, thus assisting in fully utilizing the SO data in scientific studies and comparisons with other sparse datasets. The DMPs are valuable for scientific studies and to facilitate validation of non-coincident measurements.

Description: In situ observations in a tropical subvisible cirrus cloud during the Costa Rica Aura Validation Experiment on 2 February 2006 show the presence of condensed-phase nitric acid. The cloud was observed near the tropopause at altitudes of 16.3-17.7 km in an extremely cold (183-191 K) and dry 5 ppm H2O) air mass. Relative humidities with respect to ice ranged from 150-250% throughout most of the cloud. Optical particle measurements indicate the presence of ice crystals as large as 90 microns in diameter. Condensed RN031H20 molar ratios observed in the cloud particles were 1-2 orders of magnitude greater than ratios observed previously in cirrus clouds at similar RN03 partial pressures. Nitric acid trihydrate saturation ratios were 10 or greater during much of the cloud encounter, indicating that RN03 may be present in the cloud particles as a stable condensate and not simply physically adsorbed on or trapped in the particles.

Description: The chemical composition of the lowermost stratosphere exhibits both spatial and temporal variability depending upon the relative strength of (1) isentropic transport from the tropical tropopause layer (TTL), (2) diabatic descent from the midlatitude and northern midlatitude stratosphere followed by equatorward isentropic transport, and (3) diabatic ascent from the troposphere through convection. In situ measurements made in the lowermost stratosphere over Florida illustrate the additional impact of equatorward flow around the monsoon anticyclone. This flow carries, along with older stratospheric air, the distinct signature of deep midlatitude convection. We use simultaneous in situ measurements of water vapor (H2O), ozone (O3), total odd nitrogen (NOy), carbon dioxide (CO2), and carbon monoxide (CO) in the framework of a simple box model to quantify the composition of the air sampled in the lowermost stratosphere during the mission on the basis of tracer mixing ratios ascribed to the source regions for these transport pathways. The results show that in the summer, convection has a significant impact on the composition of air in the lowermost stratosphere, being the dominant source of water vapor up to the 380 K isentrope. The implications of these results extend from the potential for heterogeneous ozone loss resulting from the increased frequency and lifetime of cirrus near the local tropopause, to air with increased water vapor that as part of the equatorward flow associated with the North American monsoon can become part of the general circulation.

Description: The Infrared Atmospheric Sounding Interferometer (IASI) on the MetOp satellite was launched on October 19, 2006. The Joint Airborne IASI Validation Experiment (JAIVEx) was conducted during April 2007 mainly for validation of the IASI on the MetOp satellite. IASI possesses an ultra-spectral resolution of 0.25/cm and a spectral coverage from 645 to 2760/cm. Ultraspectral resolution infrared spectral radiance obtained from near nadir observations provide atmospheric, surface, and cloud property information. An advanced retrieval algorithm with a fast radiative transfer model, including cloud effects, is used for atmospheric profile and cloud parameter retrieval. Preliminary retrievals of atmospheric soundings, surface properties, and cloud optical/microphysical properties with the IASI observations during the JAIVEx are obtained and presented. These retrievals are further inter-compared with those obtained from airborne FTS system, such as the NPOESS Airborne Sounder Testbed Interferometer (NAST-I), dedicated dropsondes, radiosondes, and ground based Raman Lidar. The capabilities of satellite ultra-spectral sounder such as the IASI are investigated.

Description: The climate change simulation community is moving toward use of global cloud resolving models (CRMs), however, current computational resources are not sufficient to run global CRMs over the hundreds of years necessary to produce climate change estimates. As an intermediate step between conventional general circulation models (GCMs) and global CRMs, many climate analysis centers are embedding a CRM in each grid cell of a conventional GCM. These Multiscale Modeling Frameworks (MMFs) represent a theoretical advance over the use of conventional GCM cloud and convection parameterizations, but have been shown to exhibit an overproduction of precipitation in the tropics during the northern hemisphere summer. In this study, simulations of clouds, precipitation, and radiation over the South China Sea using the CRM component of the NASA Goddard MMF are evaluated using retrievals derived from the instruments aboard the Tropical Rainfall Measuring Mission (TRMM) satellite platform for a 46-day time period that spans 5 May - 20 June 1998. The NASA Goddard Cumulus Ensemble (GCE) model is forced with observed largescale forcing derived from soundings taken during the intensive observing period of the South China Sea Monsoon Experiment. It is found that the GCE configuration used in the NASA Goddard MMF responds too vigorously to the imposed large-scale forcing, accumulating too much moisture and producing too much cloud cover during convective phases, and overdrying the atmosphere and suppressing clouds during monsoon break periods. Sensitivity experiments reveal that changes to ice cloud microphysical parameters have a relatively large effect on simulated clouds, precipitation, and radiation, while changes to grid spacing and domain length have little effect on simulation results. The results motivate a more detailed and quantitative exploration of the sources and magnitude of the uncertainty associated with specified cloud microphysical parameters in the CRM components of MMFs.

Description: We investigate the intraseasonal (30-90 day) variations in satellite-observed tropical total ozone (O3) and their connection to the Madden-Julian Oscillation (MJO). Tropical total O3 intraseasonal variations are large (approximately +/- 10 DU) and comparable to those in annual and interannual time scales. These O3 anomalies are mainly evident in the subtropics over the Pacific an eastern; hemisphere and propagate slowly eastward (approximately 5 m s-1). The subtropical negative (positive) O3 anomalies are typically collocated with the subtropical upper troposphere anticyclones (cyclones) generated by equatorial MJO convection and flank or lie to the west of the equatorial enhanced (suppressed) MJO convection. The subtropical O3 are anticorrelated with geopotential height anomalies near the tropopause and thus mainly associated with the O3 variability in the stratosphere rather the troposphere. Over the equatorial regions, total O3 anomalies are small.