ALBERT

Description: We examine the tropical ozone mixing ratio perturbation fields generated from a monthly ozone climatology using 1998 to 2006 ozonesonde data from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network and the 13 year satellite record from 1993 to 2005 obtained from the Halogen Occultation Experiment (HALOE). The lengthy time series and high vertical resolution of the ozone and temperature profiles from the SHADOZ sondes coupled with good tropical coverage north and south of the equator gives a detailed picture of the ozone structure in the lowermost stratosphere down through the tropopause where the picture obtained from HALOE measurements is blurred by coarse vertical resolution. Ozone perturbations respond to annual variations in the Brewer-Dobson Circulation (BDC) in the region just above the cold-point tropopause to around 20 km. Strong annual signals of alternating positive and negative ozone anomalies are observed and correlate well with temperature anomalies. Above 20 km, ozone and temperature perturbations are dominated by the Quasi-biennial Oscillation (QBO). Both satellite and sonde records show good agreement between positive and negative ozone mixing ratio anomalies and alternating QBO easterly and westerly wind shears from the Singapore rawinsondes with a mean periodicity of 26 months for SHADOZ and 25 months for HALOE. There is a temporal offset of one to three months with the ozone QBO preceding the wind shear. Horizontal length scales for the annual cycle and the QBO, obtained using the temperature anomalies and wind shears in the thermal wind equation, compare well with theoretical calculations.

Description: Domain filling, forward trajectory calculations are used to examine the global dehydration processes that control stratospheric water vapor. As with most Lagrangian models of this type, water vapor is instantaneously removed from the parcel to keep the relative humidity (RH) with respect to ice from exceeding saturation or a specified super-saturation value. We also test a simple parameterization of stratospheric convective moistening through ice lofting and the effect of gravity waves as a mechanism that can augment dehydration. Comparing diabatic and kinematic trajectories driven by the MERRA reanalysis, we find that, unlike the results from Liu et al. (2010), the additional transport due to the vertical velocity "noise" in the kinematic calculation creates too dry a stratosphere and a too diffuse a water-vapor tape recorder signal compared observations. We also show that the kinematically driven parcels are more likely to encounter the coldest tropopause temperatures than the diabatic trajectories. The diabatic simulations produce stratospheric water vapor mixing ratios close to that observed by Aura's Microwave Limb Sounder and are consistent with the MERRA tropical tropopause temperature biases. Convective moistening, which will increase stratospheric HDO, also increases stratospheric water vapor while the addition of parameterized gravity waves does the opposite. We find that while the Tropical West Pacific is the dominant dehydration location, but dehydration over Tropical South America is also important. Antarctica makes a small contribution to the overall stratospheric water vapor budget as well by releasing very dry air into the Southern Hemisphere stratosphere following the break up of the winter vortex.

Description: Long lived halogen-containing compounds are important atmospheric constituents since they can act both as a source of chlorine radicals, which go on to catalyse ozone loss, and as powerful greenhouse gases. The long-term impact of these species on the ozone layer is dependent on their stratospheric lifetimes. Using observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) we present calculations of the stratospheric lifetimes of CFC-12, CCl4, CH4, CH3Cl and N2O. The lifetimes were calculated using the slope of the tracer–tracer correlation of these species with CFC-11 at the tropopause. The correlation slopes were corrected for the changing atmospheric concentrations of each species based on age of air and CFC-11 measurements from samples taken aboard the Geophysica aircraft – along with the effective linear trend of the volume mixing ratio (VMR) from tropical ground based AGAGE (Advanced Global Atmospheric Gases Experiment) sites. Stratospheric lifetimes were calculated using a CFC-11 lifetime of 45 yr. These calculations produced values of 113 + (−) 26 (18) yr (CFC-12), 35 + (−) 11 (7) yr (CCl4), 69 + (−) 65 (23) yr (CH3Cl), 123 + (−) 53 (28) yr (N2O) and 195 + (−) 75 (42) yr (CH4). The errors on these values are the weighted 1σ non-systematic errors. Systematic errors were estimated by recalculating lifetimes using VMRs which had been modified to reflect differences between ACE-FTS retrieved VMRs and those from other instruments. The results of these calculations, including systematic errors, were as follows: 113 + (−) 32 (20) for CFC-12, 123 + (−) 83 (35) for N2O, 195 + (−) 139 (57) for CH4, 35 + (−) 14 (8) for CCl4 and 69 + (−) 2119 (34) yr for CH3Cl. For CH3Cl & CH4 this represents the first calculation of the stratospheric lifetime using data from a space based instrument.

Description: Ozone measurements from ozonesondes, AROTAL, DIAL, and POAM III instruments during the SOLVE-2/VINTERSOL period are composited in a time-varying, flow-following quasi-conservative (PV-θ) coordinate space; the resulting composites from each instrument are mapped onto the other instruments' locations and times. The mapped data are then used to intercompare data from the different instruments. Overall, the four ozone data sets are found to be in good agreement. AROTAL shows somewhat lower values below 16 km, and DIAL has a positive bias at the upper limits of its altitude range. These intercomparisons are consistent with those obtained from more conventional near-coincident profiles, where available. Although the PV-θ mapping technique entails larger uncertainties of individual profile differences compared to direct near-coincident comparisons, the ability to include much larger numbers of comparisons can make this technique advantageous.

Description: Estimates of the radiative forcing due to anthropogenically-produced tropospheric O3 are derived primarily from models. Here, we use tropospheric ozone and cloud data from several instruments in the A-train constellation of satellites as well as information from the GEOS-5 Data Assimilation System to accurately estimate the radiative effect of tropospheric O3 for January and July 2005. Since we cannot distinguish between natural and anthropogenic sources with the satellite data, our derived radiative effect reflects the unadjusted (instantaneous) effect of the total tropospheric O3 rather than the anthropogenic component. We improve upon previous estimates of tropospheric ozone mixing ratios from a residual approach using the NASA Earth Observing System (EOS) Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) by incorporating cloud pressure information from OMI. We focus specifically on the magnitude and spatial structure of the cloud effect on both the short- and long-wave radiative budget. The estimates presented here can be used to evaluate the various aspects of model-generated radiative forcing. For example, our derived cloud impact is to reduce the radiative effect of tropospheric ozone by ~16%. This is centered within the published range of model-produced cloud effect on unadjusted ozone radiative forcing.

Description: The domain-filling, forward trajectory calculation model developed by Schoeberl and Dessler (2011) is used to further investigate processes that produce upper tropospheric and lower stratospheric water vapor anomalies. We examine the pathways parcels take from the base of the tropical tropopause layer (TTL) to the lower stratosphere. Most parcels found in the lower stratosphere arise from East Asia, the Tropical West Pacific (TWP) and Central/South America. The belt of TTL parcel origins is very wide compared to the final dehydration zones near the top of the TTL. This is due to the convergence of rising air due to the stronger diabatic heating near the tropopause relative to levels above and below. The observed water vapor anomalies – both wet and dry – correspond to regions where parcels have minimal displacement from their initialization. These minimum displacement regions include the winter TWP and the Asian and American monsoons. To better understand the stratospheric water vapor concentration we introduce the water vapor spectrum and investigate the source of the wettest and driest components of the spectrum. We find that the driest air parcels originate below the TWP, moving upward to dehydrate in the TWP cold upper troposphere. The wettest air parcels originate at the edges of the TWP as well as in the summer American and Asian monsoons. The wet air parcels are important since they skew the mean stratospheric water vapor distribution toward higher values. Both TWP cold temperatures that produce dry parcels as well as extra-TWP processes that control the wet parcels determine stratospheric water vapor.

Description: We apply the NASA Goddard Trajectory Model to data from a series of ozonesondes to derive ozone loss rates in the lower stratosphere for the AASE-2/EASOE mission (January-March 1992) and for the SOLVE/THESEO 2000 mission (January-March 2000) in an approach similar to Match. Ozone loss rates are computed by comparing the ozone concentrations provided by ozonesondes launched at the beginning and end of the trajectories connecting the launches. We investigate the sensitivity of the Match results to the various parameters used to reject potential matches in the original Match technique. While these filters effectively eliminate from consideration 80% of the matched sonde pairs and 〉99% of matched observations in our study, we conclude that only a filter based on potential vorticity changes along the calculated back trajectories seems warranted. Our study also demonstrates that the ozone loss rates estimated in Match can vary by up to a factor of two depending upon the precise trajectory paths calculated for each trajectory. As a result, the statistical uncertainties published with previous Match results might need to be augmented by an additional systematic error. The sensitivity to the trajectory path is particularly pronounced in the month of January, for which the largest ozone loss rate discrepancies between photochemical models and Match are found. For most of the two study periods, our ozone loss rates agree with those previously published. Notable exceptions are found for January 1992 at 475K and late February/early March 2000 at 450K, both periods during which we generally find smaller loss rates than the previous Match studies. Integrated ozone loss rates estimated by Match in both of those years compare well with those found in numerous other studies and in a potential vorticity/potential temperature approach shown previously and in this paper. Finally, we suggest an alternate approach to Match using trajectory mapping. This approach uses information from all matched observations without filtering and uses a two-parameter fit to the data to produce robust ozone loss rate estimates. As compared to loss rates from our version of Match, the trajectory mapping approach produces generally smaller loss rates, frequently not statistically significantly different from zero, calling into question the efficacy of the Match approach.

Description: We examine the tropical ozone mixing ratio perturbation fields generated from a monthly ozone climatology using 1998 to 2006 ozonesonde data from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network and the 13-year satellite record from 1993 to 2005 obtained from the Halogen Occultation Experiment (HALOE). The long time series and high vertical resolution of the ozone and temperature profiles from the SHADOZ sondes coupled with good tropical coverage north and south of the equator gives a detailed picture of the ozone structure in the lowermost stratosphere down through the tropopause where the picture obtained from HALOE measurements is blurred by coarse vertical resolution. Ozone perturbations respond to annual variations in the Brewer-Dobson Circulation (BDC) in the region just above the cold-point tropopause to around 20 km. Annual cycles in ozone and temperature are well correlated. Above 20 km, ozone and temperature perturbations are dominated by the Quasi-biennial Oscillation (QBO). Both satellite and sonde records show good agreement between positive and negative ozone mixing ratio anomalies and alternating QBO westerly and easterly wind shears from the Singapore rawinsondes with a mean periodicity of 26 months for SHADOZ and 25 months for HALOE. There is a temporal offset of one to three months with the QBO wind shear ahead of the ozone anomaly field. The meridional length scales for the annual cycle and the QBO, obtained using the temperature anomalies and wind shears in the thermal wind equation, compare well with theoretical calculations.

Description: We have developed a new technique for estimating ozone mixing ratio inside deep convective clouds. The technique uses the concept of an optical centroid cloud pressure that is indicative of the photon path inside clouds. Radiative transfer calculations based on realistic cloud vertical structure as provided by CloudSat radar data show that because deep convective clouds are optically thin near the top, photons can penetrate significantly inside the cloud. This photon penetration coupled with in-cloud scattering produces optical centroid pressures that are hundreds of hPa inside the cloud. We combine measured column ozone and the optical centroid cloud pressure derived using the effects of rotational-Raman scattering to estimate O3 mixing ratio in the upper regions of deep convective clouds. The data are obtained from the Ozone Monitoring Instrument (OMI) onboard NASA's Aura satellite. Our results show that low O3 concentrations in these clouds are a common occurrence throughout much of the tropical Pacific. Ozonesonde measurements in the tropics following convective activity also show very low concentrations of O3 in the upper troposphere. These low amounts are attributed to vertical injection of ozone poor oceanic boundary layer air during convection into the upper troposphere followed by convective outflow. Over South America and Africa, O3 mixing ratios inside deep convective clouds often exceed 50 ppbv which are comparable to mean background (cloud-free) amounts and are consistent with higher concentrations of injected boundary layer/lower tropospheric O3 relative to the remote Pacific. The Atlantic region in general also consists of higher amounts of O3 precursors due to both biomass burning and lightning. Assuming that O3 is well mixed (i.e., constant mixing ratio with height) up to the tropopause, we can estimate the stratospheric column O3 over clouds. Stratospheric column ozone derived in this manner agrees well with that retrieved independently with the Aura Microwave Limb Sounder (MLS) instrument and thus provides a consistency check of our method.

Description: Satellite observations show that ice cloud effective radius (re) increases with ice water content (IWC) but decreases with aerosol optical thickness (AOT). Using least-squares fitting to the observed data, we obtain an analytical formula to describe the variations of re with IWC and AOT for several regions with distinct characteristics of re-IWC-AOT relationships. As IWC directly relates to convective strength and AOT represents aerosol loading, our empirical formula provides a means to quantify the relative roles of dynamics and aerosols in controlling re in different geographical regions, and to establish a framework for parameterization of aerosol effects on re in climate models.