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Validation of stratospheric ozone observed by the Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment during 1992

Measurements of stratospheric ozone were made by the Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment from onboard the Space Shuttle during the period 8-16 April 1992. The precision and accuracy of the measurements are discussed in the context of establishing the accuracy and compatibility of the measurements relative to other space-based measurements of ozone. Coincident measurements were obtained from the Stratospheric Aerosol and Gas Experiment (SAGE) 2 instrument onboard the Earth Radiation Budget Satellite (ERBS) and three instruments, the Microwave Limb Sounder (MLS), the Cryogenic Limb Array Etalon Spectrometer (CLAES), the Halogen Occultation Experiment (HALOE) onboard the Upper Atmospheric Research Satellite (UARS). Three of the instruments, ATMOS, SAGE-2 and MLS are demonstrated to be consistent to within +10% over the altitude range between 100 hPa and 0.5 hPa (approximately 20 to 60 km), with ATMOS and MLS displaying a zero mean bias and a root mean square deviation (rms) of 3% and SAGE-2 displaying an essentially systematic bias of -5% over the majority of the altitude range, except for below 30 hPa where SAGE-2 displays a large positive systematic bias due to the effect of the aerosol attenuation resulting from the Mt. Pinatubo volcanic eruption in 1991. The comparison with HALOE indicates that ozone levels observed by ATMOS are systematically higher than HALOE by 5 to 25% with a clear gradient in the differences; in contrast the comparison with CLAES displays differences of as much as + 30% with no obvious systematic scaling possible. Comparisons are evaluated in two separate schemes, by geographical coincidence and through zonal averages which illustrate the limitations of both schemes. Latitudinal and longitudinal variation are used to assess the sensitivity of the ATMOS measurements and to confirm the precision and accuracy, which should be less than 4% and 10% respectively.

Abrams, M. C.↗

Assessment of the atmospheric impact of volcanic eruptions

The dominant global impact of volcanic activity is likely to be related to the effects of volcanic gases on the Earth's atmosphere. Volcanic gas emissions from individual volcanic arc eruptions are likely to cause increases in the stratospheric optical depth that result in surface landmass temperature decline of 2 to 3 K for less than a decade. Trachytic and intermediate magmas are much more effective in this regard than high-silica magmas, and may also lead to extensive ozone depletion due to effect of halogens and magmatic water. Given the assumed relationship between arc volcanism and subduction rate, and the relatively small variation in global spreading rates in the geologic record, it is unlikely that the rates of arc volcanism have varied greatly during the Cenozoic. Hotspot related basaltic fissure eruptions in the subaerial environment have a higher mass yield of sulfur, but lofting of the valcanic aerosol to levels above the tropopause is required for a climate impact. High-latitude events, such as the Laki 1783 eruption can easily penetrate the tropopause and enter the stratosphere, but formation of a stratospheric volcanic aerosol form low-latitude effusive basaltic eruptions is problematical, due to the elevated low-latitude tropopause. Due to the high sulfur content of hotspot-derived basaltic magmas, their very high mass eruption rates and the episodic behavior, hotspots must be regarded as potentially major modifiers of Earth's climate through the action of their volcanic volatiles on the chemistry and physics of the atmosphere.

Sigurdsson, H.↗

Active and Widespread Halogen Chemistry in the Tropical and Subtropical Free Troposphere

Halogens in the troposphere are increasingly recognized as playing an important role for atmospheric chemistry, and possibly climate. Bromine and iodine react catalytically to destroy ozone (O3), oxidize mercury, and modify oxidative capacity that is relevant for the lifetime of greenhouse gases. Most of the tropospheric O3 and methane (CH4) loss occurs at tropical latitudes. Here we report simultaneous measurements of vertical profiles of bromine oxide (BrO) and iodine oxide (IO) in the tropical and subtropical free troposphere (10degN to 40degS), and show that these halogens are responsible for 34% of the column-integrated loss of tropospheric O3. The observed BrO concentrations increase strongly with altitude (approx.3.4 pptv at 13.5 km), and are 2-4 times higher than predicted in the tropical free troposphere. BrO resembles model predictions more closely in stratospheric air. The largest model low bias is observed in the lower tropical transition layer (TTL) over the tropical eastern Pacific Ocean, and may reflect a missing inorganic bromine source supplying an additional 2.5-6.4 pptv total inorganic bromine (Bry), or model overestimated Bry wet scavenging. Our results highlight the importance of heterogeneous chemistry on ice clouds, and imply an additional Bry source from the debromination of sea salt residue in the lower TTL. The observed levels of bromine oxidize mercury up to 3.5 times faster than models predict, possibly increasing mercury deposition to the ocean. The halogen-catalyzed loss of tropospheric O3 needs to be considered when estimating past and future ozone radiative effects.

Wang, Siyuan↗

Decadal-Scale Responses in Middle and Upper Stratospheric Ozone From SAGE II Version 7 Data

Stratospheric Aerosol and Gas Experiment (SAGE II) version 7 (v7) ozone profiles are analyzed for their decadal-scale responses in the middle and upper stratosphere for 1991 and 1992-2005 and compared with those from its previous version 6.2 (v6.2). Multiple linear regression (MLR) analysis is applied to time series of its ozone number density vs. altitude data for a range of latitudes and altitudes. The MLR models that are fit to the time series data include a periodic 11 yr term, and it is in-phase with that of the 11 yr, solar UV (Ultraviolet)-flux throughout most of the latitude/ altitude domain of the middle and upper stratosphere. Several regions that have a response that is not quite in-phase are interpreted as being affected by decadal-scale, dynamical forcings. The maximum minus minimum, solar cycle (SClike) responses for the ozone at the low latitudes are similar from the two SAGE II data versions and vary from about 5 to 2.5% from 35 to 50 km, although they are resolved better with v7. SAGE II v7 ozone is also analyzed for 1984-1998, in order to mitigate effects of end-point anomalies that bias its ozone in 1991 and the analyzed results for 1991-2005 or following the Pinatubo eruption. Its SC-like ozone response in the upper stratosphere is of the order of 4%for 1984-1998 vs. 2.5 to 3%for 1991-2005. The SAGE II v7 results are also recompared with the responses in ozone from the Halogen Occultation Experiment (HALOE) that are in terms of mixing ratio vs. pressure for 1991-2005 and then for late 1992- 2005 to avoid any effects following Pinatubo. Shapes of their respective response profiles agree very well for 1992-2005. The associated linear trends of the ozone are not as negative in 1992-2005 as in 1984-1998, in accord with a leveling off of the effects of reactive chlorine on ozone. It is concluded that the SAGE II v7 ozone yields SC-like ozone responses and trends that are of better quality than those from v6.2.

Remsberg, E. E.↗

Volcanic Eruptions and Climate

Volcanic eruptions represent some of the most climatically important and societally disruptive short-term events in human history. Large eruptions inject ash, dust, sulfurous gases (e.g. SO2, H2S), halogens (e.g. Hcl and Hbr), and water vapor into the Earth's atmosphere. Sulfurous emissions principally interact with the climate by converting into sulfate aerosols that reduce incoming solar radiation, warming the stratosphere and altering ozone creation, reducing global mean surface temperature, and suppressing the hydrological cycle. In this issue, we focus on the history, processes, and consequences of these large eruptions that inject enough material into the stratosphere to significantly affect the climate system. In terms of the changes wrought on the energy balance of the Earth System, these transient events can temporarily have a radiative forcing magnitude larger than the range of solar, greenhouse gas, and land use variability over the last millennium. In simulations as well as modern and paleoclimate observations, volcanic eruptions cause large inter-annual to decadal-scale changes in climate. Active debates persist concerning their role in longer-term (multi-decadal to centennial) modification of the Earth System, however.

Volcanoes↗

The Upper Atmosphere Research Satellite: From Coffee Table Art to Quantitative Science

The Upper Atmosphere Research Satellite (UARS) has provided an unprecedented set of observations of constituents of the stratosphere. When used in combination with data from other sources and appropriate modeling tools, these observations are useful for quantitative evaluation of stratospheric photochemical processes. This is illustrated by comparing ozone observations from airborne Differential Absorption Lidar (DIAL), from the Polar Ozone and Aerosol Measurement (POAM), from the Microwave Limb Sounder (MLS), and from the Halogen occultation Experiment (HALOE) with ozone fields generated with a three dimensional model. For 1995-96, at polar latitudes, observations from DIAL flights on December 9 and January 30, and POAM and MLS between late December and late January are compared with ozone fields from the GSFC 3D chemistry and transport model. Data from the three platforms consistently show that the observed ozone has a negative trend relative to the modeled ozone, and that the trend is uniform in time between early and mid winter, with no obvious dependence on proximity to the vortex edge. The importance of chlorine catalyzed photochemistry to this ozone loss is explored by comparing observations from MLS and HALOE with simulations for other northern winters, particularly 1997-98.

Douglass, Anne R.↗

21st Century Trends in Antarctic Temperature and Polar Stratospheric Cloud (PSC) Area in the GEOS Chemistry-Climate Model

This study examines trends in Antarctic temperature and APSC, a temperature proxy for the area of polar stratospheric clouds, in an ensemble of Goddard Earth Observing System (GEOS) chemistry-climate model (CCM) simulations of the 21st century. A selection of greenhouse gas, ozone-depleting substance, and sea surface temperature scenarios is used to test the trend sensitivity to these parameters. One scenario is used to compare temperature trends in two versions of the GEOS CCM. An extended austral winter season is examined in detail. In May, June, and July, the expected future increase in CO2-related radiative cooling drives temperature trends in the Antarctic lower stratosphere. At 50 hPa, a 1.3 K cooling is expected between 2000 and 2100. Ozone levels increase, despite this robust cooling signal and the consequent increase in APSC, suggesting the enhancement of stratospheric transport in future. In the lower stratosphere, the choice of climate change scenarios does not affect the magnitude of the early winter cooling. Midwinter temperature trends are generally small. In October, APSC trends have the same sign as the prescribed halogen trends. That is, there are negative APSC trends in "grealistic future" simulations, where halogen loading decreases in accordance with the Montreal Protocol and CO2 continues to increase. In these simulations, the speed of ozone recovery is not influenced by either the choice of sea surface temperature and greenhouse gas scenarios or by the model version.

Hurwitz, M. M.↗

Stratospheric Assimilation of Chemical Tracer Observations Using a Kalman Filter: Chi-Square Validated Results and Analysis of Variance and Correlation Dynamics - Pt. 2

A Kalman filter system designed for the assimilation of limb-sounding observations of stratospheric chemical tracers, which has four tunable covariance parameters, was developed in Part I (Menard et al. 1998) The assimilation results of CH4 observations from the Cryogenic Limb Array Etalon Sounder instrument (CLAES) and the Halogen Observation Experiment instrument (HALOE) on board of the Upper Atmosphere Research Satellite are described in this paper. A robust (chi)(sup 2) criterion, which provides a statistical validation of the forecast and observational error covariances, was used to estimate the tunable variance parameters of the system. In particular, an estimate of the model error variance was obtained. The effect of model error on the forecast error variance became critical after only three days of assimilation of CLAES observations, although it took 14 days of forecast to double the initial error variance. We further found that the model error due to numerical discretization as arising in the standard Kalman filter algorithm, is comparable in size to the physical model error due to wind and transport modeling errors together. Separate assimilations of CLAES and HALOE observations were compared to validate the state estimate away from the observed locations. A wave-breaking event that took place several thousands of kilometers away from the HALOE observation locations was well captured by the Kalman filter due to highly anisotropic forecast error correlations. The forecast error correlation in the assimilation of the CLAES observations was found to have a structure similar to that in pure forecast mode except for smaller length scales. Finally, we have conducted an analysis of the variance and correlation dynamics to determine their relative importance in chemical tracer assimilation problems. Results show that the optimality of a tracer assimilation system depends, for the most part, on having flow-dependent error correlation rather than on evolving the error variance.

Menard, Richard↗

Multi-Decadal Records of Stratospheric Composition and Their Relationship to Stratospheric Circulation Change

Constituent evolution for 1990-2015 simulated using the Global Modeling Initiative chemistry and transport model driven by meteorological fields from the Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2) is compared with three sources of observations: ground-based column measurements of HNO3 and HCl from two stations in the Network for the Detection of Atmospheric Composition Change (NDACC, 1990- ongoing), profiles of CH4 from the Halogen Occultation Experiment (HALOE) on the Upper Atmosphere Research Satellite (UARS, 1992-2005), and profiles of N2O from the Microwave Limb Sounder on the Earth Observing System satellite Aura (2005- ongoing). The differences between observed and simulated values are shown to be time dependent, with better agreement after 2000 compared with the prior decade. Furthermore, the differences between observed and simulated HNO3 and HCl columns are shown to be correlated with each other, suggesting that issues with the simulated transport and mixing cause the differences during the 1990s and that these issues are less important during the later years. Because the simulated fields are related to mean age in the lower stratosphere, we use these comparisons to evaluate the time dependence of mean age. The ongoing NDACC column observations provide critical information necessary to substantiate trends in mean age obtained using fields from MERRA-2 or any other reanalysis products.

Profiles of N2O from the Microwave Limb Sounde↗

Tropospheric Ozone in the NASA GEOS Model: Effects of Satellite NO2 Data Assimilation and Improvements in Background NOx Chemistry

Tropospheric ozone is a major atmospheric oxidant, the primary source of the hydroxyl radical, and a greenhouse gas. In the troposphere, it is produced from the oxidation of carbon monoxide and volatile organic compounds in the presence of nitrogen oxides (NOx=NO+NO2) or has its origins in the stratosphere. The tropospheric ozone burdens in global atmospheric chemistry models disagree by a factor of 1.5, indicating an incomplete understanding of ozone sources and sinks. Here we examine the tropospheric ozone simulation in NASA Global Modeling and Assimilation Office’s (GMAO’s) GEOS model with the GEOS-Chem chemistry mechanism (version 14.2), using observations from satellites, aircraft, ozonesondes, and surface sites. This modeling framework is used to produce GMAO’s GEOS Composition Forecasts (GEOS-CF), and it has been updated extensively with new emission inventories, improved model physics, satellite data assimilation capability, and an up-to-date chemical mechanism that includes tropospheric halogen chemistry and NOx recycling from particulate nitrate. Earlier versions of the model using GEOS-Chem version 12.0 showed an underestimate in tropospheric ozone in the northern hemisphere. We evaluate the ozone simulation in the updated model, focusing on the effects of assimilating satellite NO2 data from the Ozone Monitoring Instrument (OMI), constraining stratospheric ozone to satellite data, and updates to the NOx chemistry. We will examine changes in the vertical profiles of tropospheric ozone over the US in support of the Tropospheric Emissions: Monitoring of Pollution (TEMPO), and discuss implications for the tropospheric ozone budget.

V. Shah↗

An Investigation of Aerosol Measurements from the Halogen Occultation Experiment: Validation, Size Distributions, Composition, and Relation to Other Chemical Species

The efforts envisioned within the original proposal (accepted February 1994) and the extension of this proposal (accepted February 1997) included measurement validations, the retrieval of aerosol size distributions and distribution moments, aerosol correction studies, and investigations of polar stratospheric clouds. A majority of the results from this grant have been published. The principal results from this grant are discussed.

Deshler, Terry↗

The Impact of Geoengineering Aerosols on Stratospheric Temperature and Ozone

Anthropogenic greenhouse gas emissions are warming the global climate at an unprecedented rate. Significant emission reductions will be required soon to avoid a rapid temperature rise. As a potential interim measure to avoid extreme temperature increase, it has been suggested that Earth's albedo be increased by artificially enhancing stratospheric sulfate aerosols. We use a 3D chemistry climate model, fed by aerosol size distributions from a zonal mean aerosol model, to simulate continuous injection of 1-10 Mt/a into the lower tropical stratosphere. In contrast to the case for all previous work, the particles are predicted to grow to larger sizes than are observed after volcanic eruptions. The reason is the continuous supply of sulfuric acid and hence freshly formed small aerosol particles, which enhance the formation of large aerosol particles by coagulation and, to a lesser extent, by condensation. Owing to their large size, these particles have a reduced albedo. Furthermore, their sedimentation results in a non-linear relationship between stratospheric aerosol burden and annual injection, leading to a reduction of the targeted cooling. More importantly, the sedimenting particles heat the tropical cold point tropopause and, hence, the stratospheric entry mixing ratio of H2O increases. Therefore, geoengineering by means of sulfate aerosols is predicted to accelerate the hydroxyl catalyzed ozone destruction cycles and cause a significant depletion of the ozone layer even though future halogen concentrations will be significantly reduced.

Heckendorn, P.↗

The Impact of Geoengineering Aerosols on Stratospheric Temperature and Ozone

Anthropogenic greenhouse gas emissions are warming the global climate at an unprecedented rate. Significant emission reductions will be required soon to avoid a rapid temperature rise. As a potential interim measure to avoid extreme temperature increase, it has been suggested that Earth's albedo be increased by artificially enhancing stratospheric sulfate aerosols. We use a 3D chemistry climate model, fed by aerosol size distributions from a zonal mean aerosol model. to simulate continuous injection of 1-10 Mt/a into the lower tropical stratosphere. In contrast to the case for all previous work, the particles are predicted to grow to larger sizes than are observed after volcanic eruptions. The reason is the continuous supply of sulfuric acid and hence freshly formed small aerosol particles, which enhance the formation of large aerosol particles by coagulation and, to a lesser extent, by condensation. Owing to their large size, these particles have a reduced albedo. Furthermore, their sedimentation results in a non-linear relationship between stratospheric aerosol burden and annual injection, leading to a reduction of the targeted cooling. More importantly, the sedimenting particles heat the tropical cold point tropopause and, hence, the stratospheric entry mixing ratio of H2O increases. Therefore, geoengineering by means of sulfate aerosols is predicted to accelerate the hydroxyl catalyzed ozone destruction cycles and cause a significant depletion of the ozone layer even though future halogen concentrations will he significantly reduced.

Heckendorn, P.↗

Tropospheric Ozone in the NASA GEOS Model: Effects of Satellite Data Assimilation and Improvements in Background NO x Chemistry

Tropospheric ozone is a major atmospheric oxidant, the primary source of the hydroxyl radical, and a greenhouse gas. In the troposphere, it is produced from the oxidation of carbon monoxide and volatile organic compounds in the presence of nitrogen oxides (NO x =NO+NO 2 ) or has its origins in the stratosphere. The tropospheric ozone burdens in global atmospheric chemistry models disagree by a factor of 1.5, indicating an incomplete understanding of ozone sources and sinks. Here we examine the tropospheric ozone simulation in NASA Global Modeling and Assimilation Office’s (GMAO’s) GEOS model with the GEOS-Chem chemistry mechanism (version 14.2), using observations from satellites, aircraft, ozonesondes, and surface sites. This modeling framework is used to produce GMAO’s GEOS Composition Forecasts (GEOS-CF), and it has been updated extensively with new emission inventories, improved model physics, satellite data assimilation capability, and an up-to-date chemical mechanism that includes tropospheric halogen chemistry and NOx recycling from particulate nitrate. Earlier versions of the model using GEOS-Chem version 12.0 showed an underestimate in tropospheric ozone in the northern hemisphere. We evaluate the ozone simulation in the updated model, focusing on the effects of assimilating satellite NO 2 data from the Ozone Monitoring Instrument (OMI), constraining stratospheric ozone to satellite data, and updates to the NOx chemistry. We will examine changes in the vertical profiles of tropospheric ozone over the US in support of the Tropospheric Emissions: Monitoring of Pollution (TEMPO), and discuss implications for the tropospheric ozone budget.

Viral Shah↗

Future Changes in Major Stratospheric Warmings in CCMI Models

Major stratospheric warmings (MSWs) are one of the most important phenomena of wintertime Arctic stratospheric variability. They consist of a warming of the Arctic stratosphere and a deceleration of the polar night jet, triggered by an anomalously high injection of tropospheric wave activity into the stratosphere. Due to the relevance and the impact of MSWs on the tropospheric circulation, several model studies have investigated their potential responses to climate change. However, a wide range of results has been obtained, extending from a future increase in the frequency of MSWs to a decrease. These discrepancies might be explained by different factors such as a competition of radiative and dynamical contributors with opposite effects on the Arctic polar vortex, biases of models to reproduce the related processes, or the metric chosen for the identification of MSWs. In this study, future changes in wintertime Arctic stratospheric variability are examined in order to obtaina more precise picture of future changes in the occurrence of MSWs. In particular, transient REFC2 simulations of different CCMs involved in the Chemistry Climate Model Initiative (CCMI) are used. These simulations extend from 1960 to 2100 and include forcings by halogens and greenhouse gases following the specifications of the CCMI-REF-C2 scenario. Sea surface temperatures (SSTs) and sea-ice distributions are either prescribed from coupled climate model integrations or calculated internally in the case of fully coupled atmosphere-ocean CCMs. Potential changes in the frequency and main characteristics of MSWs in the future are investigated with special focus on the dependence of the results on the criterion for the identification of MSWs and the tropospheric forcing of these phenomena.

Chemistry-Climate Modeling↗

Role of Atmospheric Chemistry in the Climate Impacts of Stratospheric Volcanic Injections

The climate impact of a volcanic eruption is known to be dependent on the size, location and timing of the eruption. However, the chemistry and composition of the volcanic plume also control its impact on climate. It is not just sulfur dioxide gas, but also the coincident emissions of water, halogens and ash that influence the radiative and climate forcing of an eruption. Improvements in the capability of models to capture aerosol microphysics, and the inclusion of chemistry and aerosol microphysics modules in Earth system models, allow us to evaluate the interaction of composition and chemistry within volcanic plumes in a new way. These modeling efforts also illustrate the role of water vapor in controlling the chemical evolution, and hence climate impacts, of the plume. A growing realization of the importance of the chemical composition of volcanic plumes is leading to a more sophisticated and realistic representation of volcanic forcing in climate simulations, which in turn aids in reconciling simulations and proxy reconstructions of the climate impacts of past volcanic eruptions. More sophisticated simulations are expected to help, eventually, with predictions of the impact on the Earth system of any future large volcanic eruptions.

Disrupting↗

Evaluating stratospheric ozone and water vapour changes in CMIP6 models from 1850 to 2100

Abstract. Stratospheric ozone and water vapour are key components of the Earth system, and past and future changes to both have important impacts on global and regional climate. Here, we evaluate long-term changes in these species from the pre-industrial period (1850) to the end of the 21st century in Coupled Model Intercomparison Project phase 6 (CMIP6) models under a range of future emissions scenarios. There is good agreement between the CMIP multi-model mean and observations for total column ozone (TCO), although there is substantial variation between the individual CMIP6 models. For the CMIP6 multi-model mean, global mean TCO has increased from ∼ 300 DU in 1850 to ∼ 305 DU in 1960, before rapidly declining in the 1970s and 1980s following the use and emission of halogenated ozone-depleting substances (ODSs). TCO is projected to return to 1960s values by the middle of the 21st century under the SSP2-4.5, SSP3-7.0, SSP4-3.4, SSP4-6.0, and SSP5-8.5 scenarios, and under the SSP3-7.0 and SSP5-8.5 scenarios TCO values are projected to be ∼ 10 DU higher than the 1960s values by 2100. However, under the SSP1-1.9 and SSP1-1.6 scenarios, TCO is not projected to return to the 1960s values despite reductions in halogenated ODSs due to decreases in tropospheric ozone mixing ratios. This global pattern is similar to regional patterns, except in the tropics where TCO under most scenarios is not projected to return to 1960s values, either through reductions in tropospheric ozone under SSP1-1.9 and SSP1-2.6, or through reductions in lower stratospheric ozone resulting from an acceleration of the Brewer–Dobson circulation under other Shared Socioeconomic Pathways (SSPs). In contrast to TCO, there is poorer agreement between the CMIP6 multi-model mean and observed lower stratospheric water vapour mixing ratios, with the CMIP6 multi-model mean underestimating observed water vapour mixing ratios by ∼ 0.5 ppmv at 70 hPa. CMIP6 multi-model mean stratospheric water vapour mixing ratios in the tropical lower stratosphere have increased by ∼ 0.5 ppmv from the pre-industrial to the present-day period and are projected to increase further by the end of the 21st century. The largest increases (∼ 2 ppmv) are simulated under the future scenarios with the highest assumed forcing pathway (e.g. SSP5-8.5). Tropical lower stratospheric water vapour, and to a lesser extent TCO, shows large variations following explosive volcanic eruptions.

54 ENVIRONMENTAL SCIENCES↗

Validation of Aura Microwave Limb Sounder HCl Measurements

The Earth Observing System (EOS) Microwave Limb Sounder (MLS) aboard the Aura satellite has provided daily global HCl profiles since August 2004. We provide a characterization of the resolution, random and systematic uncertainties, and known issues for the version 2.2 MLS HCl data. The MLS sampling allows for comparisons with many (~1500 to more than 3000) closely matched profiles from the Halogen Occultation Experiment (HALOE) and Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). These data sets provide HCl latitudinal distributions that are, overall, very similar to those from (coincident) MLS profiles, although there are some discrepancies in the upper stratosphere between the MLS and HALOE gradients. As found in previous work, MLS and ACE HCl profiles agree very well (within approximately 5%, on average), but the MLS HCl abundances are generally larger (by 10-20%) than HALOE HCl. The bias versus HALOE is unlikely to arise mostly from MLS, as a similar systematic bias (of order 15%) is not observed between average MLS and balloon-borne measurements of HCl, obtained over Fort Sumner, New Mexico, in 2004 and 2005. At the largest pressure (147 hPa) for MLS HCl, a high bias (approximately 0.2 ppbv) is apparent in analyses of low to midlatitude data versus in situ aircraft chemical ionization mass spectrometry (CIMS) HCl measurements from the Aura Validation Experiment (AVE) campaigns in 2004, 2005, and 2006; this bias is also observed in comparisons of MLS and aircraftHCl/O3 correlations. Good agreement between MLS and CIMS HCl is obtained at 100 to 68 hPa. The recommended pressure range for MLS HCl is from 100 to 0.15 hPa.

Earth Observing System (EOS)↗