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At least 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
NASA NTRS1994

Coherent variations of monthly mean total ozone and lower stratospheric temperature

Space-time patterns of correlation between total ozone and lower stratospheric temperature are documented, based on 14 years (1979-1992) of global monthly mean observations. Data are obtained from the total ozone mapping spectrometer (TOMS) and microwave sounding unit (MSU) channel 4, the latter being a weighted mean temperature of the 150- to 50-mbar layer. These data are analyzed (separately) for linear trend, solar cycle, quasi-biennial oscillation (QBO), and El Nino-Southern Oscillation (ENSO) variations via linear regression: significant signals are identified for each term, and the corresponding structures in ozone and temperature are found to be highly coherent. The temperature trends derived here show significant cooling of the lower stratosphere over Northern Hemisphere (NH) midlatitudes in winter-spring and over Antarctica in Southern Hemisphere (SH) spring; the overall space-time patterns are similar to those determined for ozone trends. Interestingly, temperatures do not decrease over SH midlatitudes during midwinter, in spite of large ozone losses. These data furthermore show globally coherent ozone and temperature perturbations associated with both QBO and ENSO variations; a new result here show large total ozone anomalies in middle-to-high latitudes of both hemispheres associated with ENSO events. Residuals from the ozone and temperature time series (defined as the deseasonalized total minus the regression fits) show strong positive correlation in middle-to-high latitudes but weak correlations in the trop ics. Time periods following the volcanic eruptions of El Chichon and Pinatubo are clearly identified from the coupled signatures of decreased ozone and increased temperature, opposite to the positive ozone-temperature correlations observed at other times. The ratios of ozone to temperature anomalies derived here show quantitative signatures indicating that either radiative (trend, solar, and QBO) or dynamical (ENSO and residuals) processes are responsible for the strong ozone-temperature correlations.

Randel, William J.↗
NASA NTRS1998

Analysis of record-breaking low ozone values during the 1997 winter over NDSC Station Lauder, New Zealand

During early August 1997, the ozone column density measured over Lauder was unusually low, with a minimum value of 222 Dobson Units (DU) at August 10. These observations are striking since in August, during the Austral winter, the ozone column density should be heading towards its yearly maximum; The August mean ozone column density measured over Lauder between 1987 and 1996 was 348(+/-28) DU, the lowest monthly average in these ten years was 255 DU. Regular altitude profile measurements of ozone, performed at Network for the Detection of Stratospheric Change (NDSC) station Lauder, make it possible to do a detailed, altitude-resolved, study of the low ozone observations. The measurements show ozone poor air in two altitude regions of the stratosphere: A 'high region', extending from the 600 K to the 1050 K isentrope (25 to 34 km), and a 'low region', below about 550 K (22 km). High resolution reverse trajectory maps of potential vorticity (PV) and ozone mixing ratio, based on the assumption of passive advection by the large-scale three-dimensional winds, show that in the 'high region' the ozone poor air was part of the polar vortex, which was centered off the pole and extended over Lauder for several days, while in the 'low region' the ozone poor air was mixed in from low latitudes. A rapid recovery of the ozone column density, by more than 110 DU within 24 hours, was observed when in the low region an ozone rich filament of the polar vortex moved over Lauder, while in the high region the (ozone poor) high part of the vortex moved away.

Brinksma, E. J.↗
NASA NTRS2000

The Impact of Withholding Observations from TOMS or SBUV Instruments on the GEOS Ozone Data Assimilation System

In a data assimilation system (DAS), model forecast atmospheric fields, observations and their respective statistics are combined in an attempt to produce the best estimate of these fields. Ozone observations from two instruments are assimilated in the Goddard Earth Observing System (GEOS) ozone DAS: the Total Ozone Mapping Spectrometer (TOMS) and the Solar Backscatter Ultraviolet (SBUV) instrument. The assimilated observations are complementary; TOMS provides a global daily coverage of total column ozone, without profile information, while SBUV measures ozone profiles and total column ozone at nadir only. The purpose of this paper is to examine the performance of the ozone assimilation system in the absence of observations from one of the instruments as it can happen in the event of a failure of an instrument or when there are problems with an instrument for a limited time. Our primary concern is for the performance of the GEOS ozone DAS when it is used in the operational mode to provide near real time analyzed ozone fields in support of instruments on the Terra satellite. In addition, we are planning to produce a longer term ozone record by assimilating historical data. We want to quantify the differences in the assimilated ozone fields that are caused by the changes in the TOMS or SBUV observing network. Our primary interest is in long term and large scale features visible in global statistics of analysis fields, such as differences in the zonal mean of assimilated ozone fields or comparisons with independent observations, While some drifts in assimilated fields occur immediately, after assimilating just one day of different observations, the others develop slowly over several months. Thus, we are also interested in the length of time, which is determined from time series, that is needed for significant changes to take place.

Stajner, Ovanka↗
NASA NTRS2000

Airborne Measurements of Nitric Oxide, Nitrogen Dioxide, Ozone, and Total Reactive Nitrogen During the NASA Global Tropospheric Experiment

Fabrication of the University of Michigan Multichannel Chemiluminescence Instrument (UMMCI) was completed in early 1996 and the instrument participated in test flights on the NASA P3B at Wallops Island prior to integration and deployment for the PEM- Tropics A Mission. The UMMCI consists of 4 channels for simultaneous measurements of ozone and NO with the option for measurements of NO2 and NOy (total reactive nitrogen) when converters are placed upstream of the NO channels. Each NO channel consists of a zeroing volume and reaction vessel, while the ozone channel consists of an ozone catalyst (or scrubber) trap that is not in line with the reaction vessel. The detectors in all for channels are Hamamatsu photomultiplier tubes, which are followed by pulse amplifier discriminators on the NO channels and an electrometer on the ozone channel. Schematics of the Detector Module and NOx/03 Probe Insert and Diagrams of the Control and Data System, the Power and Ground System, the Gas Flow System, and the Calibration System Flow are attached. Intercomparisons were conducted with G. Gregory, NASA/Langley, during the test flights (following prior calibration of the ozone generator/calibrators at the Wallops Long-Path Absorption facility). Initial test results appeared to be reasonable, and instrument characterization studies proceeded for the ozone channel and the 3 NO channels until deployment for integration for the PEM-Tropics Mission. Ozone data was obtained for Flights #4, and 6-2 1, and finalized data was submitted to the PEM-Tropics Data Archive and to the Science Team during the April 1997 Data Workshop. Although it initially appeared that the instrument sensitivity varied, subsequent tests showed that this was the fault of a leak in the ozone calibrator. In fact; the instrument sensitivity has not been observed to vary in a large number of tests over the years since the PEM-Tropics mission. We have, therefore, a very high degree of confidence in the O3 data that we submitted. NO data was obtained for all flights except the mission out of Christmas Island and the subsequent return to Hawaii, during which time the NO channels were contaminated with back-flushing pure NO from the O3 channel. The NO channels were found to suffer from a varying artifact (7 - 22 pptv) which made the instrument's results unreliable for the marine boundary layer portions of the missions (where conditions were extremely clean with NO typically < 2 pptv and O3 only 8 ppbv). Nonetheless, the NO values were an upper limit and were quite useful in identifying pollution layers and outflow from the Latin American Continent. NO data was submitted to the archive for all flights during which data was obtained. Ozone data from the P3B was among the results presented in several peer-reviewed publications. Notably, the ozone data supported the first published finding of evidence for the occurrence of aerosol nucleation in the marine boundary layer. As well, the ozone data was utilized in a treatment of the wavenumber spectra of winds, temperature and trace gases and to demonstrate the occurrence of layering as observed by the P3B during PEM-Tropics A . O3 and NO data were used in an assessment of the impact of southern hemispheric biomass burning, and in the role of NOx and O3 in HOx photochemistry during the PEM Tropics A mission. These data, along with other species measured during PEM-Tropics A, have also been employed in the generation of climatologies for tropospheric ozone and its precursors by the PI's research group.

Carroll, Mary Anne↗
NASA NTRS2000

The Interaction Between Dynamics and Chemistry of Ozone in the Set-Up Phase of the Northern Hemisphere Polar Vortex

Understanding stratospheric ozone loss to the point of accurately predicting ozone in the future requires correctly distinguishing chemical from transport-induced changes in ozone. For example, evaluating the impact of chlorine reduction in controlling stratospheric ozone loss requires estimating the amount of ozone lost in chemical reactions in the polar winter and spring. The Northern Hemisphere winter polar region is a particularly crucial and interesting area because it appears that the Northern vortex may currently be poised near the threshold of extreme ozone destruction such as that which now occurs annually in the Antarctic ozone "hole." In this presentation we explore the interaction of ozone transport and chemistry through the Northern late summer and fall seasons as the vortex circulation becomes established. This phase of the seasonal cycle determines the starting point for heterogeneous processes and chlorine-driven loss that take control in the winter vortex. Using a combination of profile data from POAM, HALOE, and in situ measurements, we show that relatively low ozone at high latitudes in the middle stratosphere is associated with vortex airmasses and that these ozone abundances evolve photochemically from characteristically higher values at the end of the summer. The zonal variance of ozone mixing ratio also increases greatly at this time consistent with increasing wave-driven transport. Comparison with a three-dimensional chemistry-transport model is used to generalize the findings from the limited set of observations and quantify the relative roles of transport and chemistry in determining the ozone mixing ratio distributions.

Kawa, S.R.↗
NASA NTRS2000

Tropospheric Ozone Profile Information Derived From "Cloud Slicing"

This study introduces a new approach to obtain ozone vertical profile information given coincident satellite measurements of both cloud-top pressure and above-cloud column ozone. This method is denoted "cloud slicing". In this study information of cloud-top pressure is derived from Geostationary Orbital Earth Satellite (GOES) infrared data, while above-cloud column ozone is obtained from the Earth Probe total ozone mapping spectrometer (TOMS) instrument. Several case examples are presented showing the feasibility of this technique as well as providing new geophysical results. Because the TOMS instrument measures backscattered UV radiation, it does detect ozone lying below dense water vapor clouds. This opaque property of TOMS can be used directly in conjunction with co-located cloud-top pressure data to derive ozone profile information in the troposphere. The cloud slicing method is an extension of the "Convective Cloud Differential" (CCD) method. In the CCD method, tropospheric column ozone (i.e., the total vertical column of ozone lying in the troposphere) is computed by taking total column ozone with low reflectivity (R less than 0.2) and subtracting from this a nearby measurement of above-cloud column ozone amount under conditions of high reflectivity (R greater than 0.9). (High reflectivity away from snow/ice conditions coincides with strong convection and tropopause-level clouds). The key element in determining tropospheric ozone profile information from the cloud slicing method is to have simultaneous and co-located measurements of both above-cloud column ozone and cloud-top pressure.

Ziemke, Jerald R.↗
NASA NTRS2002

Upper Tropospheric Ozone Between Latitudes 60S and 60N Derived from Nimbus 7 TOMS/THIR Cloud Slicing

This study evaluates the spatial distributions and seasonal cycles in upper tropospheric ozone (pressure range 200-500 hPa) from low to high latitudes (60S to 60N) derived from the satellite retrieval method called "Cloud Slicing." Cloud Slicing is a unique technique for determining ozone profile information in the troposphere by combining co-located measurements of cloud-top, pressure and above-cloud column ozone. For upper tropospheric ozone, co-located measurements of Nimbus 7 Total Ozone Mapping Spectrometer (TOMS) above-cloud column ozone, and Nimbus 7 Temperature Humidity Infrared Radiometer (THIR) cloud-top pressure during 1979-1984 were incorporated. In the tropics, upper tropospheric ozone shows year-round enhancement in the Atlantic region and evidence of a possible semiannual variability. Upper tropospheric ozone outside the tropics shows greatest abundance in winter and spring seasons in both hemispheres with largest seasonal and largest amounts in the NH. These characteristics are similar to lower stratospheric ozone. Comparisons of upper tropospheric column ozone with both stratospheric ozone and a proxy of lower stratospheric air mass (i.e., tropopause pressure) from National Centers for Environmental Prediction (NCEP) suggest that stratosphere-troposphere exchange (STE) may be a significant source for the seasonal variability of upper tropospheric ozone almost everywhere between 60S and 60N except in low latitudes around 10S to 25N where other sources (e.g., tropospheric transport, biomass burning, aerosol effects, lightning, etc.) may have a greater role.

Ziemke, Jerald R.↗
NASA NTRS1996

Decadal evolution of the Antarctic ozone hole

Ozone column amounts obtained by the total ozone mapping spectrometer (TOMS) in the southern polar region are analyzed during late austral winter and spring (days 240-300) for 1980-1991 using area-mapping techniques and area-weighted vortex averages. The vortex here is defined using the -50 PVU (1 PVU = 1.0 x 10(-6) K kg-1 m2 s-1) contour on the 500 K isentropic surface. The principal results are: (1) there is a distinct change after 1985 in the vortex-averaged column ozone depletion rate during September and October, the period of maximum ozone loss, and (2) the vortex-averaged column ozone in late August (day 240) has dropped by 70 Dobson units (DU) in a decade due to the loss in the dark and the dilution effect. The mean ozone depletion rate in the vortex between day 240 and the day of minimum vortex-averaged ozone is about 1 DU d-1 at the beginning of the decade, increasing to about 1.8 DU d-1 by 1985, and then apparently saturating thereafter. The vortex-average column ozone during September and October has declined at the rate of 11.3 DU yr-1 (3.8%) from 1980 to 1987 (90 DU over 8 years) and at a smaller rate of 2 DU yr-1 (0.9%) from 1987 to 1991 (10 DU over 5 years, excluding the anomalous year 1988). We interpret the year-to-year trend in the ozone depletion rate during the earlier part of the decade as due to the rise of anthropogenic chlorine in the atmosphere. The slower trend at the end of the decade indicates saturation of ozone depletion in the vortex interior, in that chlorine amounts in the mid-1980s were already sufficiently high to deplete most of the ozone in air within the isolated regions of the lower-stratospheric polar vortex. In subsequent years, increases in stratospheric chlorine may have enhanced wintertime chemical loss of ozone in the south polar vortex even before major losses during the Antarctic spring.

Non-NASA Center↗
NASA NTRS2007

Chemical Data Assimilation Estimates of Continental US Ozone and Nitrogen Budgets during INTEX-A

Global ozone analyses, based on assimilation of stratospheric profile and ozone column measurements, and NOy predictions from the Real-time Air Quality Modeling System (RAQMS) are used to estimate the ozone and NOy budget over the Continental US during the July-August 2004 Intercontinental Chemical Transport Experiment-North America (INTEX-A). Comparison with aircraft, satellite, surface, and ozonesonde measurements collected during the INTEX-A show that RAQMS captures the main features of the global and Continental US distribution of tropospheric ozone, carbon monoxide, and NOy with reasonable fidelity. Assimilation of stratospheric profile and column ozone measurements is shown to have a positive impact on the RAQMS upper tropospheric/lower stratosphere ozone analyses, particularly during the period when SAGE III limb scattering measurements were available. Eulerian ozone and NOy budgets during INTEX-A show that the majority of the Continental US export occurs in the upper troposphere/lower stratosphere poleward of the tropopause break, a consequence of convergence of tropospheric and stratospheric air in this region. Continental US photochemically produced ozone was found to be a minor component of the total ozone export, which was dominated by stratospheric ozone during INTEX-A. The unusually low photochemical ozone export is attributed to anomalously cold surface temperatures during the latter half of the INTEX-A mission, which resulted in net ozone loss during the first 2 weeks of August. Eulerian NOy budgets are shown to be very consistent with previously published estimates. The NOy export efficiency was estimated to be 24 percent, with NOx+PAN accounting for 54 percent of the total NOy export during INTEX-A.

Pierce, Robert B.↗
NASA NTRS2010

Multi-Model Assessment of the Factors Driving the Ozone Evolution Over the 21st Century

The evolution of ozone from 1960 to 2100 is examined in simulations from fourteen chemistry-climate models. There is general agreement among the models at the broadest levels, with all showing column ozone decreasing at all latitudes from 1960 to around 2000, then increasing at all latitudes over the first half of the 21 st century (21 C), and latitudinal variations in the rate of increase and date of return to historical values. In the second half of the century, ozone is projected to carry on increasing, level off or even decrease depending on the latitude, resulting in variable dates of return to historical values at latitudes where column ozone has declined below those levels. Separation into partial column above and below 20 hPa reveals that these latitudinal differences are almost completely due to differences in the lower stratosphere. At all latitudes, upper stratospheric ozone increases throughout the 21 C and returns to 1960 levels before the end of the century, although there is a spread among the models in dates that ozone returns to historical values. Using multiple linear regression the upper stratospheric ozone increase comes from almost equal contributions due to decrease in halogens and cooling from increased greenhouse gas concentrations. The evolution of lower stratospheric ozone differs with latitude. In the tropical lower stratosphere an increase in tropical upwelling causes a steady decrease in ozone through the 21C, and total column ozone does not return to 1960 levels in all models. In contrast, lower stratospheric and total column ozone in middle and high latitudes increases during the 21 C and returns to 1960 levels. For all models there is an earlier return for ozone to historical levels in the northern hemisphere. This is thought to be due to interhemispheric differences in transport.

Oman, L.↗
NASA NTRS2012

Highlights of TOMS Version 9 Total Ozone Algorithm

The fundamental basis of TOMS total ozone algorithm was developed some 45 years ago by Dave and Mateer. It was designed to estimate total ozone from satellite measurements of the backscattered UV radiances at few discrete wavelengths in the Huggins ozone absorption band (310-340 nm). Over the years, as the need for higher accuracy in measuring total ozone from space has increased, several improvements to the basic algorithms have been made. They include: better correction for the effects of aerosols and clouds, an improved method to account for the variation in shape of ozone profiles with season, latitude, and total ozone, and a multi-wavelength correction for remaining profile shape errors. These improvements have made it possible to retrieve total ozone with just 3 spectral channels of moderate spectral resolution (approx. 1 nm) with accuracy comparable to state-of-the-art spectral fitting algorithms like DOAS that require high spectral resolution measurements at large number of wavelengths. One of the deficiencies of the TOMS algorithm has been that it doesn't provide an error estimate. This is a particular problem in high latitudes when the profile shape errors become significant and vary with latitude, season, total ozone, and instrument viewing geometry. The primary objective of the TOMS V9 algorithm is to account for these effects in estimating the error bars. This is done by a straightforward implementation of the Rodgers optimum estimation method using a priori ozone profiles and their error covariances matrices constructed using Aura MLS and ozonesonde data. The algorithm produces a vertical ozone profile that contains 1-2.5 pieces of information (degrees of freedom of signal) depending upon solar zenith angle (SZA). The profile is integrated to obtain the total column. We provide information that shows the altitude range in which the profile is best determined by the measurements. One can use this information in data assimilation and analysis. A side benefit of this algorithm is that it is considerably simpler than the present algorithm that uses a database of 1512 profiles to retrieve total ozone. These profiles are tedious to construct and modify. Though conceptually similar to the SBUV V8 algorithm that was developed about a decade ago, the SBUV and TOMS V9 algorithms differ in detail. The TOMS algorithm uses 3 wavelengths to retrieve the profile while the SBUV algorithm uses 6-9 wavelengths, so TOMS provides less profile information. However both algorithms have comparable total ozone information and TOMS V9 can be easily adapted to use additional wavelengths from instruments like GOME, OMI and OMPS to provide better profile information at smaller SZAs. The other significant difference between the two algorithms is that while the SBUV algorithm has been optimized for deriving monthly zonal means by making an appropriate choice of the a priori error covariance matrix, the TOMS algorithm has been optimized for tracking short-term variability using month and latitude dependent covariance matrices.

Bhartia, Pawan↗
NASA NTRS2014

Understanding Differences in Chemistry Climate Model Projections of Stratospheric Ozone

Chemistry climate models (CCMs) are used to project future evolution of stratospheric ozone as concentrations of ozone-depleting substances (ODSs) decrease and greenhouse gases increase, cooling the stratosphere. CCM projections exhibit not only many common features but also a broad range of values for quantities such as year of ozone return to 1980 and global ozone level at the end of the 21st century. Multiple linear regression is applied to each of 14 CCMs to separate ozone response to ODS concentration change from that due to climate change. We show that the sensitivity of lower stratospheric ozone to chlorine change Delta Ozone/Delta inorganic chlorine is a near-linear function of partitioning of total inorganic chlorine into its reservoirs; both inorganic chlorine and its partitioning are largely controlled by lower stratospheric transport. CCMs with best performance on transport diagnostics agree with observations for chlorine reservoirs and produce similar ozone responses to chlorine change. After 2035, differences in Delta Ozone/Delta inorganic chlorine contribute little to the spread in CCM projections as the anthropogenic contribution to inorganic chlorine becomes unimportant. Differences among upper stratospheric ozone increases due to temperature decreases are explained by differences in ozone sensitivity to temperature change Delta Ozone/Delta T due to different contributions from various ozone loss processes, each with its own temperature dependence. Ozone decrease in the tropical lower stratosphere caused by a projected speedup in the Brewer-Dobson circulation may or may not be balanced by ozone increases in the middle- and high-latitude lower stratosphere and upper troposphere. This balance, or lack thereof, contributes most to the spread in late 21st century projections.

Stratospheric Transport↗
NASA NTRS2019

Ozone Vertical Profile Satellite Measurements by S-NPP OMPS, Aura MLS, and Sentinel-5P TROPOMI

NASA has been monitoring ozone variations from space since 1970 with the launch of the Backscatter Ultraviolet instrument (BUV) on Nimbus- 4. Ozone in the Earth’s stratosphere and troposphere plays a crucial role in protecting life from harmful solar UV radiation, and it also influences Earth’s climate. The vertical distribution of ozone is used in modeling forecasts, verifying model analysis and simulations, and improving the measurement of tropospheric ozone that is a toxic constituent of air pollution. The Microwave Limb Sounder (MLS) on the EOS Aura spacecraft has been monitoring long-term continuous stratosphere ozone vertical behaviors since 2004. The Ozone Mapper Profile Suite (OMPS) on the Suomi National Polar-orbiting Partnership (S-NPP) was launched in 2011. Two of its three instruments, the Limb Profiler (LP) and the Nadir Profiler (NP), are designed to map ozone profiles with full global coverage (~6 days for NP) and a high level of vertical accuracy (1-km reporting record for LP) in the stratosphere and upper troposphere. The TROPOspheric Monitoring Instrument (TROPOMI) on the Copernicus Sentinel-5 Precursor (S5P), launched in 2017, aims to retrieve ozone profiles in both the troposphere and up to top-of-atmosphere (TOA) by using UV radiation measurements in a spectral range of 270-320 nm. S5P/TROPOMI ozone profile products are planned to become available in April 2020. This presentation will concentrate on satellite ozone vertical profile data collections from OMPS and MLS which are archived at the NASA Goddard Earth Sciences Data and Information Services Center (GES DISC). TROPOMI ozone vertical profiles for the troposphere and to top-of-atmosphere will become available at NASA GES DISC in 2020. The presentation briefly explores their potential complementary usability in determining three-dimensional ozone global distributions with high temporal and spatial resolutions.

Zeng, Jian↗
NASA NTRSDate not supplied

Formaldehyde Column Density as an Indicator for Elevated Surface Ozone

Efforts to observe near-surface ozone directly from space are hindered by the limited sensitivity of ozone satellite retrievals to the lower troposphere. Formaldehyde (HCHO) column observations from the NASA DISCOVER-AQ campaign showed a strong relationship with surface ozone, particularly when biogenic volatile organic compounds (VOCs) were the dominant ozone precursor due to their strong temperature-driven variability. Both tropospheric ozone and HCHO are secondarily produced through the oxidation of VOCs and in regions where the main fate of RO2 is reaction with NO, thus formaldehyde and ozone are generally co-produced. This work explores the relationship between column formaldehyde and surface ozone using data from two air quality research campaigns, the Long Island Sound Tropospheric Ozone Study (LISTOS) in 2018 and the Korea U.S. - Air Quality (KORUS-AQ) campaign in 2016. These campaigns included HCHO column information from airborne in-situ profiling and remote sensing and ground-based Pandora spectrometers in combination with surface ozone monitors in each region. These data are used to further explore the HCHO-ozone relationship and its potential for identifying areas of elevated ozone using remote sensing or satellite observations of column HCHO alone. These two regions offer a valuable comparison given their different VOC mixtures and the higher NOx levels in Seoul that result in ozone titration effects. This work will also address the potential for this application with future geostationary satellite observations.

Laura Margaret Judd↗
NASA NTRS2013

Stratospheric Ozone Response in Experiments G3 and G4 of the Geoengineering Model Intercomparison Project (GeoMIP)

Geoengineering with stratospheric sulfate aerosols has been proposed as a means of temporarily cooling the planet, alleviating some of the side effects of anthropogenic CO2 emissions. However, one of the known side effects of stratospheric injections of sulfate aerosols is a decrease in stratospheric ozone. Here we show results from two general circulation models and two coupled chemistry climate models that have simulated stratospheric sulfate aerosol geoengineering as part of the Geoengineering Model Intercomparison Project (GeoMIP). Changes in photolysis rates and upwelling of ozone-poor air in the tropics reduce stratospheric ozone, suppression of the NOx cycle increases stratospheric ozone, and an increase in available surfaces for heterogeneous chemistry modulates reductions in ozone. On average, the models show a factor 20-40 increase of the sulfate aerosol surface area density (SAD) at 50 hPa in the tropics with respect to unperturbed background conditions and a factor 3-10 increase at mid-high latitudes. The net effect for a tropical injection rate of 5 Tg SO2 per year is a decrease in globally averaged ozone by 1.1-2.1 DU in the years 2040-2050 for three models which include heterogeneous chemistry on the sulfate aerosol surfaces. GISS-E2-R, a fully coupled general circulation model, performed simulations with no heterogeneous chemistry and a smaller aerosol size; it showed a decrease in ozone by 9.7 DU. After the year 2050, suppression of the NOx cycle becomes more important than destruction of ozone by ClOx, causing an increase in total stratospheric ozone. Contribution of ozone changes in this experiment to radiative forcing is 0.23 W m-2 in GISS-E2-R and less than 0.1 W m-2 in the other three models. Polar ozone depletion, due to enhanced formation of both sulfate aerosol SAD and polar stratospheric clouds, results in an average 5 percent increase in calculated surface UV-B.

aerosol↗
NASA NTRS2014

Reducing Uncertainty in Chemistry Climate Model Predictions of Stratospheric Ozone

Chemistry climate models (CCMs) are used to predict the future evolution of stratospheric ozone as ozone-depleting substances decrease and greenhouse gases increase, cooling the stratosphere. CCM predictions exhibit many common features, but also a broad range of values for quantities such as year of ozone-return-to-1980 and global ozone level at the end of the 21st century. Multiple linear regression is applied to each of 14 CCMs to separate ozone response to chlorine change from that due to climate change. We show that the sensitivity of lower atmosphere ozone to chlorine change deltaO3/deltaCly is a near linear function of partitioning of total inorganic chlorine (Cly) into its reservoirs; both Cly and its partitioning are controlled by lower atmospheric transport. CCMs with realistic transport agree with observations for chlorine reservoirs and produce similar ozone responses to chlorine change. After 2035 differences in response to chlorine contribute little to the spread in CCM results as the anthropogenic contribution to Cly becomes unimportant. Differences among upper stratospheric ozone increases due to temperature decreases are explained by differences in ozone sensitivity to temperature change deltaO3/deltaT due to different contributions from various ozone loss processes, each with their own temperature dependence. In the lower atmosphere, tropical ozone decreases caused by a predicted speed-up in the Brewer-Dobson circulation may or may not be balanced by middle and high latitude increases, contributing most to the spread in late 21st century predictions.

chemistry climate models↗
NASA NTRS2015

Evaluating a New Homogeneous Total Ozone Climate Data Record from GOME/ERS-2, SCIAMACHY/Envisat, and GOME-2/MetOp-A

The European Space Agency's Ozone Climate Change Initiative (O3-CCI) project aims at producing and validating a number of high-quality ozone data products generated from different satellite sensors. For total ozone, the O3-CCI approach consists of minimizing sources of bias and systematic uncertainties by applying a common retrieval algorithm to all level 1 data sets, in order to enhance the consistency between the level 2 data sets from individual sensors. Here we present the evaluation of the total ozone products from the European sensors Global Ozone Monitoring Experiment (GOME)/ERS-2, SCIAMACHY/Envisat, and GOME-2/MetOp-A produced with the GOME-type Direct FITting (GODFIT) algorithm v3. Measurements from the three sensors span more than 16 years, from 1996 to 2012. In this work, we present the latest O3-CCI total ozone validation results using as reference ground-based measurements from Brewer and Dobson spectrophotometers archived at the World Ozone and UV Data Centre of the World Meteorological Organization as well as from UV-visible differential optical absorption spectroscopy (DOAS)/Système D′Analyse par Observations Zénithales (SAOZ) instruments from the Network for the Detection of Atmospheric Composition Change. In particular, we investigate possible dependencies in these new GODFIT v3 total ozone data sets with respect to latitude, season, solar zenith angle, and different cloud parameters, using the most adequate type of ground-based instrument. We show that these three O3-CCI total ozone data products behave very similarly and are less sensitive to instrumental degradation, mainly as a result of the new reflectance soft-calibration scheme. The mean bias to the ground-based observations is found to be within the 1 plus or minus 1 percent level for all three sensors while the near-zero decadal stability of the total ozone columns (TOCs) provided by the three European instruments falls well within the 1-3 percent requirement of the European Space Agency's Ozone Climate Change Initiative project.

Satellite sensors↗
NASA NTRS2014

Tropospheric Ozone Increases over the Southern Africa Region: Bellwether for Rapid Growth in Southern Hemisphere Pollution?

Increases in free-tropospheric (FT) ozone based on ozonesonde records from the early 1990s through 2008 over two subtropical stations, Irene (near Pretoria, South Africa) and Réunion (21 deg. S, 55 deg. E; approx. 2800 km NE of Irene in the Indian Ocean), have been reported. Over Irene a large increase in the urban-influenced boundary layer (BL, 1.5-4 km) was also observed during the 18-year period, equivalent to 30%decade−1. Here we show that the Irene BL trend is at least partly due to a gradual change in the sonde launch times from early morning to the midday period. The FT ozone profiles over Irene in 1990-2007 are re-examined, filling in a 1995-1999 gap with ozone profiles taken during the Measurements of Ozone by Airbus In-service Aircraft (MOZAIC) project over nearby Johannesburg. A multivariate regression model that accounts for the annual ozone cycle, El Niño-Southern Oscillation (ENSO) and possible tropopause changes was applied to monthly averaged Irene data from 4 to 11 km and to 1992-2011 Réunion sonde data from 4 to 15 km. Statistically significant trends appear predominantly in the middle and upper troposphere (UT; 4-11 km over Irene, 4-15 km over Réunion) in winter (June-August), with increases 1 ppbv yr(exp. −1) over Irene and approx. 2 ppbv yr(exp. −1) over Réunion. These changes are equivalent to approx. 25 and 35-45%decade( exp. −1), respectively. Both stations also display smaller positive trends in summer, with a 45%decade(exp. −1) ozone increase near the tropopause over Réunion in December. To explain the ozone increases, we investigated a time series of dynamical markers, e.g., potential vorticity (PV) at 330-350 K. PV affects UT ozone over Irene in November-December but displays little relationship with ozone over Réunion. A more likely reason for wintertime FT ozone increases over Irene and Réunion appears to be long-range transport of growing pollution in the Southern Hemisphere. The ozone increases are consistent with trajectory origins of air parcels sampled by the sondes and with recent NOx emissions trends estimated for Africa, South America and Madagascar. For Réunion trajectories also point to sources from the eastern Indian Ocean and Asia.

Trends↗