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Tropospheric and stratospheric ozone from assimilation of Aura data

Ozone is an atmospheric trace gas with multiple impacts on the environment. Global ozone fields are needed for air quality predictions, estimation of the ultraviolet radiation reaching the surface, climate-radiation studies, and may also have an impact on longer-term weather predictions. We estimate global ozone fields in the stratosphere and troposphere by combining the data from EOS Aura satellite with an ozone model using data assimilation. Ozone exhibits a large temporal variability in the lower stratosphere. Our previous work showed that assimilation of satellite data from limb-sounding geometry helps constrain ozone profiles in that region. We assimilated ozone data from the Aura Microwave Limb Sounder (MLS) and the Ozone Monitoring Instrument (OMI) into the ozone system at NASA's Global Modeling and Assimilation Office (GMAO). Ozone is transported within a general circulation model (GCM) which includes parameterizations for stratospheric photochemistry, tropospheric chemistry, and a simple scheme for heterogeneous ozone loss. The focus of this study is on the representation of ozone in the lower stratosphere and tropospheric ozone columns. We plan to extend studies of tropospheric ozone distribution through assimilation of ozone data from the Tropospheric Emission Spectrometer (TES). Comparisons with ozone sondes and occultation data show that assimilation of Aura data reproduces ozone gradients and variability in the lower stratosphere well. We proceed by separating the contributions to temporal changes in the ozone field into those that are due to the model and those that are due to the assimilation of Aura data. The impacts of Aura data are illustrated and their role in the representation of ozone variability in the lower stratosphere and troposphere is shown.

Stajner, I.↗

Attribution of Stratospheric and Tropospheric Ozone Changes Between 1850 and 2014 in CMIP6 Models

We quantify the impacts of halogenated ozone-depleting substances (ODSs), greenhouse gases (GHGs), and short-lived ozone precursors on ozone changes between 1850 and 2014 using single-forcing perturbation simulations from several Earth system models with interactive chemistry participating in the Coupled Model Intercomparison Project Aerosol and Chemistry Model Intercomparison Project. We present the responses of ozone to individual forcings and an attribution of changes in ozone columns and vertically resolved stratospheric and tropospheric ozone to these forcings. We find that whilst substantial ODS-induced ozone loss dominates the stratospheric ozone changes since the 1970s, in agreement with previous studies, increases in tropospheric ozone due to increases in short-lived ozone precursors and methane since the 1950s make increasingly important contributions to total column ozone (TCO) changes. Increases in methane also lead to substantial extra-tropical stratospheric ozone increases. Impacts of nitrous oxide and carbon dioxide on stratospheric ozone are significant but their impacts on TCO are small overall due to several opposing factors and are also associated with large dynamical variability. The multi-model mean (MMM) results show a clear change in the stratospheric ozone trends after 2000 due to now declining ODSs, but the trends are generally not significantly positive, except in the extra-tropical upper stratosphere, due to relatively small changes in forcing over this period combined with large model uncertainty. Although the MMM ozone compares well with the observations, the inter-model differences are large primarily due to the large differences in the models' representation of ODS-induced ozone depletion.

Halogenated ozone-depleting substances↗

Ground Based, Millimeter Wave Measurement of Ozone in the Middle Atmosphere

There is a need for highly reliable measurements of stratospheric ozone. Policy makers worldwide concerned with public health rely oil a clear consensus from the scientific community as a basis for ozone-related environmental policy that has a significant impact oil national economies. Tile latest Such consensus was presented in WMO, and used in a 1999 meeting of the parties considering amendments to the Montreal Protocol oil Substances that Deplete the Ozone Layer. Tile scientific community, in turn, needs highly precise and accurate measurements of ozone levels, and small time derivatives of these levels, both in continued - development of its understanding of the physical and chemical processes involved and as clear evidence that these processes are occurring as stated. Over most of the world, changes in ozone levels are small. For example, over the heavily populated northern midlatitudes, the linearized rate of ozone decline is between 0.2% per year and 0.7% per year, depending on altitude. These values are small enough to make measurement requirements technically challenging. Data quality may suffer from imperfections in individual instruments. In one instance, early results from a satellite-borne ozone sensor were later found to be invalid because of calibration drift. Even in the absence of drift, tile absolute calibration of a new sensor may differ slightly from that of its predecessor in service. Most ozone remote sensing instruments operate at ultraviolet or infrared wavelengths where scattering from dust and aerosols must be taken into account; results from these systems may be or are affected following a major volcanic eruption, such as tile one at Mt. Pinatubo in 1991. Given these difficulties, a consensus of measurements from several independent systems is required to insure a reliable understanding of stratospheric ozone levels. Because of the above-described need for highly precise and accurate ozone measurements using several independent techniques, there was interest in developing several techniques which were known but not highly developed in the 1980's into systems capable of being used in ail operational manner to make measurements with the level of quality needed to-detect small trends in ozone levels. A ground-based microwave instrument capable of remotely sensing stratospheric ozone had been designed by tile Principal Investigator of the present project. This instrument was built at tile Millitech Corporation in South Deerfield, Massachusetts before tile present work began. (Funding for design and construction of the instrument came from sources other than the present grant.) Tile instrument measured the spectrum of one of the many emission lines produced by purely rotational transitions of ozone, one at a frequency of 110.8 GHz. The altitude distribution of ozone can. in principle, be retrieved from the details of the pressure-broadened spectrum of the ozone transition. However, the level of contamination of the spectral measurement by instrumentally induced artifacts must be very low in order to retrieve a ozone profile of useful quality from it. The Millitech instrument demonstrated spectral purity at ail adequate level, and there were promising ideas for instrumental improvements and for further development of the technique. The initial objectives of the present project, then, were to develop techniques for calibrating the Millitech instrument, to minimize artifacts in tile spectra it produces, to optimally retrieve ozone profiles from tile spectra, to test tile quality of the microwave profiles by comparing them with profiles obtained using several other, independent techniques over both short and periods of time, and to perform research using the ozone data gathered with the instrument.

Parrish, Alan↗

The Re-Analysis of Ozone Profile Data from a 41-Year Series of SBUV Instruments

In this study we present the validation of ozone profiles from a number of Solar Back Scattered Ultra Violet (SBUV) and SBUV/2 instruments that were recently reprocessed using an updated (Version 8.6) algorithm. The SBUV dataset provides the longest available record of global ozone profiles, spanning a 41-year period from 1970 to 2011 (except a 5-year gap in the 1970s) and includes ozone profile records obtained from the Nimbus-4 BUV and Nimbus-7 SBUV instruments, and a series of SBUV(/2) instruments launched on NOAA operational satellites (NOAA 09, 11, 14, 16, 17, 18, 19). Although modifications in instrument design were made in the evolution from the BUV instrument to the modern SBUV(/2) model, the basic principles of the measurement technique and retrieval algorithm remain the same. The long term SBUV data record allows us to create a consistent, calibrated dataset of ozone profiles that can be used for climate studies and trend analyses. In particular, we focus on estimating the various sources of error in the SBUV profile ozone retrievals using independent observations and analysis of the algorithm itself. For the first time we include in the metadata a quantitative estimate of the smoothing error, defined as the error due to profile variability that the SBUV observing system cannot inherently measure. The magnitude of the smoothing error varies with altitude, latitude, season and solar zenith angle. Between 10 and 1 hPa the smoothing errors for the SBUV monthly zonal mean retrievals are of the order of 1 %, but start to increase above and below this layer. The largest smoothing errors, as large as 15-20%, were detected in in the troposphere. The SBUV averaging kernels, provided with the ozone profiles in version 8.6, help to eliminate the smoothing effect when comparing the SBUV profiles with high vertical resolution measurements, and make it convenient to use the SBUV ozone profiles for data assimilation and model validation purposes. The smoothing error can also be minimized by combining layers of data, and we will discuss recommendations for this approach as well. The SBUV ozone profiles have been intensively validated against satellite profile measurements obtained from the Microwave Limb Sounders (MLS) (on board the UARS and AURA satellites), Stratospheric Aerosol and Gas Experiment (SAGE) and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). Also, we compare coincident and collocated SBUV ozone retrievals with observations made by ground-based instruments, such as microwave spectrometers, lidars, Umkehr instruments and balloon-borne ozonosondes. Finally, we compare the SBUV ozone profiles with output from the NASA GSFC GEOS-CCM model. In the stratosphere between 25 and 1 hPa the mean biases and standard deviations are within 5% for monthly mean ozone profiles. Above and below this layer the vertical resolution of the SBUV algorithm decreases and the effects of vertical smoothing should be taken into account. Though the SBUV algorithm has a coarser vertical resolution in the lower stratosphere and troposphere, it is capable of precisely estimating the integrated ozone column between the surface and 25 hPa. The time series of the tropospheric - lower stratospheric ozone column derived from SBUV agrees within 5% with the corresponding values observed by an ensemble of ozone sonde stations in North Hemisphere. Drift of the ozone time series obtained from each SBUV(/2) instrument relative to ground based and satellite measurements are evaluated and some features of individual SBUV(l2) instruments are discussed. In addition to evaluating individual instruments against independent observations, we also focus on the instrument to instrument consistency in the series. Overall, Version 8.6 ozone profiles obtained from two different SBUV(l2) instruments compare within a couple of percent during overlap periods and are consistently varying in time, with some exceptions. Some of the noted discrepancies might bssociated with ozone diurnal variations, since the difference in the local time of the observations for a pair of SBUV(l2) instruments could be several hours. Other issues include the potential short-term drift in measurements as the instrument orbit drifts, and measurements are obtained at high solar zenith angles (>85 ). Based on the results of the validation, a consistent, calibrated dataset of SBUV ozone profiles has been created based on internal calibration only.

Kramarova, Natalya↗

Retrieval of Ozone Column Content from Airborne Sun Photometer Measurements During SOLVE II: Comparison with SAGE III, POAM III,THOMAS and GOME Measurements

During the Second SAGE 111 Ozone Loss and Validation Experiment (SOLVE II), the 14- channel NASA Ames Airborne Trackmg Sunphotometer (AATS-14) was mounted on the NASA DC-8 and successfully measured spectra of total and aerosol optical depth (TOD and AOD) during the sunlit portions of eight science flights. Values of ozone column content above the aircraft have been derived from the AATS-14 data by using a linear least squares method. For each AATS-14 measured TOD spectrum, this method iteratively finds the ozone column content that yields the best match between measured and calculated TOD. The calculations assume the known Chappuis ozone band shape and a three-parameter AOD shape (quadratic in log-log space). Seven of the AATS-14 channels (each employing an interference filter with a nominal full-width at half maximum bandpass of -5 nm) are within the Chappuis band, with center wavelengths between 452.9 nm and 864.5 nm. One channel (604.4 nm) is near the peak, and three channels (499.4, 519.4 and 675.1 nm) have ozone absorption within 30-40% of that at the peak. For the typical DC-8 SOLVE II cruising altitudes of approx. 8-12 km and the background stratospheric aerosol conditions that prevailed during SOLVE 11, absorption of incoming solar radiation by ozone comprised a significant fraction of the aerosol-plus-ozone optical depth measured in the four AATS-14 channels centered between 499.4 and 675.1 nm. Typical AODs above the DC-8 ranged from 0.003-0.008 in these channels. For comparison, an ozone overburden of 0.3 atm-cm (300 DU) translates to ozone optical depths of 0.009,0.014, 0.041, and 0.012, respectively, at these same wavelengths. In this paper, we compare AATS-14 values of ozone column content with temporally and spatially near-coincident values derived from measurements acquired by the Stratospheric Aerosol and Gas Experiment III (SAGE III) and the Polar Ozone and Aerosol Measurement 111 (POAM III) satellite sensors. We also compare AATS-14 ozone retrievals during selected DC-8 latitudinal and longitudinal transects with total column ozone data acquired by the Total Ozone Mapping Spectrometer (TOMS) and the Global Ozone Monitoring Experiment (GOME) satellite sensors. To enable this comparison, the amount of ozone in the column below the aircraft is estimated by combining SAGE and/or POAM data with high resolution, fast response in-situ ozone measurements acquired during the DC-8 ascent at the start of each science flight.

Livingston, J.↗

Sensitivity of the Assimilated Ozone in the UTLS to Model and Data Selection Changes

This presentation will discuss the sensitivity of assimilated ozone fields in the upper troposphere and lower stratosphere (UTLS) to a number of factors, focusing mainly on aspects of data selection and the prediction model. This is important, because assimilation represents an attempt to construct our best estimates of the true ozone field; however, inaccuracies in the UTLS ozone distribution translate into an uncertainty in factors such as the calculated radiative forcing of climate or the inferred stratosphere-troposphere exchange (STE) of ozone. The 3D ozone data assimilation system, from NASA's Global Modeling and Assimilation Office (GMAO), combines observations of total ozone column and stratospheric profiles with predictions from an off-line, parameterized chemistry and transport model (pCTM) to produce six-hourly, global analyses. The first experiments discussed assimilate ozone retrievals from the Earth-Probe Total Ozone Mapping Spectrometer (EPTOMS) and stratospheric profiles from the Solar Backscatter UltraViolet/2 (SBUV/2) instrument. The SBUV/2 ozone data have a coarse vertical resolution, with increased uncertainty below the ozone maximum, and TOMS provides only total ozone columns. Thus, the assimilated ozone profiles in the UTLS region are only weakly constrained by the incoming SBUV and TOMS data. Consequently, the assimilated ozone distribution should be sensitive to changes in inputs to the statistical analysis scheme. Sensitivity studies have been conducted to examine the responses to TOMS and SBUV/2 data selection, modifications of the forecast and observation error covariance models, and the model formulation (turning off chemistry or using different wind analyses in the pCTM). The second set of experiments includes an additional data type: ozone retrieved from infrared limb-emission by MIPAS on Envisat. These data offer not only improved vertical resolution in the stratosphere, but also give measurements in the polar night. Comparisons of the assimilated ozone fields from both sets of experiments with independent observations, primarily ozone sondes, are used to determine the impact of each of these changes. It is shown that many of the changes have a significant impact on the UTLS ozone estimates. Implications for interpretation of STE and radiative forcing of climate are discussed.

Pawson, Steven↗

Assimilation of MLS and OMI Ozone Data

Ozone data from Aura Microwave Limb Sounder (MLS) and Ozone Monitoring Instrument (OMI) were assimilated into the ozone model at NASA's Global Modeling and Assimilation Office (GMAO). This assimilation produces ozone fields that are superior to those from the operational GMAO assimilation of Solar Backscatter Ultraviolet (SBUV/2) instrument data. Assimilation of Aura data improves the representation of the "ozone hole" and the agreement with independent Stratospheric Aerosol and Gas Experiment (SAGE) III and ozone sonde data. Ozone in the lower stratosphere is captured better: mean state, vertical gradients, spatial and temporal variability are all improved. Inclusion of OMI and MLS data together, or separately, in the assimilation system provides a way of checking how consistent OMI and MLS data are with each other, and with the ozone model. We found that differences between OMI total ozone column data and model forecasts decrease after MLS data are assimilated. This indicates that MLS stratospheric ozone profiles are consistent with OMI total ozone columns. The evaluation of error characteristics of OMI and MLS ozone will continue as data from newer versions of retrievals becomes available. We report on the initial step in obtaining global assimilated ozone fields that combine measurements from different Aura instruments, the ozone model at the GMAO, and their respective error characteristics. We plan to use assimilated ozone fields in estimation of tropospheric ozone. We also plan to investigate impacts of assimilated ozone fields on numerical weather prediction through their use in radiative models and in the assimilation of infrared nadir radiance data from NASA's Advanced Infrared Sounder (AIRS).

Stajner, I.↗

Interactive Ozone and Methane Chemistry in GISS-E2 Historical and Future Climate Simulations

The new generation GISS climate model includes fully interactive chemistry related to ozone in historical and future simulations, and interactive methane in future simulations. Evaluation of ozone, its tropospheric precursors, and methane shows that the model captures much of the largescale spatial structure seen in recent observations. While the model is much improved compared with the previous chemistry-climate model, especially for ozone seasonality in the stratosphere, there is still slightly too rapid stratospheric circulation, too little stratosphere-to-troposphere ozone flux in the Southern Hemisphere and an Antarctic ozone hole that is too large and persists too long. Quantitative metrics of spatial and temporal correlations with satellite datasets as well as spatial autocorrelation to examine transport and mixing are presented to document improvements in model skill and provide a benchmark for future evaluations. The difference in radiative forcing (RF) calculated using modeled tropospheric ozone versus tropospheric ozone observed by TES is only 0.016W/sq. m. Historical 20th Century simulations show a steady increase in whole atmosphere ozone RF through 1970 after which there is a decrease through 2000 due to stratospheric ozone depletion. Ozone forcing increases throughout the 21st century under RCP8.5 owing to a projected recovery of stratospheric ozone depletion and increases in methane, but decreases under RCP4.5 and 2.6 due to reductions in emissions of other ozone precursors. RF from methane is 0.05 to 0.18W/ sq. m higher in our model calculations than in the RCP RF estimates. The surface temperature response to ozone through 1970 follows the increase in forcing due to tropospheric ozone. After that time, surface temperatures decrease as ozone RF declines due to stratospheric depletion. The stratospheric ozone depletion also induces substantial changes in surface winds and the Southern Ocean circulation, which may play a role in a slightly stronger response per unit forcing during later decades. Tropical precipitation shifts south during boreal summer from 1850 to 1970, but then shifts northward from 1970 to 2000, following upper tropospheric temperature gradients more strongly than those at the surface.

Ozone↗

The threee-dimensional morphology of the Antarctic ozone hole

The three-dimensional morphology of the spring antarctic ozone distribution as determined by the Nimbus 7 Solar Backscatter Ultraviolet (SBUV) spectrometer instrument is presented for the period 1 to 11 October in 1986. The data show that a clearly defined minimum in ozone relative to the local ozone field extends throughout the stratosphere from the tropopause to above 50 km, though decreasing in intensity with altitude. Near 18 km ozone in the ozone hole is 50 percent less than the average surrounding ozone. But even at 50 km the ozone is 20 percent less than the surrounding ozone field. The ozone minimum in the upper stratosphere is displaced about 6 degrees toward the equator so that observations at a fixed station may provide the illusion that the ozone minimum is restricted only to low altitudes. While the ozone minimum is spatially coherent throughout the stratosphere, there are differences in the behavior of ozone at different altitudes that suggest the existence of at least three distinct altitude domains. Below 30 km ozone is characterized by classic ozone hole behavior. Between 33 and 43 km ozone is more stable, actually increasing during September and October. Above 43 km ozone has always decreased during September to a minimum in October, but it has suffered a long term decrease of 7 to 12 percent since 1979 similar to that seen at low altitudes.

Aikin, Arthur C.↗

Ozone Budgets from a Global Chemistry/ Transport Model and Comparison to Observations from POLARIS

The objective of the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) field mission was to obtain data to better characterize the summertime seasonal decrease of ozone at mid to high latitudes. The decrease in ozone occurs mainly in the lower stratosphere and is expected to result from in situ chemical destruction. Instrumented balloons and aircraft were used in POLARIS, along with satellites, to measure ozone and chemical species which are involved with stratospheric ozone chemistry. In order to close the seasonal ozone budget, however, ozone transport must also be estimated. Comparison to a global chemistry and transport model (CTM) of the stratosphere indicates how well the summertime ozone loss processes are simulated and thus how well we can predict the ozone response to changing amounts of chemical source gases. Moreover, the model gives insight into the possible relative magnitude of transport contributions to the seasonal ozone decline. Initial comparison to the Goddard CTM, which uses transport winds and temperatures from meteorological data assimilation, shows a high ozone bias in the model and an attenuated summertime ozone loss cycle. Comparison of the model chemical partitioning, and ozone catalytic loss rates to those derived from measurements shows fairly close agreement both at ER-2 altitudes (20 km) and higher. This suggests that the model transport is too active in resupplying ozone to the high latitude region, although chemistry failings cannot be completely ruled out. Comparison of ozone and related species will be shown along with a full diagnosis of the model ozone budget and its possible sources of error.

Kawa, S. Randy↗

History of Ozone Research: From Schonbein to the Present

In 1840, C.F. Schonbein recognized that the smell generated in several different electrical and chemical processes was a single substance. He named this substance "ozein" from the Greek for "to smell". This substance we know today as ozone. Several periods can be distinguished in the continued development of our understanding of ozone. Throughout the late 19th century, the identity and properties of ozone were established and described. Ozone was recognized to be a constituent of normal air and tests were established to measure its concentration. Its disinfectant properties were recognized. New methods were developed for making ozone in the laboratory. In 1879, ultraviolet spectroscopic techniques were applied to the measurement of the solar spectrum and it was discovered by Comu that the spectrum was cut off at about 300 nm wavelength. Hartley suggested, based on laboratory measurements, that this cutoff was due to ozone in the atmosphere which he correctly asserted was somewhere in the upper atmosphere. This began the period of development of the amount and distribution of ozone throughout the atmosphere. In 1930, Chapman put forward the first theory of the formation and destruction of ozone. By the mid-1960s it was becoming obvious that the description of the chemical loss term was inadequate. By the early 1970s the chemical destruction of ozone by the oxides of hydrogen, nitrogen, chlorine, and bromine was recognized as an essential element in the chemical balance determining the ozone concentration. Today, ozone is a broad research project which crosses the boundaries of traditional disciplines. Stratospheric ozone loss due to chlorofluorocarbons is a newsworthy item. The Antarctic ozone hole opens up every spring. The provisions of the Montreal Protocol were agreed upon by countries around the world and promise to reduce the future levels of ozone-destroying chlorine in the stratosphere. Ozone concentrations in polluted cities are a subject of local and national regulations to limit its potential for causing health problems and corrosive effects on materials. A lot is known about ozone but many new questions are still being developed.

Stolarski, Richard S.↗

Constructing Synoptic Maps of Stratospheric Column Ozone from HALOE, SAGE and Balloonsonde Data Using Potential Vorticity Isentropic Coordinate Transformations

In this study we utilize potential vorticity - isentropic (PVI) coordinate transformations as a means of combining ozone data from different sources to construct daily, synthetic three-dimensional ozone fields. This methodology has been used successfully to reconstruct ozone maps in particular regions from aircraft data over the period of the aircraft campaign. We expand this method to create high-resolution daily global maps of profile ozone data, particularly in the lower stratosphere, where high-resolution ozone data are sparse. Ozone climatologies in PVI-space are constructed from satellite-based SAGE II and UARS/HALOE data, both of which-use solar occultation techniques to make high vertical resolution ozone profile measurements, but with low spatial resolution. A climatology from ground-based balloonsonde data is also created. The climatologies are used to establish the relationship between ozone and dynamical variability, which is defined by the potential vorticity (in the form of equivalent latitude) and potential temperature fields. Once a PVI climatology has been created from data taken by one or more instruments, high-resolution daily profile ozone field estimates are constructed based solely on the PVI fields, which are available on a daily basis from NCEP analysis. These profile ozone maps could be used for a variety of applications, including use in conjunction with total ozone maps to create a daily tropospheric ozone product, as input to forecast models, or as a tool for validating independent ozone measurements when correlative data are not available. This technique is limited to regions where the ozone is a long-term tracer and the flow is adiabatic. We evaluate the internal consistency of the technique by transforming the ozone back to physical space and comparing to the original profiles. Biases in the long-term average of the differences are used to identify regions where the technique is consistently introducing errors. Initial results show the technique is useful in the lower stratosphere at most latitudes throughout the year,and in the winter hemisphere in the middle stratosphere. The results are problematic in the summer hemisphere middle stratosphere due to increased ozone photochemistry and weak PV gradients. Alternate techniques in these regions will be discussed. An additional limitation is the quality and resolution of the meteorological data.

Hollandsworth, Stacey M.↗

Ozone Budgets from a Global Chemistry/Transport Model and Comparison to Observations from POLARIS

The objective of the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) field mission was to obtain data to better characterize the summertime seasonal decrease of ozone at mid to high latitudes. The decrease in ozone occurs mainly in the lower stratosphere and is expected to result from in situ chemical destruction. Instrumented balloons and aircraft were used in POLARIS, along with satellites, to measure ozone and chemical species which are involved with stratospheric ozone chemistry. In order to close the seasonal ozone budget, however, ozone transport must also be estimated. Comparison to a global chemistry and transport model (CTM) of the stratosphere indicates how well the summertime ozone loss processes are simulated and thus how well we can predict the ozone response to changing amounts of chemical source gases. Moreover, the model gives insight into the possible relative magnitude of transport contributions to the seasonal ozone decline. Initial comparison to the Goddard CTM, which uses transport winds and temperatures from meteorological data assimilation, shows a high ozone bias in the model and an attenuated summertime ozone loss cycle. Comparison of the model chemical partitioning and ozone catalytic loss rates to those derived from measurements shows fairly close agreement both at ER-2 altitudes (20 km) and higher. This suggests that the model transport is too active in resupplying ozone to the high latitude region, although chemistry failings cannot be completely ruled out. Comparison of ozone and related species will be shown along with a full diagnosis of the model ozone budget and its possible sources of error.

Kawa, S. Randolph↗

An Assessment of the Ozone Loss During the 1999-2000 SOLVE Arctic Campaign

Ozone observations from ozonesondes, the lidars aboard the DC-8, in situ ozone measurements from the ER-2, and satellite ozone measurements from Polar Ozone and Aerosol Measurement III (POAM) were used to assess ozone loss during the Sage III Ozone Loss and Validation Experiment (SOLVE) 1999-2000 Arctic campaign. Two methods of analysis were used. In the first method a simple regression analysis is performed on the ozonesonde and POAM measurements within the vortex. In the second method, the ozone measurements from all available ozone data were injected into a free running diabatic trajectory model and carried forward in time from December 1 to March 15. Vortex ozone loss was then estimated by comparing the ozone values of those parcels initiated early in the campaign with those parcels injected later in the campaign. Despite the variety of observational techniques used during SOLVE, the measurements provide a fairly consistent picture. Over the whole vortex, the largest ozone loss occurs between 550 and 400 K potential temperatures (approximately 23-16 km) with over 1.5 ppmv lost by March 15, the end of the SOLVE mission period. An ozone loss rate of 0.04-0.05 ppmv/day was computed for March 15. Ozonesondes launched after March 15 suggest that an additional 0.5 ppmv or more ozone was lost between March 15 and April 1. The small disagreement between ozonesonde and POAM analysis of January ozone loss is found to be due to biases in vortex sampling. POAM makes most of its solar occultation measurements at the vortex edge during January 2000 which bias samples toward air parcels that have been exposed to sunlight and likely do experience ozone loss. Ozonesonde measurements and the trajectory technique use observations that are more distributed within the interior of the vortex. Thus the regression analysis of the POAM measurements tends to overestimate mid-winter vortex ozone loss. Finally, our loss calculations are broadly consistent with other loss computations using ER-2 tracer data and MLS satellite data, but we find no evidence for the 1992 high mid-January loss reported using the Match technique.

Schoeberl, Mark R.↗

Ozone Layer Observations

The US National Aeronautics and Space Administration (NASA) has been monitoring the ozone layer from space using optical remote sensing techniques since 1970. With concern over catalytic destruction of ozone (mid-1970s) and the development of the Antarctic ozone hole (mid-1980s), long term ozone monitoring has become the primary focus of NASA's series of ozone measuring instruments. A series of TOMS (Total Ozone Mapping Spectrometer) and SBUV (Solar Backscatter Ultraviolet) instruments has produced a nearly continuous record of global ozone from 1979 to the present. These instruments infer ozone by measuring sunlight backscattered from the atmosphere in the ultraviolet through differential absorption. These measurements have documented a 15 Dobson Unit drop in global average ozone since 1980, and the declines in ozone in the antarctic each October have been far more dramatic. Instruments that measure the ozone vertical distribution, the SBUV and SAGE (Stratospheric Aerosol and Gas Experiment) instruments for example, show that the largest changes are occurring in the lower stratosphere and upper troposphere. The goal of ozone measurement in the next decades will be to document the predicted recovery of the ozone layer as CFC (chlorofluorocarbon) levels decline. This will require a continuation of global measurements of total column ozone on a global basis, but using data from successor instruments to TOMS. Hyperspectral instruments capable of measuring in the UV will be needed for this purpose. Establishing the relative roles of chemistry and dynamics will require instruments to measure ozone in the troposphere and in the stratosphere with good vertical resolution. Instruments that can measure other chemicals important to ozone formation and destruction will also be needed.

McPeters, Richard↗

Increasing Springtime Ozone Mixing Ratios in the Free Troposphere Over Western North America

In the lowermost layer of the atmosphere - the troposphere - ozone is an important source of the hydroxyl radical, an oxidant that breaks down most pollutants and some greenhouse gases. High concentrations of tropospheric ozone are toxic, however, and have a detrimental effect on human health and ecosystem productivity1. Moreover, tropospheric ozone itself acts as an effective greenhouse gas. Much of the present tropospheric ozone burden is a consequence of anthropogenic emissions of ozone precursors resulting in widespread increases in ozone concentrations since the late 1800s. At present, east Asia has the fastest-growing ozone precursor emissions. Much of the springtime east Asian pollution is exported eastwards towards western North America. Despite evidence that the exported Asian pollution produces ozone, no previous study has found a significant increase in free tropospheric ozone concentrations above the western USA since measurements began in the late 1970s. Here we compile springtime ozone measurements from many different platforms across western North America. We show a strong increase in springtime ozone mixing ratios during 1995-2008 and we have some additional evidence that a similar rate of increase in ozone mixing ratio has occurred since 1984. We find that the rate of increase in ozone mixing ratio is greatest when measurements are more heavily influenced by direct transport from Asia. Our result agrees with previous modelling studies, which indicate that global ozone concentrations should be increasing during the early part of the twenty-first century as a result of increasing precursor emissions, especially at northern mid-latitudes, with western North America being particularly sensitive to rising Asian emissions. We suggest that the observed increase in springtime background ozone mixing ratio may hinder the USA s compliance with its ozone air quality standard.

Cooper, O. R.↗

Pre-industrial to End 21st Century Projections of Tropospheric Ozone from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75 %) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337+/-23 Tg, the ensemble mean burden for 1850 time slice is approx. 30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: −4% (−16 %) for RCP2.6, 2% (−7%) for RCP4.5, 1% (−9%) for RCP6.0, and 7% (18 %) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40-150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A unified approach to ozone budget specifications and a rigorous investigation of the factors that drive tropospheric ozone is recommended to help future studies attribute ozone changes and inter-model differences more clearly.

Troposphere↗

Trend Quality Ozone from NPP OMPS: The Version 2 Processing

A version 2 processing of data from two ozone monitoring instruments on Suomi NPP, the OMPS nadir ozone mapper and the OMPS nadir ozone profiler, has now been completed. The previously released data were useful for many purposes but were not suitable for use in ozone trend analysis. In this processing, instrument artifacts have been identified and corrected, an improved scattered light correction and wavelength registration have been applied, and soft calibration techniques were implemented to produce a calibration consistent with data from the series of SBUV/2 instruments. The result is a high-quality ozone time series suitable for trend analysis. Total column ozone data from the OMPS nadir mapper now agree with data from the SBUV/2 instrument on NOAA 19 with a zonal average bias of −0.2 % over the 60° S to 60° N latitude zone. Differences are somewhat larger between OMPS nadir profiler and N19 total column ozone, with an average difference of −1.1 % over the 60° S to 60° N latitude zone and a residual seasonal variation of about 2 % at latitudes higher than about 50°. For the profile retrieval, zonal average ozone in the upper stratosphere (between 2.5 and 4 hPa) agrees with that from NOAA 19 within ±3 % and an average bias of −1.1 %. In the lower stratosphere (between 25 and 40 hPa) agreement is within ±3 % with an average bias of +1.1 %. Tropospheric ozone produced by subtracting stratospheric ozone measured by the OMPS limb profiler from total column ozone measured by the nadir mapper is consistent with tropospheric ozone produced by subtracting stratospheric ozone from MLS from total ozone from the OMI instrument on Aura. The agreement of tropospheric ozone is within 10 % in most locations.

OMPS nadir ozone mapper↗