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Variability in Tropical Tropospheric Ozone as Observed by SHADOZ

The SHADOZ (Southern Hemisphere Additional Ozonesondes) ozone sounding network was initiated in 1998 to improve the coverage of tropical in-situ ozone measurements for satellite validation, algorithm development and related process studies. Over 2000 soundings have been archived at the central website, , for 12 stations: Ascension Island; Nairobi and Malindi, Kenya; Irene, South Africa; Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil; Paramaribo, Surinam. Some results to date indicate reliability of the measurement and highly variable interactions between ozone and tropical meteorology. For example: 1. By using ECC sondes with similar procedures, 5-10% accuracy and precision (1-sigma) of the sonde total ozone measurement was achieved [Thompson et al., 2003al; 2. Week-to-week variability in tropospheric ozone is so great that statistics are frequently not Gaussian and most stations vary up to a factor of 3 in column amount over the course of a year [Thompson et al., 2002b]. 3. Longitudinal variability in tropospheric ozone profiles is a consistent feature, with a 10- 15 DU column-integrated difference between Atlantic and Pacific sites; this is the cause of the zonal wave-one feature in total ozone [Shiotani, 1992]. The ozone record from Paramaribo, Surinam (6N, 55W) is a marked contrast to southern tropical ozone because Surinam is often north of the Intertropical Convergence Zone. Interpretations of SHADOZ time-series and approaches to classification suggested by SHADOZ data over Africa and the Indian Ocean will be described.

Thompson, Anne M.↗

Insights into Tropical Tropospheric Ozone from the 1998-2000 SHADOZ (Southern Hemisphere Additional Ozonesondes) Data Record

We describe the first overview of total, stratospheric and tropospheric ozone in the southern hemisphere tropics based on a three year, ten site record of ozone soundings from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network. Observations covering 1998-2000 were made over Ascension Island; Nairobi, Kenya; Irene, South Africa; Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil. The ozone data, with simultaneous temperature profiles to approximately 7 hPa and relative humidity to approximately 200 hPa, are at an archive: http://code9l6. gsfc.nasa.gov/Data_services/shadoz. Prominent features are highly variable tropospheric ozone, a zonal wave-one pattern in total (and tropospheric) column ozone, and signatures of the Quasi-Biennial Oscillation (QBO) in stratospheric ozone. Total, stratospheric and tropospheric column ozone amounts usually peak between August and November and are lowest in the first half of the year. Tropospheric ozone variability over the Indian and Pacific Ocean displays influences of the waning 1997-1998 Indian Ocean Dipole and ENSO (El Nino / Southern Oscillation), seasonal convection and pollution transport from Africa. Tropospheric ozone over the Atlantic Basin reflects regional subsidence and recirculation as well as pollution ozone from biomass burning.

Thompson, Anne M.↗

Impact of Surface Emissions to the Zonal Variability of Tropical Tropospheric Ozone and Carbon Monoxide for November 2004

The chemical and dynamical processes governing the zonal variability of tropical tropospheric ozone and carbon monoxide are investigated for November 2004 using satellite observations, in-situ measurements, and chemical transport models in conjunction with inverse-estimated surface emissions. Vertical ozone profile estimates from the Tropospheric Emission Spectrometer (TES) and ozone sonde measurements from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network show the so called zonal 'wave-one' pattern, which is characterized by peak ozone concentrations (70-80 ppb) centered over the Atlantic, as well as elevated concentrations of ozone over Indonesia and Australia (60-70 ppb) in the lower troposphere. Observational evidence from TES CO vertical profiles and Ozone Monitoring Instrument (OMI) NO2 columns point to regional surface emissions as an important contributor to the elevated ozone over Indonesia. This contribution is investigated with the GEOS-Chem chemistry and transport model using surface emission estimates derived from an optimal inverse model, which was constrained by TES and Measurements Of Pollution In The Troposphere (MOPITT) CO profiles (Jones et al., 2007). These a posteriori estimates, which were over a factor of 2 greater than climatological emissions, reduced differences between GEOS-Chem and TES ozone observations by 30-40% and led to changes in GEOS-Chem upper tropospheric ozone of up to 40% over Indonesia. The remaining residual differences can be explained in part by upper tropospheric ozone produced from lightning NOx in the South Atlantic. Furthermore, model simulations from GEOS-Chem indicate that ozone over Indonesian/Australian is more sensitive to changes in surface emissions of NOx than ozone over the tropical Atlantic.

tropical tropospheric ozone↗

Quantifying Interannual Variability of the UTLS Ozone Using Assimilation of Satellite Data

An accurate representation of spatial and temporal variability of the Upper Troposphere Lower Stratosphere (UTLS) ozone is essential for understanding both the tropospheric ozone budget and ozone s contribution to radiative forcing. The complex, dynamically driven structure of trace gas fields in the UTLS presents a challenge to data-based and modelling studies. Small features are not fully resolved in data from limb-sounding instruments such as the Microwave Limb Sounder on EOS-Aura (the EOS-MLS), but are captured in assimilation of those data as vertical structure is added from the assimilated meteorology. This will be demonstrated using a multi-year assimilation of EOS-MLS observations in the Goddard Earth Observing System, Version 5 (GEOS-5) data assimilation system. The results demonstrate the realism of the seasonal and year to year variability of laminar structures in the mid-latitudinal ozone field between years 2005-2007, for which independent validation data are available from the HIRDLS instrument. The analysis is done in the context of the underlying large scale dynamics. The lifetimes of most research instruments are too short for them to be used throughout the duration of long-term (at least 3 decades) reanalyses. For example, the EOS-MLS instrument has operated since mid-2004 until present. By contrast, Solar Backscatter Ultra Violet (SBUV) measurements provide continuous data since late 1978, but their vertical resolution is insufficient to represent the profile shape in the UTLS. Assimilation of these SBUV/2 observations in the GEOS-5 data assimilation system has hitherto not captured a realistic ozone structure in the UTLS, even though transport studies using GEOS-5 wind fields do show such structures. We show that careful construction of the background error covariance structure in GEOS-5 can lead to more realistic UTLS ozone fields when assimilating SBUV/2 observations. The reasoning behind this will be discussed, emphasizing the need to retain the sharp gradient of ozone concentrations across the tropopause. We analyze the UTLS ozone distributions in multi-year SBUV/2 assimilation experiments, comparing the results against the independent HIRDLSdataset and, for a longer period, with the MLS assimilation and discuss the consequences for tropospheric ozone and radiative forcing.

Wargan, K.↗

Recent advances in satellite observations of solar variability and global atmospheric ozone

A description is given of the temporal behavior of the sun as an ultraviolet variable star in relation to daily zonal means of atmospheric ozone from the total amount to that above the 10-mb and 4-mb pressure levels. A significant correlation has been observed between enhancements in the ultraviolet solar irradiances and terrestrial passages of the solar magnetic field sector boundary structure. However, it has not yet been possible to separate solar from the dynamical effects on the variability in the zonal means of ozone. Attention is given to global changes in ozone which have been derived from the satellite observations in terms of season, solar variability, and major stratospheric disturbances such as stratospheric warmings.

Heath, D. F.↗

Seasonal Variability of Middle Latitude Ozone in the Lowermost Stratosphere Derived from Probability Distribution Functions

We present a study of the distribution of ozone in the lowermost stratosphere with the goal of characterizing the observed variability. The air in the lowermost stratosphere is divided into two population groups based on Ertel's potential vorticity at 300 hPa. High (low) potential vorticity at 300 hPa indicates that the tropopause is low (high), and the identification of these two groups is made to account for the dynamic variability. Conditional probability distribution functions are used to define the statistics of the ozone distribution from both observations and a three-dimensional model simulation using winds from the Goddard Earth Observing System Data Assimilation System for transport. Ozone data sets include ozonesonde observations from northern midlatitude stations (1991-96) and midlatitude observations made by the Halogen Occultation Experiment (HALOE) on the Upper Atmosphere Research Satellite (UARS) (1994- 1998). The conditional probability distribution functions are calculated at a series of potential temperature surfaces spanning the domain from the midlatitude tropopause to surfaces higher than the mean tropical tropopause (approximately 380K). The probability distribution functions are similar for the two data sources, despite differences in horizontal and vertical resolution and spatial and temporal sampling. Comparisons with the model demonstrate that the model maintains a mix of air in the lowermost stratosphere similar to the observations. The model also simulates a realistic annual cycle. Results show that during summer, much of the observed variability is explained by the height of the tropopause. During the winter and spring, when the tropopause fluctuations are larger, less of the variability is explained by tropopause height. This suggests that more mixing occurs during these seasons. During all seasons, there is a transition zone near the tropopause that contains air characteristic of both the troposphere and the stratosphere. The relevance of the results to the assessment of the environmental impact of aircraft effluence is also discussed.

Rood, Richard B.↗

Ozone Pollution, Transport and Variability: Examples from Satellite and In-Situ Observations

Regional and intercontinental transport of ozone has been observed from satellite, aircraft and sounding data. Over the past several years, we have developed new tropospheric ozone retrieval techniques from the TOMS (Total Ozone Mapping Spectrometer) satellite instrument that are of sufficient resolution to follow pollution episodes. The modified-residual technique uses Level 2 total ozone and was used to follow the 1997 fires in the wake of the El-Nino-related fires in southeast Asia and the Indonesian maritime continent. The TOMS-direct method ('TDOT' = TOMS Direct Ozone in the Troposphere) is a newer algorithm that uses TOMS radiances directly to extract tropospheric ozone. Ozonesonde data that have been taken in campaigns (e.g. TRACE-P) and more consistently in the SHADOZ (Southern Hemisphere Additional Ozonesondes) project, reveal layers of pollution traceable with trajectories. Examples will be shown of long-range transport and recirculation over Africa during SAFARI-2000.

Thompson, Anne↗

Solar UV variability - Effects on stratospheric ozone, trace constituents and thermal structure

The effect of long-term (11-year solar cycle) solar UV variability on stratospheric chemical and thermal structure has been studied using a time-dependent one-dimensional model. Previous studies have suggested substantial variations in local and total ozone, and in stratospheric thermal structure from solar minimum to solar maximum. It is shown that significant variations also occur in some of the trace constituents. Members of the HOx family and N2O exhibit the largest variations, and these changes, if detected, may provide additional means of verifying the presence of solar UV variability and its effects. Some of the species show large phase differences with the assumed solar flux variation. The role of chemical and transport time constants on the time variations of the trace species is examined. Comparisons with reported ozone and temperature data show reasonable agreement for the period 1960 to 1972.

Natarajan, M.↗

Impact of interannual variability (1979-1986) of transport and temperature on ozone as computed using a two-dimensional photochemical model

Values of the monthly mean heating rates and the residual circulation characteristics were calculated using NMC data for temperature and the solar backscattered UV ozone for the period between 1979 and 1986. The results were used in a two-dimensional photochemical model in order to examine the effects of temperature and residual circulation on the interannual variability of ozone. It was found that the calculated total ozone was more sensitive to variations in interannual residual circulation than in the interannual temperature. The magnitude of the modeled ozone variability was found to be similar to the observed variability, but the observed and modeled year-to-year deviations were, for the most part, uncorrelated, due to the fact that the model did not account for most of the QBO forcing and for some of the observed tropospheric changes.

Jackman, Charles H.↗

Ozone Contamination in Aircraft Cabins. Appendix B: Overview papers. In-flight measurements

The NASA Global Atmospheric Sampling Program ozone measurements were obtained to establish to characteristics of the ambient ozone concentration during routine operations and to determine the attenuation of ambient concentrations of cabin air systems from simultaneous ambient and in cabin measurements. The characteristics of ambient ozone include: (1) maximum concentration; (2) duration of ozone encounters; (3) frequency of ozone during a flight; (4) variability of ozone during a flight; (5) in relation to routes, altitude, and meteorological conditions.

Perkins, P. J.↗

The Role of Lightning in Controlling Interannual Variability of Tropical Tropospheric Ozone and OH and its Implications for Climate

Nitrogen oxides (NO(x) = NO + NO2) produced by lightning make a major contribution to the production of the dominant tropospheric oxidants (OH and ozone). These oxidants control the lifetime of many trace gases including long-lived greenhouse gases, and control the source-receptor relationship of inter-hemispheric pollutant transport. Lightning is affected by meteorological variability, and therefore represents a potentially important tropospheric chemistry-climate feedback. Understanding how interannual variability (IAV) in lightning affects IAV in ozone and OH in the recent past is important if we are to predict how oxidant levels may change in a future warmer climate. However, lightning parameterizations for chemical transport models (CTMs) show low skill in reproducing even climatological distributions of flash rates from the Lightning Imaging Sensor (LIS) and the Optical Transient Detector (OTD) satellite instruments. We present an optimized regional scaling algorithm for CTMs that enables sufficient sampling of spatiotemporally sparse satellite lightning data from LIS to constrain the spatial, seasonal, and interannual variability of tropical lightning. We construct a monthly time series of lightning flash rates for 1998-2010 and 35degS-35degN, and find a correlation of IAV in total tropical lightning with El Nino. We use the IAV-constraint to drive a 9-year hindcast (1998-2006) of the GEOS-Chem 3D chemical transport model, and find the increased IAV in LNO(x) drives increased IAV in ozone and OH, improving the model fs ability to simulate both. Although lightning contributes more than any other emission source to IAV in ozone, we find ozone more sensitive to meteorology, particularly convective transport. However, we find IAV in OH to be highly sensitive to lightning NO(x), and the constraint improves the ability of the model to capture the temporal behavior of OH anomalies inferred from observations of methyl chloroform and other gases. The sensitivity of OH is explained using photochemical reaction rates which show a "magnification" effect of the initial lightning NO perturbation on OH primary production, HO(x) recycling, and OH loss frequencies. This influence on OH may represent a negative feedback, if lightning increases in a warming world..

Murray, Lee T.↗

Investigation of the Short-Time Variability of Tropical Tropospheric Ozone

Since 1998, a ground based tropospheric ozone lidar has been running at Reunion Island and has been involved with a daily measurement campaign that was performed in the latter part of the biomass burning season, during November-December 1999. The averaged ozone profile obtained during November-December 1 999 agrees well with averaged ozone profile obtained from ozonesondes launch at Reunion during November-December (1992- 2001). Comparing weekly sonde launches (part of the Southern Hemisphere Additional Ozonesondes: SHADOZ program) with the daily ground-based lidar observations shows that some striking features of the day to day variability profiles are not observed in the sonde measurements. Ozone profiles respond to the nature of disturbances which vary from the one day to the next. The vertical ozone distribution at Reunion is examined as a function of prevailing atmospheric circulation. Backtrajectories show that most of the enhanced ozone crossed over biomass burning and convectively active regions in Madagascar and the southern African continent. The analyses of the meteorological data show that ozone stratification profiles are in agreement with the movement of the synoptical situations in November-December 1999. Three different sequences of transport are explained using wind fields. The first sequence from 23 to 25 November is characterized by Northerly transport, the second sequence from 26 to 30 November, the air masses are influenced by meridional transport. The third sequence from 2 to 6 December is characterized by westerly transport associated with the subtropical jet stream. The large standard deviations of lidar profiles in the middle and upper troposphere are in agreement with the upper wind variabilities which evidence passing ridge and trough disturbances. During the transition period between the dry season and the wet season, multiple ozone sources including stratosphere-troposphere exchanges, convection and biomass burning contribute to tropospheric ozone at Reunion Island through sporadic events characterized by a large spatial and temporal variability.

Randriambelo, Tantely↗

Average Versus High Surface Ozone Levels over the Continental USA: Model Bias, Background Influences, and Interannual Variability

US background ozone (O3) includes O3 produced from anthropogenic O3 precursors emitted outside of the USA, from global methane, and from any natural sources. Using a suite of sensitivity simulations in the GEOS-Chem global chemistry transport model, we estimate the influence from individual background sources versus US anthropogenic sources on total surface O3 over 10 continental US regions from 2004 to 2012. Evaluation with observations reveals model biases of +0-19ppb in seasonal mean maximum daily 8h average (MDA8) O3, highest in summer over the eastern USA. Simulated high-O3 events cluster too late in the season. We link these model biases to excessive regional O3 production (e.g., US anthropogenic, biogenic volatile organic compounds (BVOCs), and soil NOx, emissions), or coincident missing sinks. On the 10 highest observed O3 days during summer (O3_top10obs_JJA), US anthropogenic emissions enhance O3 by 5-11ppb and by less than 2ppb in the eastern versus western USA. The O3 enhancement from BVOC emissions during summer is 1-7 ppb higher on O3_top10obs_JJA days than on average days, while intercontinental pollution is up to 2ppb higher on average versus on O3_top10obs_JJA days. During the summers of 2004-2012, monthly regional mean US background O3 MDA8 levels vary by up to 15ppb from year to year. Observed and simulated summertime total surface O3 levels on O3_top10obs_JJA days decline by 3ppb (averaged over all regions) from 2004-2006 to 2010-2012, reflecting rising US background (+2ppb) and declining US anthropogenic O3 emissions (6ppb) in the model. The model attributes interannual variability in US background O3 on O3_top10obs days to natural sources, not international pollution transport. We find that a 3-year averaging period is not long enough to eliminate interannual variability in background O3 on the highest observed O3 days.

Guo, Jean J.↗

Perspectives on African Ozone from Sondes, Dobson and Aircraft Measurements

We have been studying variability in ozone over Africa using data from ozonesondes (vertical profiles from surface to stratosphere), aircraft (the MOZAIC dataset with cruise altitude and landing/takeoff profiles) and the ground (Dobson spectrophotometer total ozone column measurement). The following may give context for ozone investigations during AMMA: 1. Total ozone measurements since 1989 show considerable variability in mean value among the African stations in Algeria, Kenya, Egypt, South Africa, as well as in seasonal cycles and year-to-year. Trends are not evident. 2. The impacts of convection, stratospheric injection, biomass burning and lightning appear in ozone sounding profile data. Time-series analysis and case studies point to periodic influences of long-range interactions with the Atlantic ("ozone paradox," wave-one") and Indian Oceans. 3. Tropospheric ozone variations, observed in tropospheric profiles and integrated column amount, follow general seasonal patterns but short- term variability is so strong that simple averages are inadequate for describing "climatology" and statistical classification approaches may be required.

Thompson, A. M.↗

Literature review of some selected types of results and statistical analyses of total-ozone data

The depletion of ozone in the stratosphere is examined, and causes for the depletion are cited. Ground station and satellite measurements of ozone, which are taken on a worldwide basis, are discussed. Instruments used in ozone measurement are discussed, such as the Dobson spectrophotometer, which is credited with providing the longest and most extensive series of observations for ground based observation of stratospheric ozone. Other ground based instruments used to measure ozone are also discussed. The statistical differences of ground based measurements of ozone from these different instruments are compared to each other, and to satellite measurements. Mathematical methods (i.e., trend analysis or linear regression analysis) of analyzing the variability of ozone concentration with respect to time and lattitude are described. Various time series models which can be employed in accounting for ozone concentration variability are examined.

Myers, R. H.↗

Interannual Variability and Trends of Extratropical Ozone: Northern Hemisphere - Part 1

The authors apply principal component analysis (PCA) to the extratropical total column ozone from the combined merged ozone data product and the European Centre for Medium-Range Weather Forecasts assimilated ozone from January 1979 to August 2002. The interannual variability (IAV) of extratropical O-3 in the Northern Hemisphere (NH) is characterized by four main modes. Attributable to dominant dynamical effects, these four modes account for nearly 60% of the total ozone variance in the NH. The patterns of variability are distinctly different from those derived for total O-3 in the tropics. To relate the derived patterns of O-3 to atmospheric dynamics, similar decompositions are performed for the 30 100-Wa geopotential thickness. The results reveal intimate connections between the IAV of total ozone and the atmospheric circulation. The first two leading modes are nearly zonally symmetric and represent the connections to the annular modes and the quasi-biennial oscillation. The other two modes exhibit in-quadrature, wavenumber-1 structures that, when combined, describe the displacement of the polar vortices in response to planetary waves. In the NH, the extrema of these combined modes have preferred locations that suggest fixed topographical and land-sea thermal forcing of the involved planetary waves. Similar spatial patterns and trends in extratropical column ozone are simulated by the Goddard Earth Observation System chemistryclimate model (GEOS-CCM). The decreasing O-3 trend is captured in the first mode. The largest trend occurs at the North Pole, with values similar to-1 Dobson Unit (DU) yr(-1). There is almost no trend in tropical O-3. The trends derived from PCA are confirmed using a completely independent method, empirical mode decomposition, for zonally averaged O-3 data. The O-3 trend is also captured by mode 1 in the GEOS-CCM, but the decrease is substantially larger than that in the real atmosphere.

Yung, Yuk L.↗

Two-Dimensional Model Simulations of Interannual Variability in the Tropical Stratosphere

Meteorological data from the United Kingdom Meteorological Office (UKMO) and constituent data from the Upper Atmospheric Research Satellite (UARS) are used to construct yearly zonal mean dynamical fields for the 1990s for use in the GSFC 2-D chemistry and transport model. This allows for interannual dynamical variability to be included in the model constituent simulations. In this study, we focus on the tropical stratosphere. We find that the phase of quasi-biennial oscillation (QBO) signals in equatorial CH4, and profile and total column 03 data is resolved quite well using this empirically- based 2-D model transport framework. However. the QBO amplitudes in the model constituents are systematically underestimated relative to the observations at most levels. This deficiency is probably due in part to the limited vertical resolutions of the 2-D model and the UKMO and UARS input data sets. We find that using different heating rate calculations in the model affects the interannual and QBO amplitudes in the constituent fields, but has little impact on the phase. Sensitivity tests reveal that the QBO in transport dominates the ozone interannual variability in the lower stratosphere. with the effect of the temperature QBO being dominant in the tipper stratosphere via the strong temperature dependence of the ozone loss reaction rates. We also find that the QBO in odd nitrogen radicals, which is caused by the QBO modulated transport of NOy, plays a significant but not dominant role in determining the ozone QBO variability in the middle stratosphere. The model mean age of air is in good overall agreement with that determined from tropical lower,middle stratospheric OMS balloon observations of SF6 and CO2. The interannual variability of tile equatorial mean age in the model increases with altitude and maximizes near 40 km, with a range, of 4-5 years over the 1993-2000 time period.

Fleming, Eric L.↗

Seasonal Variability of Middle Latitude Ozone in the Lowermost Stratosphere Derived from Probability Distribution Functions

We present a study of the distribution of ozone in the lowermost stratosphere with the goal of understanding the relative contribution to the observations of air of either distinctly tropospheric or stratospheric origin. The air in the lowermost stratosphere is divided into two population groups based on Ertel's potential vorticity at 300 hPa. High [low] potential vorticity at 300 hPa suggests that the tropopause is low [high], and the identification of the two groups helps to account for dynamic variability. Conditional probability distribution functions are used to define the statistics of the mix from both observations and model simulations. Two data sources are chosen. First, several years of ozonesonde observations are used to exploit the high vertical resolution. Second, observations made by the Halogen Occultation Experiment [HALOE] on the Upper Atmosphere Research Satellite [UARS] are used to understand the impact on the results of the spatial limitations of the ozonesonde network. The conditional probability distribution functions are calculated at a series of potential temperature surfaces spanning the domain from the midlatitude tropopause to surfaces higher than the mean tropical tropopause [about 380K]. Despite the differences in spatial and temporal sampling, the probability distribution functions are similar for the two data sources. Comparisons with the model demonstrate that the model maintains a mix of air in the lowermost stratosphere similar to the observations. The model also simulates a realistic annual cycle. By using the model, possible mechanisms for the maintenance of mix of air in the lowermost stratosphere are revealed. The relevance of the results to the assessment of the environmental impact of aircraft effluence is discussed.

Cerniglia, M. C.↗