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At least 19 records

Change in Tropospheric Ozone in the Recent Decades and its Contribution to Global Total Ozone

Tropospheric ozone is a key chemically active trace gas and radiative forcer. Understanding its long-term changes is important to properly interpret observed changes in total column ozone and stratospheric ozone recovery. We investigate global and regional tropospheric ozone changes and their impact on total column ozone during 2005-2018 using satellite measurements and the NASA Goddard Earth Observing System Chemistry Climate Model (GEOSCCM). Global total ozone increased ~4 DU during 2005-2018 (+0.28±0.06 DU yr(exp -1)) as inferred from Ozone Monitoring Instrument (OMI). Consistent with previous studies, the OMI/MLS (Microwave Limb Sounder) derived global tropospheric ozone increased 2.2 DU during this period, 60% of the global total column ozone increase. While GEOSCCM reproduces reasonably well the total column increase, it overestimates the stratospheric ozone increase and underestimates the tropospheric ozone increase. We find that the tropospheric ozone increases are likely attributed to a growth of regional emissions of key ozone precursors, especially volatile organic compounds (VOCs) as reflected by the positive trends in formaldehyde (CH2O). Although carbon monoxide (CO) has been decreasing everywhere around the globe, it has relatively small impact on the tropospheric ozone trend. Trends in nitrogen dioxide (NO2) vary with regions, and these changes counteract or reinforce the positive effects of CH2O on the tropospheric ozone increases. The model underestimates the observed tropospheric ozone increase, especially over the US and Europe, because of underestimated NO2 emissions changes used in the model. The stratospheric ozone contribution increases during this period in the Northern Hemisphere and contributes to the tropospheric ozone increase.

Atmospheric chemistry↗

Tropospheric Ozone from the TOMS TDOT (TOMS-Direct-Ozone-in-Troposphere) Technique During SAFARI-2000

There are a number of published residual-type methods for deriving tropospheric ozone from TOMS (Total Ozone Mapping Spectrometer). The basic concept of these methods is that within a zone of constant stratospheric ozone, the tropospheric ozone column can be computed by subtracting stratospheric ozone from the TOMS Level 2 total ozone column, We used the modified-residual method for retrieving tropospheric ozone during SAFARI-2000 and found disagreements with in-situ ozone data over Africa in September 2000. Using the newly developed TDOT (TOMS-Direct-Ozone-in-Troposphere) method that uses TOMS radiances and a modified lookup table based on actual profiles during high ozone pollution periods, new maps were prepared and found to compare better to soundings over Lusaka, Zambia (15.5 S, 28 E), Nairobi and several African cities where MOZAIC aircraft operated in September 2000. The TDOT technique and comparisons are described in detail.

Stone, J. B.↗

Tropospheric Ozone Assessment Report: Tropospheric Ozone From 1877 to 2016, Observed Levels, Trends and Uncertainties

From the earliest observations of ozone in the lower atmosphere in the 19th century, both measurement methods and the portion of the globe observed have evolved and changed. These methods have different uncertainties and biases, and the data records differ with respect to coverage (space and time), information content, and representativeness. In this study, various ozone measurement methods and ozone datasets are reviewed and selected for inclusion in the historical record of background ozone levels, based on relationship of the measurement technique to the modern UV absorption standard, absence of interfering pollutants, representativeness of the well-mixed boundary layer and expert judgement of their credibility. There are significant uncertainties with the 19th and early 20th-century measurements related to interference of other gases. Spectroscopic methods applied before 1960 have likely underestimated ozone by as much as 11% at the surface and by about 24% in the free troposphere, due to the use of differing ozone absorption coefficients. There is no unambiguous evidence in the measurement record back to 1896 that typical mid-latitude background surface ozone values were below about 20 nmol mol–1, but there is robust evidence for increases in the temperate and polar regions of the northern hemisphere of 30–70%, with large uncertainty, between the period of historic observations, 1896–1975, and the modern period (1990–2014). Independent historical observations from balloons and aircraft indicate similar changes in the free troposphere. Changes in the southern hemisphere are much less. Regional representativeness of the available observations remains a potential source of large errors, which are difficult to quantify. The great majority of validation and intercomparison studies of free tropospheric ozone measurement methods use ECC ozonesondes as reference. Compared to UV-absorption measurements they show a modest (~1–5% ±5%) high bias in the troposphere, but no evidence of a change with time. Umkehr, lidar, and FTIR methods all show modest low biases relative to ECCs, and so, using ECC sondes as a transfer standard, all appear to agree to within one standard deviation with the modern UV-absorption standard. Other sonde types show an increase of 5–20% in sensitivity to tropospheric ozone from 1970–1995. Biases and standard deviations of satellite retrieval comparisons are often 2–3 times larger than those of other free tropospheric measurements. The lack of information on temporal changes of bias for satellite measurements of tropospheric ozone is an area of concern for long-term trend studies.

UV absorption standard↗

The 1998-2000 SHADOZ (Southern Hemisphere ADditional OZonesondes) Tropical Ozone Climatology: Stratospheric and Tropospheric Ozone Variability and the Zonal Wave-One - 2

This is the second 'reference' or 'archival' paper for the SHADOZ (Southern Hemisphere Additional Ozonesondes) network and is a follow-on to the recently accepted paper with similar first part of title. The latter paper compared SHADOZ total ozone with satellite and ground-based instruments and showed that the equatorial wave-one in total ozone is in the troposphere. The current paper presents details of the wave-one structure and the first overview of tropospheric ozone variability over the southern Atlantic, Pacific and Indian Ocean basins. The principal new result is that signals of climate effects, convection and offsets between biomass burning seasonality and tropospheric ozone maxima suggest that dynamical factors are perhaps more important than pollution in determining the tropical distribution of tropospheric ozone. The SHADOZ data at ( ) are setting records in website visits and are the first time that the zonal view of tropical ozone structure has been recorded - thanks to the distribution of the 10 sites that make up this validation network.

Thompson, Anne M.↗

Development of a Portable, Ground-based Ozone Lidar Instrument for Tropospheric Ozone Research and Educational Training

The objective of this research project is to develop a portable, eye-safe, ground-based ozone lidar instrument specialized for ozone differential absorption lidar (DIAL) measurements in the troposphere. This research project directly supports the goal of NASA's Earth Science Enterprise to understand the distribution and budget of tropospheric ozone (objective 1.5 of the Earth Science Strategic Enterprise Plan, 1998-2002). It can participate in ground validation experiments for TES, a tropospheric ozone satellite mission due to be launched in 2002. It can also be utilized for correlative ground measurements in future GTE (Global Tropospheric Experiment) and space-based ozone lidar missions, such as ORACLE. Multiple ground-based ozone lidar systems would improve the data obtained through current ozone-sonde networks. This prototype instrument could to serve as the basic unit for these and other future monitoring projects requiring multi-instrument networks, such as that proposed for the Global Tropospheric Ozone Project (GTOP). GTOP is currently being formulated by a scientific panel of the International Global Atmospheric Chemistry Project to meet its goal to better understand the processes that control the global distribution of tropospheric ozone. In order for the lidar to be widely deployed in networks, it must be fairly easy to use and maintain as well as being cost-competitive with a ground station launching ozonesondes several times a day. A second 2-year grant to continue this effort with students participating in ground tests and system improvements has been awarded by the Office of Equal Employment Opportunities (OEOP). This project also supports existing NASA lidar missions through its development of advanced, compact lidar technology. Innovations in both transmitters and receivers have been made in this project. Finally, this system could be modified in the future to probe more deeply into the stratosphere. This could be accomplished by increasing the emitted energy or optimizing the wavelengths for this purpose. In addition to NASA, this system has applications to the EPA, NOAA, and the DOD. An AFOSR grant has been awarded based on the results of this effort to fund advanced transmitter development at medium (20-40 mJ) energies. A second proposal to the DOD with a letter of support from Air Force Research Laboratory, has been submitted to extend this uv laser technology to 100 mJ levels. Thus, this project has enabled students and faculty at Hampton University to begin to develop research efforts in support of the mission of the DOD. This instrument will be based at Hampton University (HU) to meet our educational goal to train students in lidar technology as well as atmospheric ozone data analysis and interpretation. It will be also available for off-site measurement campaigns and will serve as a test bed for further instrument development. Later development beyond this grant to extend the scientific usefulness of the instrument may include incorporation of an aerosol channel and upgrading the laser to make stratospheric ozone measurements. Seven undergraduates, three graduate students, and one postdoctoral. researcher (formerly an HU student) have been active participants in this research effort.

Chyba, Thomas↗

Tropical Tropospheric Ozone (TTO) Maps from Nimbus 7 and Earth-Probe TOMS by the Modified-Residual Method: Validation, Evaluation and Trends based on Atlantic Regional Time Series - 1

The well-known wave-one pattern seen in tropical total ozone [Shiotani, 1992; Ziemke et al., 1996, 1998] has been used to develop a modified-residual (MR) method for retrieving time-averaged stratospheric ozone and tropospheric ozone column amount from TOMS (Total Ozone Mapping Spectrometer) over the 14 complete calendar years of Nimbus 7 observations (1979-1992) and from TOMS on the Earth-Probe (1996-present) and ADEOS platforms (1996- 1997). Nine- to sixteen-day averaged tropical tropospheric ozone (TTO) maps, validated with ozonesondes, show a seasonality expected from dynamical and chemical influences. The maps may be viewed on a homepage: http://metosrv2.umd.edu/~tropo. Stratospheric column ozone, which is also derived by the modified-residual method, compares well with sondes (to within 6-7 DU) and with stratospheric ozone column derived from other satellites (within 8-10 DU). Validation of the TTO time-series is presently limited to ozonesonde comparisons with Atlantic stations and sites on the adjacent continents (Ascension Island, Natal, Brazil; Brazzaville); for the sounding periods, TTO at all locations agrees with the sonde record to +/-7 DU. TTO time-series and the magnitude of the wave-one pattern show ENSO signals in the strongest El Nifio periods from 1979-1998. From 12degN and 12degS, zonally averaged tropospheric ozone shows no significant trend from 1980-1990. Trends are also not significant during this period in localized regions, e.g. from just west of South America across to southern Africa. This is consistent with the ozonesonde record at Natal, Brazil (the only tropical ozone data publicly available for the 1980's), which shows a not statistically significant increase. The lack of trend in tropospheric ozone agrees with a statistical analysis based on another method for deriving TTO from TOMS, the so-called Convective-Cloud-Differential approach of Ziemke et al. [1998].

Thompson, Anne M.↗

Development of a Portable, Ground-Based Ozone Lidar Instrument for Tropospheric Ozone Research and Educational Training

The objective of this project is to develop a portable, eye-safe, ground-based ozone lidar instrument specialized for ozone differential absorption lidar (DIAL) measurements in the troposphere. This prototype instrument is intended to operate at remote field sites and to serve as the basic unit for monitoring projects requiring multi-instrument networks, such as that discussed in the science plan for the Global Tropospheric Ozone Project (GTOP). This instrument will be based at HU for student training in lidar technology as well as atmospheric ozone data analysis and interpretation. It will be also available for off-site measurement campaigns and will serve as a test bed for further instrument development. Later development beyond this grant to extend the scientific usefulness of the instrument may include incorporation of an aerosol channel and upgrading the laser to make stratospheric ozone measurements. Undergraduate and graduate students have been and will be active participants in this research effort.

Chyba, Thomas↗

Trends in Global Tropospheric Ozone Inferred from a Composite Record of TOMS/OMI/MLS/OMPS Satellite Measurements and the MERRA-2 GMI Simulation

Past studies have suggested that ozone in the troposphere has increased globally throughout much of the 20th century due to increases in anthropogenic emissions and transport. We show, by combining satellite measurements with a chemical transport model, that during the last four decades tropospheric ozone does indeed indicate increases that are global in nature, yet still highly regional. Satellite ozone measurements from Nimbus-7 and Earth Probe Total Ozone Mapping Spectrometer (TOMS) are merged with ozone measurements from the Aura Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) to determine trends in tropospheric ozone for 1979–2016. Both TOMS (1979–2005) and OMI/MLS (2005–2016) depict large increases in tropospheric ozone from the Near East to India and East Asia and further eastward over the Pacific Ocean. The 38-year merged satellite record shows total net change over this region of about +6 to +7 Dobson units (DU) (i.e., ∼15 %–20 % of average background ozone), with the largest increase (∼4 DU) occurring during the 2005–2016 Aura period. The Global Modeling Initiative (GMI) chemical transport model with time-varying emissions is used to aid in the interpretation of tropospheric ozone trends for 1980–2016. The GMI simulation for the combined record also depicts the greatest increases of +6 to +7 DU over India and East Asia, very similar to the satellite measurements. In regions of significant increases in tropospheric column ozone (TCO) the trends are a factor of 2–2.5 larger for the Aura record when compared to the earlier TOMS record; for India and East Asia the trends in TCO for both GMI and satellite measurements are ∼+3 DU decade(exp −1) or greater during 2005–2016 compared to about +1.2 to +1.4 DU decade(exp −1) for 1979–2005. The GMI simulation and satellite data also reveal a tropospheric ozone increases in ∼+4 to +5 DU for the 38-year record over central Africa and the tropical Atlantic Ocean. Both the GMI simulation and satellite-measured tropospheric ozone during the latter Aura time period show increases of ∼+3 DU decade−1 over the N Atlantic and NE Pacific.

Ziemke, Jerald R.↗

The photochemistry of synoptic-scale ozone synthesis Implications for the global tropospheric ozone budget

The oxidation of nonmethane hydrocarbons represents a source of tropospheric ozone that is primarily confined to the boundary layers of several highly industrialized regions. (Each region has an area greater than one million km/sq cm). Using a photochemical model, the global tropospheric ozone budget is reexamined by including the in-situ production from these localized regimes. The results from these calculations suggest that the net source due to this photochemistry, which takes place on the synoptic scale, is approximately as large as the amount calculated for global scale photochemical processes which consider only the oxidation of methane and carbon monoxide. Such a finding may have a considerable impact on our understanding of the tropospheric ozone budget. The model results for ozone show reasonable agreement with the climatological summer distribution of ozone and the oxides of nitrogen at the surface and with the vertical distribution of ozone and nonmethane hydrocarbons obtained during a 1980 field program.

Fishman, J.↗

Ozone Profiles and Tropospheric Ozone from Global Ozone Monitoring Experiment

Ozone profiles are derived from backscattered radiances in the ultraviolet spectra (290-340 nm) measured by the nadir-viewing Global Ozone Monitoring Experiment using optimal estimation. Tropospheric O3 is directly retrieved with the tropopause as one of the retrieval levels. To optimize the retrieval and improve the fitting precision needed for tropospheric O3, we perform extensive wavelength and radiometric calibrations and improve forward model inputs. Retrieved O3 profiles and tropospheric O3 agree well with coincident ozonesonde measurements, and the integrated total O3 agrees very well with Earth Probe TOMS and Dobson/Brewer total O3. The global distribution of tropospheric O3 clearly shows the influences of biomass burning, convection, and air pollution, and is generally consistent with our current understanding.

Liu, X.↗

Tropical Tropospheric Ozone From Nimbus 7 and Earth-Probe Toms: Validation, ENSO Signals and Trends

The well-known wave-one pattern seen in tropical total ozone has been used to develop a modified-residual (MR) method for retrieving time-averaged stratospheric ozone and tropospheric ozone column amount from TOMS (Total Ozone Mapping Spectrometer) over the 14 complete years of Nimbus 7 observations (1979-1992) and from Earth-Probe (1996-present) and ADEOS/TOMS (1996-1997). Nine- to sixteen-day averaged tropical tropospheric ozone (TTO) maps show a seasonality expected from dynamical and chemical influences. Validation of the TTO time-series is presently limited to Atlantic sounding stations, notably Ascension Island, Natal, Brazil, and Brazzaville, Congo. Stratospheric column ozone, which is also derived from the modified-residual method, compares well with sondes and with stratospheric ozone column derived from other satellites.

Thompson, Anne M.↗

Science Accomplishments from a Decade of Aura OMI/MLS Tropospheric Ozone Measurements

Measurements of tropospheric ozone from combined Aura OMI and MLS instruments have yielded a large number of new and important science discoveries over the last decade. These discoveries have generated a much greater understanding of biomass burning, lightning NO, and stratosphere-troposphere exchange sources of tropospheric ozone, ENSO dynamics and photochemistry, intra-seasonal variability-Madden-Julian Oscillation including convective transport, radiative forcing, measuring ozone pollution from space, improvements to ozone retrieval algorithms, and evaluation of chemical-transport and chemistry-climate models. The OMI-MLS measurements have been instrumental in giving us better understanding of the dynamics and chemistry involving tropospheric ozone and the many drivers affecting the troposphere in general. This discussion will provide an overview focusing on our main science results.

ENSO↗

Correlative nature of ozone and carbon monoxide in the troposphere - Implications for the tropospheric ozone budget

The small-scale vertical variability of troposheric O3 and CO is examined using a set of simultaneous measurements obtained in July and August 1974 between 55 deg S and 67 deg N. From this set of vertical profiles, it is found that many of the fluctuations are coincident in both species, and a method is presented that quantifies the correlation between the observed O3 and CO variability. A two-dimensional depiction of the distribution of these O3-CO correlations reveals that there are regions in the troposphere where these trace gases are positively correlated and that, at the same time, there are preferred locations where these two species are primarily anticorrelated. The regions of anticorrelation are found to be consistent with the traditional picture of the tropospheric ozone cycle, suggesting that this gas is chemically unreactive in the troposphere. On the other hand, the location and magnitude of the region in which these two species are positively correlated indicates that there is considerable in situ production of tropospheric ozone.

Fishman, J.↗

Observing Tropospheric Ozone From Space

The importance of tropospheric ozone embraces a spectrum of relevant scientific issues ranging from local environmental concerns, such as damage to the biosphere and human health, to those that impact global change questions, Such is climate warming. From an observational perspective, the challenge is to determine the tropospheric ozone global distribution. Because its lifetime is short compared with other important greenhouse gases that have been monitored over the past several decades, the distribution of tropospheric ozone cannot be inferred from a relatively small set of monitoring stations. Therefore, the best way to obtain a true global picture is from the use of space-based instrumentation where important spatial gradients over vast ocean expanses and other uninhabited areas can be properly characterized. In this paper, the development of the capability to measure tropospheric ozone from space over the past 15 years is summarized. Research in the late 1980s successfully led to the determination of the climatology of tropospheric ozone as a function of season; more recently, the methodology has improved to the extent where regional air pollution episodes can be characterized. The most recent modifications now provide quasi-global (50 N) to 50 S) maps on a daily basis. Such a data set would allow for the study of long-range (intercontinental) transport of air pollution and the quantification of how regional emissions feed into the global tropospheric ozone budget. Future measurement capabilities within this decade promise to offer the ability to provide Concurrent maps of the precursors to the in situ formation of tropospheric ozone from which the scientific community will gain unprecedented insight into the processes that control global tropospheric chemistry

Fishman, Jack↗

A Madden-Julian Oscillation in Tropospheric Ozone

This is the first study to indicate a Madden-Julian Oscillation (MJO) in tropospheric ozone. Tropospheric ozone is derived using differential measurements of total column ozone and stratospheric column ozone measured from total ozone mapping spectrometer (TOMS) and microwave limb sounder (MLS) instruments. Two broad regions of significant MJO signal are identified in the tropics, one in the western Pacific and the other in the eastern Pacific. Over both regions, MJO variations in tropospheric ozone represent 5-10 Dobson Unit (DU) peak-to-peak anomalies. These variations are significant compared to mean background amounts of 20 DU or less over most of the tropical Pacific. MJO signals of this magnitude would need to be considered when investigating and interpreting particular pollution events since ozone is a precursor of the hydroxyl (OH) radical, the main oxidizing agent of pollutants in the lower atmosphere.

Ziemke, J. R.↗

A Madden-Julian Oscillation in Tropospheric Ozone

This is the first study to indicate a Madden-Julian Oscillation (MJO) in tropospheric ozone. Tropospheric ozone is derived using differential measurements of total column ozone and stratospheric column ozone measured from total ozone mapping spectrometer (TOMS) and microwave limb sounder (MLS) instruments. Two broad regions of significant MJO signal are identified in the tropics, one in the western Pacific and the other in the eastern Pacific. Over both regions, MJO variations in tropospheric ozone represent 5- 10 DU peak-to-peak anomalies. These variations are significant compared to mean background amounts of 20 DU or less over most of the tropical Pacific. The implications of these results are: (1) model values of TCO in the tropical Pacific region, when accounted for the MJO may be highly variable depending upon the phase of the MJO, and (2) MJO signals of this magnitude would need to be considered when investigating and interpreting particular pollution events since ozone is a precursor of the hydroxyl (OH) radical, the main oxidizing agent of pollutants in the lower atmosphere.

Ziemke, J. R.↗

Estimating the Tropospheric Ozone Distribution by the Assimilation of Satellite Data

Tropospheric ozone is important to the environment, because it acts as a strong oxidant to control the concentrations of many reduced gases (methane, carbon monoxide, ... ), its radiative forcing plays a significant role in the greenhouse effect, and direct contact with ozone is harmful to human health. Tropospheric ozone, whose main sources are intrusion from the stratosphere and chemical production from source gases associated with urban pollution or biomass burning, varies on a wide range of spatial and temporal scales. Its transport and chemistry can be influenced by weather, seasonal, or multiannual variability. Despite the importance of tropospheric ozone, it contributes only about 10% of the total ozone loading in the atmosphere. Consequently, satellite instruments lose sensitivity below the stratospheric ozone peak, and provide little information about middle and lower tropospheric ozone. This talk will discuss recent modifications made to the satellite ozone data assimilation system at NASA's Data Assimilation Office (DAO) in order to provide better tropospheric ozone columns and profiles. We use a version of the system that assimilates only the data from the Solar Backscatter UltraViolet/2 (SBUV/2) instrument. The quality of the assimilated ozone in the tropical troposphere is evaluated by comparison with independent observations obtained from the Southern Hemispheric Additional Ozonesondes (SHADOZ) network. It is shown that the quality of ozone fields is sensitive to the winds used in the transport model. Increasing the vertical resolution of the model also has a beneficial impact. The assimilated ozone in the lower troposphere was substantially improved by inclusion of tropospheric ozone production, loss, and dry deposition rates from the Harvard GEOS-CHEM model. The mechanisms behind these results will be examined and the implications for our understanding of tropospheric ozone will be discussed.

Hayashi, Hiroo↗