scholarly journals Tropospheric Ozone Assessment Report: Database and Metrics Data of Global Surface Ozone Observations

Elem Sci Anth ◽  
2017 ◽  
Vol 5 (0) ◽  
pp. 58 ◽  
Author(s):  
Martin G. Schultz ◽  
Sabine Schröder ◽  
Olga Lyapina ◽  
Owen Cooper ◽  
Ian Galbally ◽  
...  
Elem Sci Anth ◽  
2018 ◽  
Vol 6 ◽  
Author(s):  
A. Gaudel ◽  
O. R. Cooper ◽  
G. Ancellet ◽  
B. Barret ◽  
A. Boynard ◽  
...  

The Tropospheric Ozone Assessment Report (TOAR) is an activity of the International Global Atmospheric Chemistry Project. This paper is a component of the report, focusing on the present-day distribution and trends of tropospheric ozone relevant to climate and global atmospheric chemistry model evaluation. Utilizing the TOAR surface ozone database, several figures present the global distribution and trends of daytime average ozone at 2702 non-urban monitoring sites, highlighting the regions and seasons of the world with the greatest ozone levels. Similarly, ozonesonde and commercial aircraft observations reveal ozone’s distribution throughout the depth of the free troposphere. Long-term surface observations are limited in their global spatial coverage, but data from remote locations indicate that ozone in the 21st century is greater than during the 1970s and 1980s. While some remote sites and many sites in the heavily polluted regions of East Asia show ozone increases since 2000, many others show decreases and there is no clear global pattern for surface ozone changes since 2000. Two new satellite products provide detailed views of ozone in the lower troposphere across East Asia and Europe, revealing the full spatial extent of the spring and summer ozone enhancements across eastern China that cannot be assessed from limited surface observations. Sufficient data are now available (ozonesondes, satellite, aircraft) across the tropics from South America eastwards to the western Pacific Ocean, to indicate a likely tropospheric column ozone increase since the 1990s. The 2014–2016 mean tropospheric ozone burden (TOB) between 60°N–60°S from five satellite products is 300 Tg ± 4%. While this agreement is excellent, the products differ in their quantification of TOB trends and further work is required to reconcile the differences. Satellites can now estimate ozone’s global long-wave radiative effect, but evaluation is difficult due to limited in situ observations where the radiative effect is greatest.


2017 ◽  
Author(s):  
Ben Newsome ◽  
Mat Evans

Abstract. Chemical rate constants determine the composition of the atmosphere and how this composition has changed over time. They are central to our understanding of climate change and air quality degradation. Atmospheric chemistry models, whether online or offline, box, regional or global use these rate constants. Expert panels synthesise laboratory measurements, making recommendations for the rate constants that should be used. This results in very similar or identical rate constants being used by all models. The inherent uncertainties in these recommendations are, in general, therefore ignored. We explore the impact of these uncertainties on the composition of the troposphere using the GEOS-Chem chemistry transport model. Based on the JPL and IUPAC evaluations we assess 50 mainly inorganic rate constants and 10 photolysis rates, through simulations where we increase the rate of the reactions to the 1σ upper value recommended by the expert panels. We assess the impact on 4 standard metrics: annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime. Uncertainty in the rate constants for NO2 + OH    M →  HNO3, OH + CH4 → CH3O2 + H2O and O3 + NO → NO2 + O2 are the three largest source of uncertainty in these metrics. We investigate two methods of assessing these uncertainties, addition in quadrature and a Monte Carlo approach, and conclude they give similar outcomes. Combining the uncertainties across the 60 reactions, gives overall uncertainties on the annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime of 11, 12, 17 and 17 % respectively. These are larger than the spread between models in recent model inter-comparisons. Remote regions such as the tropics, poles, and upper troposphere are most uncertain. This chemical uncertainty is sufficiently large to suggest that rate constant uncertainty should be considered when model results disagree with measurement. Calculations for the pre-industrial allow a tropospheric ozone radiative forcing to be calculated of 0.412 ± 0.062 Wm−2. This uncertainty (15 %) is comparable to the inter-model spread in ozone radiative forcing found in previous model-model inter-comparison studies where the rate constants used in the models are all identical or very similar. Thus the uncertainty of tropospheric ozone radiative forcing should expanded to include this additional source of uncertainty. These rate constant uncertainties are significant and suggest that refinement of supposedly well known chemical rate constants should be considered alongside other improvements to enhance our understanding of atmospheric processes.


Elem Sci Anth ◽  
2019 ◽  
Vol 7 ◽  
Author(s):  
David Tarasick ◽  
Ian E. Galbally ◽  
Owen R. Cooper ◽  
Martin G. Schultz ◽  
Gerard Ancellet ◽  
...  

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.


Elem Sci Anth ◽  
2018 ◽  
Vol 6 ◽  
Author(s):  
Zoë L. Fleming ◽  
Ruth M. Doherty ◽  
Erika von Schneidemesser ◽  
Christopher S. Malley ◽  
Owen R. Cooper ◽  
...  

This study quantifies the present-day global and regional distributions (2010–2014) and trends (2000–2014) for five ozone metrics relevant for short-term and long-term human exposure. These metrics, calculated by the Tropospheric Ozone Assessment Report, are: 4th highest daily maximum 8-hour ozone (4MDA8); number of days with MDA8 > 70 ppb (NDGT70), SOMO35 (annual Sum of Ozone Means Over 35 ppb) and two seasonally averaged metrics (3MMDA1; AVGMDA8). These metrics were explored at ozone monitoring sites worldwide, which were classified as urban or non-urban based on population and nighttime lights data. Present-day distributions of 4MDA8 and NDGT70, determined predominantly by peak values, are similar with highest levels in western North America, southern Europe and East Asia. For the other three metrics, distributions are similar with North–South gradients more prominent across Europe and Japan. Between 2000 and 2014, significant negative trends in 4MDA8 and NDGT70 occur at most US and some European sites. In contrast, significant positive trends are found at many sites in South Korea and Hong Kong, with mixed trends across Japan. The other three metrics have similar, negative trends for many non-urban North American and some European and Japanese sites, and positive trends across much of East Asia. Globally, metrics at many sites exhibit non-significant trends. At 59% of all sites there is a common direction and significance in the trend across all five metrics, whilst 4MDA8 and NDGT70 have a common trend at ~80% of all sites. Sensitivity analysis shows AVGMDA8 trends differ with averaging period (warm season or annual). Trends are unchanged at many sites when a 1995–2014 period is used; although fewer sites exhibit non-significant trends. Over the longer period 1970–2014, most Japanese sites exhibit positive 4MDA8/SOMO35 trends. Insufficient data exist to characterize ozone trends for the rest of Asia and other world regions.


Author(s):  
Jack G. Calvert ◽  
John J. Orlando ◽  
William R. Stockwell ◽  
Timothy J. Wallington

Reactive (or “odd”) nitrogen is emitted into the atmosphere in a variety of forms, with the most important being NOx (NO and NO2), ammonia (NH3), and nitrous oxide (N2O). Emissions of these species into the atmosphere have been summarized, for example, by the IPCC Fourth Assessment Report (the AR4; IPCC, 2007). Some discussion of NOx emissions and trends has also been presented in Chapter I. Emissions of NOx are mainly the result of anthropogenic activity associated with fossil fuel combustion and industrial activity. For the 1990s, the AR4 estimates total anthropogenic NOx emissions of 33.4 TgN yr−1, with natural emissions (mostly from soil and lightning) accounting for an additional 8.4–13.7 TgN yr−1. Ammonia emissions are comparable in magnitude to those for NOx, with anthropogenic emissions (45.5 TgN yr−1) again exceeding natural emissions (10.6 TgN yr−1). Although the majority of the ammonia produces aerosols or is scavenged by aerosol and is subsequently lost from the atmosphere, some gas phase oxidation does occur, which can in part lead to NOx production. The N2O source strength is about 17.7 TgN yr−1, with natural sources outweighing anthropogenic ones (IPCC, 2007). However, N2O is essentially inert in the troposphere, and thus the vast majority of its photooxidation and concomitant NOx release occurs in the stratosphere. The major NOx − related reactions occurring in the Earth’s troposphere are summarized in Figure III-A-1. As just alluded to, the species NO and NO2 are jointly referred to as NOx and are often treated collectively. This is because, under daytime conditions, these two species are rapidly interconverted, with the interconversion occurring on a much shorter timescale than the loss of either species.


2016 ◽  
Vol 16 (21) ◽  
pp. 14025-14039 ◽  
Author(s):  
Dimitris Akritidis ◽  
Andrea Pozzer ◽  
Prodromos Zanis ◽  
Evangelos Tyrlis ◽  
Bojan Škerlak ◽  
...  

Abstract. We study the contribution of tropopause folds in the summertime pool of tropospheric ozone over the eastern Mediterranean and the Middle East (EMME) with the aid of the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model. Tropopause fold events in EMAC simulations were identified with a 3-D labeling algorithm that detects folds at grid points where multiple crossings of the dynamical tropopause are computed. Subsequently the events featuring the largest horizontal and vertical extent were selected for further study. For the selection of these events we identified a significant contribution of the stratospheric ozone reservoir to the high concentrations of ozone in the middle and lower free troposphere over the EMME. A distinct increase of ozone is found over the EMME in the middle troposphere during summer as a result of the fold activity, shifting towards the southeast and decreasing altitude. We find that the interannual variability of near-surface ozone over the eastern Mediterranean (EM) during summer is related to that of both tropopause folds and ozone in the free troposphere.


2018 ◽  
Vol 11 (7) ◽  
pp. 2825-2840 ◽  
Author(s):  
Tim Butler ◽  
Aurelia Lupascu ◽  
Jane Coates ◽  
Shuai Zhu

Abstract. A system for source attribution of tropospheric ozone produced from both NOx and volatile organic compound (VOC) precursors is described, along with its implementation in the Community Earth System Model (CESM) version 1.2.2 using CAM4. The user can specify an arbitrary number of tag identities for each NOx or VOC species in the model, and the tagging system rewrites the model chemical mechanism and source code to incorporate tagged tracers and reactions representing these tagged species, as well as ozone produced in the stratosphere. If the user supplies emission files for the corresponding tagged tracers, the model will produce tagged ozone tracers which represent the contribution of each of the tag identities to the modelled total tropospheric ozone. Our tagged tracers preserve Ox. The size of the tagged chemical mechanism scales linearly with the number of specified tag identities. Separate simulations are required for NOx and VOC tagging, which avoids the sharing of tag identities between NOx and VOC species. Results are presented and evaluated for both NOx and VOC source attribution. We show that northern hemispheric surface ozone is dominated year-round by anthropogenic emissions of NOx, but that the mix of corresponding VOC precursors changes over the course of the year; anthropogenic VOC emissions contribute significantly to surface ozone in winter–spring, while biogenic VOCs are more important in summer. The system described here can provide important diagnostic information about modelled ozone production, and could be used to construct source–receptor relationships for tropospheric ozone.


2018 ◽  
Author(s):  
Kai-Lan Chang ◽  
Owen R. Cooper ◽  
J. Jason West ◽  
Marc L. Serre ◽  
Martin G. Schultz ◽  
...  

Abstract. We have developed a new statistical approach (M3Fusion) for combining surface ozone observations from thousands of monitoring sites around the world with the output from multiple atmospheric chemistry models to produce a global surface ozone distribution with greater accuracy than can be provided by any individual model. The ozone observations from 4766 monitoring sites were provided by the Tropospheric Ozone Assessment Report (TOAR) surface ozone database which contains the world's largest collection of surface ozone metrics. Output from six models was provided by the participants of the Chemistry-Climate Model Initiative (CCMI) and NASA's Global Modeling and Assimilation Office (GMAO). We analyze the 6-month maximum of the maximum daily 8-hour average ozone value (DMA8) for relevance to ozone health impacts. We interpolate the irregularly-spaced observations onto a fine resolution grid by using integrated nested Laplace approximations, and compare the ozone field to each model in each world region. This method allows us to produce a global surface ozone field based on TOAR observations, which we then use to select the combination of global models with the greatest skill in each of 8 world regions; models with greater skill in a particular region are given higher weight. This blended model product is bias-corrected within two degrees of observation locations to produce the final fused surface ozone product. We show that our fused product has an improved mean squared error compared to the simple multi-model ensemble mean.


2020 ◽  
Author(s):  
Tamara Emmerichs ◽  
Huug Ouwersloot ◽  
Astrid Kerkweg ◽  
Silvano Fares ◽  
Ivan Mammarella ◽  
...  

<p>Surface ozone is a harmful air pollutant, heavily influenced by chemical production and loss processes. Dry deposition to vegetation is a relevant loss process responsible for 20 % of the total tropospheric ozone loss. Its parametrization in atmospheric chemistry models represents a major source of uncertainty for the global tropospheric ozone budget and might account for the mismatch with observations. The model used in this study, the Modular Earth Submodel System (MESSy2) linked to ECHAM5 as atmospheric circulation model (EMAC) is no exception. Like many global models, EMAC employs a “resistances in series” scheme with the major surface deposition via plant stomata which is hardly sensitive to meteorology depending only on solar radiation. Unlike many global models, however, EMAC uses a simplified high resistance for non-stomatal deposition which makes this pathway negligible.                             </p><p>Hence, a revision of the dry deposition scheme of EMAC is desirable. The scheme has been extended with empirical adjustment factors to predict stomatal responses to temperature and vapour pressure deficit. Furthermore, an explicit formulation of humidity depending non-stomatal deposition at the leaf surface (cuticle) has been implemented based on established schemes. Next, the soil moisture availability function for plants has been critically reviewed and modified in order to avoid a stomatal closure where the model shows a strong soil dry bias, e.g. Amazon basin in dry season.</p><p>The last part of the presentation will show comparisons of dry deposition velocities and fluxes comparing simulations with data obtained from four experimental sites where ozone deposition is measured with micrometeorological techniques. The impacts of the changes on daily and seasonal patterns of ozone dry deposition will be discussed with a highlight on surface ozone, global distribution and budget.</p>


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