Tropospheric Ozone Trends Research Articles

The role of natural factors in constraining long-term tropospheric ozone trends over Southern China

Southern China has experienced severe photochemical pollution events in recent years, and the tropospheric ozone has emerged as the major pollutant of concern. Despite some recent efforts, the role of natural factors in constraining long-term trends of ozone in this region is poorly understood. In this study, we addressed this issue using tropospheric column ozone (TCO) datasets (2005–2017) from the Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) and surface ozone datasets from 16 monitoring stations in Southern China (2006–2016). Consequently, we studied the influence of atmospheric dynamical factors, such as solar cycle, El-Nino Southern Oscillation (ENSO), Quasi-Biennial Oscillation (QBO), and Arctic Oscillation (AO), and local-scale meteorological factors, such as precipitation, surface temperature, planetary boundary layer height, and horizontal winds, on regional ozone trends. Stepwise multivariate regression analysis and harmonic function fitting were adopted to quantitatively simulate the influence of these natural drivers on ozone change. We found that within our research periods, both surface ozone and TCO in Southern China had a significant upward trend, with slopes of 0.97% y−1 (0.23 ppbv y−1) and 0.82% y−1 (0.28 DU y−1), respectively. Natural factors explained 44.4% of the TCO uptrend and 27.0% of the surface ozone uptrend. Among the natural factors, the solar cycle plays the most important role in tropospheric and surface ozone modulation. Its 11-year cycle had a large impact on TCO for 2–7 DU and on surface ozone for 3–8 ppbv. However, the ENSO, QBO, and AO indices did not affect tropospheric ozone trends significantly. In addition, we showed that precipitation and wind fields associated with the Asian summer monsoon played a critical role in lowering ozone levels over Southern China, accounting for 24.8% and 81.5% of summertime TCO and surface ozone variability, respectively. Finally, a significant fraction of TCO and surface ozone uptrends (55.6% and 73.0%, respectively) remained unexplained even after consideration of these natural factors in the periods 2005–2017 and 2006–2016, respectively. These unexplained factors are most likely related to anthropogenic emissions and should be studied further.

Trends in global tropospheric ozone inferred from a composite record of TOMS/OMI/MLS/OMPS satellite measurements and the MERRA-2 GMI simulation

Abstract. 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−1 or greater during 2005–2016 compared to about +1.2 to +1.4 DU decade−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.

Surface and tropospheric ozone trends in the Southern Hemisphere since 1990: possible linkages to poleward expansion of the Hadley circulation

Increases in free tropospheric ozone over the past two decades are mainly in the Northern Hemisphere that have been widely documented, while ozone trends in the Southern Hemisphere (SH) remain largely unexplained. Here we first show that in-situ and satellite observations document increases of tropospheric ozone in the SH over 1990–2015. We then use a global chemical transport model to diagnose drivers of these trends. We find that increases of anthropogenic emissions (including methane) are not the most significant contributors. Instead, we explain the trend as due to changes in meteorology, and particularly in transport patterns. We propose a possible linkage of the ozone increases to meridional transport pattern shifts driven by poleward expansion of the SH Hadley circulation (SHHC). The SHHC poleward expansion allows more downward transport of ozone from the stratosphere to the troposphere at higher latitudes, and also enhances tropospheric ozone production through stronger lifting of tropical ozone precursors to the upper troposphere. These together may lead to increasing tropospheric ozone in the extratropical SH, particularly in the middle/upper troposphere and in austral autumn. Poleward expansion of the Hadley circulation is partly driven by greenhouse warming, and the associated increase in tropospheric ozone potentially provides a positive climate feedback amplifying the warming that merits further quantification.

Harmonisation and trends of 20-year tropical tropospheric ozone data

Abstract. Using a convective-cloud differential (CCD) method, developed in-house and applied to retrievals of total ozone and cloud data from three European satellite instruments (viz. GOME/ERS-2, 1995–2003; SCIAMACHY/Envisat, 2002–2012 and GOME-2/MetOp-A, 2007–2015), monthly mean tropical tropospheric columns of ozone (TTCO) have been retrieved, which are in good agreement with ozonesondes (biases less than 6 DU). As small differences in TTCO between the individual instruments were evident, it was necessary to develop a scheme to harmonise the three datasets into one consistent time series starting from 1996 until 2015. Correction offsets (biases) between the instruments using SCIAMACHY as intermediate reference have been calculated and six different harmonisation or merging scenarios have been evaluated. Depending on the merging approach, the magnitude, pattern and uncertainty in the trends strongly vary. The harmonisation or merging represents an additional source of uncertainty in the trends (2 DU decade−1 on average, in most of the cases exceeding the uncertainty from the regression). For studying further details on tropospheric ozone trends on various spatial scales in the tropics, we stick with one preferred merged dataset that shows best agreement with ozonesondes. In this merged dataset, no correction was applied for GOME, and mean biases with respect to SCIAMACHY in the overlapping period (2007–2012) were calculated and applied for GOME-2 in each grid box (2.5° × 5°). In contrast with other studies we found that the tropospheric trend averaged over the tropics (−15° S to 15° N) is not statistically significant. The mean tropospheric ozone trend equals −0.2 ± 0.6 DU decade−1 (2σ). Regionally, tropospheric ozone has a statistically significant increase of ∼ 3 DU decade−1 over southern Africa ( ∼ 1.5 % yr−1), the southern tropical Atlantic ( ∼ 1.5 % yr−1), southeastern tropical Pacific Ocean ( ∼ 1 % yr−1), and central Oceania ( ∼ 2 % yr−1) and by ∼ 2 DU decade−1 over central Africa (2–2.5 % yr−1) and south India ( ∼ 1.5 % yr−1). On the other hand, tropospheric O3 decreases by ∼ 3 DU decade−1 over the Caribbean Sea and parts of the North Pacific Ocean ( ∼ 2 % yr−1), and by less than 2 DU decade−1 over some regions of the southern Pacific and Indian oceans ( ∼ 0.5–1 % yr−1).

Long-term trends of surface ozone and its influencing factors at the Mt Waliguan GAW station, China – Part 2: The roles of anthropogenic emissions and climate variability

Abstract. Inter-annual variability and long-term trends in tropospheric ozone are both environmental and climate concerns. Ozone measured at Mt Waliguan Observatory (WLG, 3816 m a.s.l.) on the Tibetan Plateau over the period of 1994–2013 has increased significantly by 0.2–0.3 ppbv yr−1 during spring and autumn but shows a much smaller trend in winter and no significant trend in summer. Here we explore the factors driving the observed ozone changes at WLG using backward trajectory analysis, chemistry–climate model hindcast simulations (GFDL AM3), a trajectory-mapped ozonesonde data set, and several climate indices. A stratospheric ozone tracer implemented in GFDL AM3 indicates that stratosphere-to-troposphere transport (STT) can explain ∼ 60 % of the simulated springtime ozone increase at WLG, consistent with an increase in the NW air-mass frequency inferred from the trajectory analysis. Enhanced STT associated with the strengthening of the mid-latitude jet stream contributes to the observed high ozone anomalies at WLG during the springs of 1999 and 2012. During autumn, observations at WLG are more heavily influenced by polluted air masses originating from South East Asia than in the other seasons. Rising Asian anthropogenic emissions of ozone precursors are the key driver of increasing autumnal ozone observed at WLG, as supported by the GFDL AM3 model with time-varying emissions, which captures the observed ozone increase (0.26 ± 0.11 ppbv yr−1). AM3 simulates a greater ozone increase of 0.38 ± 0.11 ppbv yr−1 at WLG in autumn under conditions with strong transport from South East Asia and shows no significant ozone trend in autumn when anthropogenic emissions are held constant in time. During summer, WLG is mostly influenced by easterly air masses, but these trajectories do not extend to the polluted regions of eastern China and have decreased significantly over the last 2 decades, which likely explains why summertime ozone measured at WLG shows no significant trend despite ozone increases in eastern China. Analysis of the Trajectory-mapped Ozonesonde data set for the Stratosphere and Troposphere (TOST) and trajectory residence time reveals increases in direct ozone transport from the eastern sector during autumn, which adds to the autumnal ozone increase. We further examine the links of ozone variability at WLG to the quasi-biennial oscillation (QBO), the East Asian summer monsoon (EASM), and the sunspot cycle. Our results suggest that the 2–3-, 3–7-, and 11-year periodicities are linked to the QBO, EASM index, and sunspot cycle, respectively. A multivariate regression analysis is performed to quantify the relative contributions of various factors to surface ozone concentrations at WLG. Through an observational and modelling analysis, this study demonstrates the complex relationships between surface ozone at remote locations and its dynamical and chemical influencing factors.

Tropospheric Ozone Assessment Report: Assessment of global-scale model performance for global and regional ozone distributions, variability, and trends

The goal of the Tropospheric Ozone Assessment Report (TOAR) is to provide the research community with an up-to-date scientific assessment of tropospheric ozone, from the surface to the tropopause. While a suite of observations provides significant information on the spatial and temporal distribution of tropospheric ozone, observational gaps make it necessary to use global atmospheric chemistry models to synthesize our understanding of the processes and variables that control tropospheric ozone abundance and its variability. Models facilitate the interpretation of the observations and allow us to make projections of future tropospheric ozone and trace gas distributions for different anthropogenic or natural perturbations. This paper assesses the skill of current-generation global atmospheric chemistry models in simulating the observed present-day tropospheric ozone distribution, variability, and trends. Drawing upon the results of recent international multi-model intercomparisons and using a range of model evaluation techniques, we demonstrate that global chemistry models are broadly skillful in capturing the spatio-temporal variations of tropospheric ozone over the seasonal cycle, for extreme pollution episodes, and changes over interannual to decadal periods. However, models are consistently biased high in the northern hemisphere and biased low in the southern hemisphere, throughout the depth of the troposphere, and are unable to replicate particular metrics that define the longer term trends in tropospheric ozone as derived from some background sites. When the models compare unfavorably against observations, we discuss the potential causes of model biases and propose directions for future developments, including improved evaluations that may be able to better diagnose the root cause of the model-observation disparity. Overall, model results should be approached critically, including determining whether the model performance is acceptable for the problem being addressed, whether biases can be tolerated or corrected, whether the model is appropriately constituted, and whether there is a way to satisfactorily quantify the uncertainty.

Tropospheric Ozone Assessment Report: Present-day tropospheric ozone distribution and trends relevant to vegetation

This Tropospheric Ozone Assessment Report (TOAR) on the current state of knowledge of ozone metrics of relevance to vegetation (TOAR-Vegetation) reports on present-day global distribution of ozone at over 3300 vegetated sites and the long-term trends at nearly 1200 sites. TOAR-Vegetation focusses on three metrics over vegetation-relevant time-periods across major world climatic zones: M12, the mean ozone during 08:00–19:59; AOT40, the accumulation of hourly mean ozone values over 40 ppb during daylight hours, and W126 with stronger weighting to higher hourly mean values, accumulated during 08:00–19:59. Although the density of measurement stations is highly variable across regions, in general, the highest ozone values (mean, 2010–14) are in mid-latitudes of the northern hemisphere, including southern USA, the Mediterranean basin, northern India, north, north-west and east China, the Republic of Korea and Japan. The lowest metric values reported are in Australia, New Zealand, southern parts of South America and some northern parts of Europe, Canada and the USA. Regional-scale assessments showed, for example, significantly higher AOT40 and W126 values in East Asia (EAS) than Europe (EUR) in wheat growing areas (p < 0.05), but not in rice growing areas. In NAM, the dominant trend during 1995–2014 was a significant decrease in ozone, whilst in EUR it was no change and in EAS it was a significant increase. TOAR-Vegetation provides recommendations to facilitate a more complete global assessment of ozone impacts on vegetation in the future, including: an increase in monitoring of ozone and collation of field evidence of the damaging effects on vegetation; an investigation of the effects on peri-urban agriculture and in mountain/upland areas; inclusion of additional pollutant, meteorological and inlet height data in the TOAR dataset; where not already in existence, establishing new region-specific thresholds for vegetation damage and an innovative integration of observations and modelling including stomatal uptake of the pollutant.

The Long Term Trends of Tropospheric Ozone in Major Regions in Korea

The Long Term Trends of Tropospheric Ozone in Major Regions in Korea

Attribution of recent ozone changes in the Southern Hemisphere mid-latitudes using statistical analysis and chemistry–climate model simulations

Abstract. Ozone (O3) trends and variability from a 28-year (1987–2014) ozonesonde record at Lauder, New Zealand, have been analysed and interpreted using a statistical model and a global chemistry–climate model (CCM). Lauder is a clean rural measurement site often representative of the Southern Hemisphere (SH) mid-latitude background atmosphere. O3 trends over this period at this location are characterised by a significant positive trend below 6 km, a significant negative trend in the tropopause region and the lower stratosphere between 9 and 15 km, and no significant trend in the free troposphere (6–9 km) and the stratosphere above 15 km. We find that significant positive trends in lower tropospheric ozone are correlated with increasing temperature and decreasing relative humidity at the surface over this period, whereas significant negative trends in the upper troposphere and the lower stratosphere appear to be strongly linked to an upward trend of the tropopause height. Relative humidity and the tropopause height also dominate O3 variability at Lauder in the lower troposphere and the tropopause region, respectively. We perform an attribution of these trends to anthropogenic forcings including O3 precursors, greenhouse gases (GHGs), and O3-depleting substances (ODSs), using CCM simulations. Results indicate that changes in anthropogenic O3 precursors contribute significantly to stratospheric O3 reduction, changes in ODSs contribute significantly to tropospheric O3 reduction, and increased GHGs contribute significantly to stratospheric O3 increases at Lauder. Methane (CH4) likely contributes positively to O3 trends in both the troposphere and the stratosphere, but the contribution is not significant at the 95 % confidence level over this period. An extended analysis of CCM results covering 1960–2010 (i.e. starting well before the observations) reveals significant contributions from all forcings to O3 trends at Lauder – i.e. increases in GHGs and the increase in CH4 alone all contribute significantly to O3 increases, net increases in ODSs lead to O3 reduction, and increases in non-methane O3 precursors cause O3 increases in the troposphere and reductions in the stratosphere. This study suggests that a long-term ozonesonde record obtained at a SH mid-latitude background site (corroborated by a surface O3 record at a nearby SH mid-latitude site, Baring Head, which also shows a significant positive trend) is a useful indicator for detecting atmospheric composition and climate change associated with human activities.

Commentary on “O3 variability in the troposphere as observed by IASI over 2008–2016: Contribution of atmospheric chemistry and dynamics” by Wespes et al.

AbstractEvaluation and attribution of variability and trends in tropospheric ozone requires consideration not only of the spatial distribution of ozone precursor emissions and their changes in time but also of variations in transport at regional and global scales. Satellite measurements of tropospheric ozone are now beginning to provide the vertical resolution, length of record, and density of coverage needed for disentangling the factors that influence variability and trends. A recent study by Wespes et al. (2017, https://doi.org/10.1002/2016JD025875), utilizing an 8 year data set from the Infrared Atmospheric Sounding Instrument (IASI) satellite instrument to perform a global scale, spatially resolved analysis of influences of geophysical drivers on tropospheric ozone variability, represents a key step toward understanding long‐term changes in the distribution of tropospheric ozone and its corresponding impacts on air quality, chemistry, and climate.

Trends of tropical tropospheric ozone from 20 years of European satellite measurements and perspectives for the Sentinel-5 Precursor

Abstract. In preparation of the TROPOMI/S5P launch in early 2017, a tropospheric ozone retrieval based on the convective cloud differential method was developed. For intensive tests we applied the algorithm to the total ozone columns and cloud data of the satellite instruments GOME, SCIAMACHY, OMI, GOME-2A and GOME-2B. Thereby a time series of 20 years (1995–2015) of tropospheric column ozone was generated. To have a consistent total ozone data set for all sensors, one common retrieval algorithm, namely GODFITv3, was applied and the L1 reflectances were also soft calibrated. The total ozone columns and the cloud data were input into the tropospheric ozone retrieval. However, the tropical tropospheric column ozone (TCO) for the individual instruments still showed small differences and, therefore, we harmonised the data set. For this purpose, a multilinear function was fitted to the averaged difference between SCIAMACHY's TCO and those from the other sensors. The original TCO was corrected by the fitted offset. GOME-2B data were corrected relative to the harmonised data from OMI and GOME-2A. The harmonisation leads to a better agreement between the different instruments. Also, a direct comparison of the TCO in the overlapping periods proves that GOME-2A agrees much better with SCIAMACHY after the harmonisation. The improvements for OMI were small. Based on the harmonised observations, we created a merged data product, containing the TCO from July 1995 to December 2015. A first application of this 20-year record is a trend analysis. The tropical trend is 0.7 ± 0.12 DU decade−1. Regionally the trends reach up to 1.8 DU decade−1 like on the African Atlantic coast, while over the western Pacific the tropospheric ozone declined over the last 20 years with up to 0.8 DU decade−1. The tropical tropospheric data record will be extended in the future with the TROPOMI/S5P data, where the TCO is part of the operational products.

Comparison of Long Term Tropospheric Ozone Trends Measured by Lidar and ECC Ozonesondes from 1991 to 2010 in Southern France

ECC (Electrochemical Concentration Cell) ozonesondes and UV DIAL (Differential Absorption Lidar) measurements have been carried out simultaneously at OHP (Observatoire de Haute Provence, 44°N, 6.7°E, 690 m) since 1991. A unique long-term trend assessment by two different instruments operated routinely at the same location is possible. Air mass trajectories have been calculated for all the ozone observations available at OHP. The bias between the seasonal mean calculated with lidar and ECC ozone vertical profiles for 4 timeperiods of 5 years is 0.6 ppbv in the free troposphere (4-8 km). Larger differences (> 10 ppbv) are explained by the need for clear sky conditions during lidar observations. The measurements of both instruments have been combined to decrease the impact of short-term atmospheric variability on the trend estimate.

Ensemble simulations of the role of the stratosphere in the attribution of northern extratropical tropospheric ozone variability

Abstract. Despite the need to understand the impact of changes in emissions and climate on tropospheric ozone, the attribution of tropospheric interannual ozone variability to specific processes has proven difficult. Here, we analyze the stratospheric contribution to tropospheric ozone variability and trends from 1953 to 2005 in the Northern Hemisphere (NH) mid-latitudes using four ensemble simulations of the free running (FR) Whole Atmosphere Community Climate Model (WACCM). The simulations are externally forced with observed time-varying (1) sea-surface temperatures (SSTs), (2) greenhouse gases (GHGs), (3) ozone depleting substances (ODS), (4) quasi-biennial oscillation (QBO), (5) solar variability (SV) and (6) stratospheric sulfate surface area density (SAD). A detailed representation of stratospheric chemistry is simulated, including the ozone loss due to volcanic eruptions and polar stratospheric clouds. In the troposphere, ozone production is represented by CH4–NOx smog chemistry, where surface chemical emissions remain interannually constant. Despite the simplicity of its tropospheric chemistry, at many NH measurement locations, the interannual ozone variability in the FR WACCM simulations is significantly correlated with the measured interannual variability. This suggests the importance of the external forcing applied in these simulations in driving interannual ozone variability. The variability and trend in the simulated 1953–2005 tropospheric ozone from 30 to 90° N at background surface measurement sites, 500 hPa measurement sites and in the area average are largely explained on interannual timescales by changes in the 30–90° N area averaged flux of ozone across the 100 hPa surface and changes in tropospheric methane concentrations. The average sensitivity of tropospheric ozone to methane (percent change in ozone to a percent change in methane) from 30 to 90° N is 0.17 at 500 hPa and 0.21 at the surface; the average sensitivity of tropospheric ozone to the 100 hPa ozone flux (percent change in ozone to a percent change in the ozone flux) from 30 to 90° N is 0.19 at 500 hPa and 0.11 at the surface. The 30–90° N simulated downward residual velocity at 100 hPa increased by 15% between 1953 and 2005. However, the impact of this on the 30–90° N 100 hPa ozone flux is modulated by the long-term changes in stratospheric ozone. The ozone flux decreases from 1965 to 1990 due to stratospheric ozone depletion, but increases again by approximately 7% from 1990 to 2005. The first empirical orthogonal function of interannual ozone variability explains from 40% (at the surface) to over 80% (at 150 hPa) of the simulated ozone interannual variability from 30 to 90° N. This identified mode of ozone variability shows strong stratosphere–troposphere coupling, demonstrating the importance of the stratosphere in an attribution of tropospheric ozone variability. The simulations, with no change in emissions, capture almost 50% of the measured ozone change during the 1990s at a variety of locations. This suggests that a large portion of the measured change is not due to changes in emissions, but can be traced to changes in large-scale modes of ozone variability. This emphasizes the difficulty in the attribution of ozone changes, and the importance of natural variability in understanding the trends and variability of ozone. We find little relation between the El Niño–Southern Oscillation (ENSO) index and large-scale tropospheric ozone variability over the long-term record.

Seasonal behavior and long-term trends of tropospheric ozone, its precursors and chemical conditions over Iran: A view from space

To identify spatial and temporal variations over the Iranian region, this study analyzed tropospheric formaldehyde (HCHO) and nitrogen dioxide (NO2) columns from Ozone Monitoring Instrument (OMI), carbon monoxide (CO) columns from the Measurement of Pollution in the Troposphere (MOPITT), and tropospheric column O3 (TCO) from OMI/MLS (Microwave Limb Sounder) satellites from 2005 to 2012. The study discovered high levels of HCHO (∼12 × 1015 molec./cm2) from plant isoprene emissions in the air above parts of the northern forest of Iran during the summer and from the oxidation of HCHO precursors emitted from petrochemical industrial facilities and biomass burning in South West Iran. This study showed that maximum NO2 levels (∼18 × 1015 molec./cm2) were concentrated in urban cities, indicating the predominance of anthropogenic sources. The results indicate that maximum concentrations were found in the winter, mainly because of weaker local winds and higher heating fuel consumption, in addition to lower hydroxyl radicals (OH). The high CO concentrations (∼2 × 1018 molec./cm2) in the early spring were inferred to mainly originate from a strong continental air mass from anthropogenic CO “hotspots” including regions around Caspian Sea, Europe, and North America, although the external sources of CO were partly suppressed by the Arabian anticyclone and topographic barriers. Variations in the TCO were seen to peak during the summer (∼40 DU), due to intensive solar radiation and stratospheric sources. This study also examined long-term trends in TCO and its precursors over a period of eight years in five urban cities in Iran. To perform the analysis, we estimated seasonal changes and inter-seasonal variations using least-squares harmonic estimation (LS-HE), which reduced uncertainty in the trend by 5–15%. The results showed significant increases in the levels of HCHO (∼0.08 ± 0.06 × 1015 molec./cm2 yr−1), NO2 (∼0.08 ± 0.02 × 1015 molec./cm2 yr−1), and peak annual TCO (∼0.59 ± 0.56 DU yr−1) but decreases in minimum annual TCO (∼−0.42 ± 0.60 DU yr−1) caused by an increase in NO2 species and annual CO (∼−0.95 ± 0.41 × 1016 molec./cm2 yr−1) partly resulting from the transport of reduced CO. The time series of the HCHO/NO2 column ratio (a proxy for the chemical conditions) indicated that during the last decade, the cities of Tehran, Ahvaz, and Isfahan exhibited steady chemical conditions while Tabriz and Mashhad exhibited a change from NOx-saturated/mixed to more NOx-sensitive chemical conditions.

Consistency of tropospheric ozone observations made by different platforms and techniques in the global databases

A large quantity of tropospheric ozone observations are conducted all over the world using different platforms and techniques for different purposes and goals. These observations are commonly used to derive seasonal cycles, interannual variations and long-term trends of ozone in the troposphere. In addition, they are used for comparison with three-dimensional chemistry-transport models to evaluate their performance and hence to test our current understanding of the tropospheric ozone variability. It is still challenging to provide robust tropospheric ozone trends throughout the world because of the great variability of ozone, its complex photochemical reactions, the rarity of long-term records, the diversity of measurement techniques and platforms, and the issues with data quality. In this work, we evaluated, with emphasis on the lower troposphere, the consistency of tropospheric ozone observations made by means of multiple platforms, including surface sites, sondes and regular aircraft, that are publicly available in the global databases, but excluding space-borne platforms. Concomitant observations were examined on an hourly basis (except for ±3 hours for sonde versus aircraft) for pairs of locations at less than 100-km distance. Generally, we found good agreement between sonde and surface observations. We also found that there was no need to apply any correction factor to ozonesonde observations except for Brewer–Mast sondes at Hohenpeissenberg. Because of a larger distance between the site pairs, the correlations found between the aircraft and surface measurements were poorer than those between sonde and surface measurements. However, a relatively simple wind segregation improved the agreement between the aircraft versus surface measurements. We found also that due to diurnal cycles, the sonde launching at a fixed local time led to positive or negative biases against the surface observations, suggesting that great attention should be paid to local time and diurnal variations when using ozonesonde in the analysis of seasonal cycles, long-term trends and interannual variations of lower tropospheric ozone. The comparison of surface data at Mt. Happo to regular aircraft data over Tokyo/Narita showed a relatively reasonable agreement, ensuring regionally representative ozone data sets in this region for trend analysis.

False Discovery Control in Large-Scale Spatial Multiple Testing.

This article develops a unified theoretical and computational framework for false discovery control in multiple testing of spatial signals. We consider both point-wise and cluster-wise spatial analyses, and derive oracle procedures which optimally control the false discovery rate, false discovery exceedance and false cluster rate, respectively. A data-driven finite approximation strategy is developed to mimic the oracle procedures on a continuous spatial domain. Our multiple testing procedures are asymptotically valid and can be effectively implemented using Bayesian computational algorithms for analysis of large spatial data sets. Numerical results show that the proposed procedures lead to more accurate error control and better power performance than conventional methods. We demonstrate our methods for analyzing the time trends in tropospheric ozone in eastern US.

Tropospheric ozone trends at Mauna Loa Observatory tied to decadal climate variability

Tropospheric ozone is a potent greenhouse gas, biological irritant and significant source of highly reactive hydroxyl radicals. Simulations with a chemistry climate model suggest that shifts in atmospheric circulation can account for the seasonally dependent trends in tropospheric ozone levels observed at Mauna Loa, Hawaii, over the past three decades.

Global distribution and trends of tropospheric ozone: An observation-based review

AbstractTropospheric ozone plays a major role in Earth’s atmospheric chemistry processes and also acts as an air pollutant and greenhouse gas. Due to its short lifetime, and dependence on sunlight and precursor emissions from natural and anthropogenic sources, tropospheric ozone’s abundance is highly variable in space and time on seasonal, interannual and decadal time-scales. Recent, and sometimes rapid, changes in observed ozone mixing ratios and ozone precursor emissions inspired us to produce this up-to-date overview of tropospheric ozone’s global distribution and trends. Much of the text is a synthesis of in situ and remotely sensed ozone observations reported in the peer-reviewed literature, but we also include some new and extended analyses using well-known and referenced datasets to draw connections between ozone trends and distributions in different regions of the world. In addition, we provide a brief evaluation of the accuracy of rural or remote surface ozone trends calculated by three state-of-the-science chemistry-climate models, the tools used by scientists to fill the gaps in our knowledge of global tropospheric ozone distribution and trends.

Stratospheric impact on tropospheric ozone variability and trends: 1990–2009

Abstract. The influence of stratospheric ozone on the interannual variability and trends in tropospheric ozone is evaluated between 30 and 90° N from 1990–2009 using ozone measurements and a global chemical transport model, the Community Atmospheric Model with chemistry (CAM-chem). Long-term measurements from ozonesondes, at 150 and 500 hPa, and the Measurements of OZone and water vapour by in-service Airbus aircraft programme (MOZAIC), at 500 hPa, are analyzed over Japan, Canada, the Eastern US and Northern and Central Europe. The measurements generally emphasize northern latitudes, although the simulation suggests that measurements over the Canadian, Northern and Central European regions are representative of the large-scale interannual ozone variability from 30 to 90° N at 500 hPa. CAM-chem is run with input meteorology from the National Center for Environmental Prediction; a tagging methodology is used to identify the stratospheric contribution to tropospheric ozone concentrations. A variant of the synthetic ozone tracer (synoz) is used to represent stratospheric ozone. Both the model and measurements indicate that on large spatial scales stratospheric interannual ozone variability drives significant tropospheric variability at 500 hPa and the surface. In particular, the simulation and the measurements suggest large stratospheric influence at the surface sites of Mace Head (Ireland) and Jungfraujoch (Switzerland) as well as many 500 hPa measurement locations. Both the measurements and simulation suggest the stratosphere has contributed to tropospheric ozone trends. In many locations between 30–90° N 500 hPa ozone significantly increased from 1990–2000, but has leveled off since (from 2000–2009). The simulated global ozone budget suggests global stratosphere-troposphere exchange increased in 1998–1999 in association with a global ozone anomaly. Discrepancies between the simulated and measured ozone budget include a large underestimation of measured ozone variability and discrepancies in long-term stratospheric ozone trends. This suggests the need for more sophisticated simulations including better representations of stratospheric chemistry and circulation.

Long‐term ozone trends at rural ozone monitoring sites across the United States, 1990–2010

This analysis provides an up‐to‐date assessment of long‐term (1990–2010) rural ozone trends using all available data in the western (12 sites) and eastern (41 sites) USA. Rather than focus solely on average ozone values or air quality standard violations, we consider the full range of ozone values, reporting trends for the 5th, 50th and 95th percentiles. Domestic ozone precursor emissions decreased strongly during 1990–2010. Accordingly 83%, 66% and 20% of summertime eastern U.S. sites experienced statistically significant ozone decreases in the 95th, 50th and 5th percentiles, respectively. During spring 43% of the eastern sites have statistically significant ozone decreases for the 95th percentile with no sites showing a significant increase. At the 50th percentile there is little overall change in the eastern U.S. In contrast, only 17% (2 sites) and 8% (1 site) of summertime western U.S. sites have statistically significant ozone decreases in the 95th and 50th percentiles, respectively. During spring no western site has a significant decrease, while 50% have a significant median increase. This dichotomy in U.S. ozone trends is discussed in terms of changing anthropogenic and biomass burning emissions. Consideration is given to the concept that increasing baseline ozone flowing into the western U.S. is counteracting ozone reductions due to domestic emission reductions. An update to the springtime free tropospheric ozone trend above western North America shows that ozone has increased significantly from 1995 to 2011 at the rate of 0.41 ± 0.27 ppbv yr−1. Finally, the ozone changes are examined in relation to regional temperature trends.