Increase In Tropospheric Ozone Research Articles

Atmospheric composition and climate impacts of a future hydrogen economy

Abstract. Hydrogen is expected to play a key role in the global energy transition to net zero emissions in many scenarios. However, fugitive emissions of hydrogen into the atmosphere during its production, storage, distribution and use could reduce the climate benefit and also have implications for air quality. Here, we explore the atmospheric composition and climate impacts of increases in atmospheric hydrogen abundance using the UK Earth System Model (UKESM1) chemistry–climate model. Increases in hydrogen result in increases in methane, tropospheric ozone and stratospheric water vapour, resulting in a positive radiative forcing. However, some of the impacts of hydrogen leakage are partially offset by potential reductions in emissions of methane, carbon monoxide, nitrogen oxides and volatile organic compounds from the consumption of fossil fuels. We derive a refined methodology for determining indirect global warming potentials (GWPs) from parameters derived from steady-state simulations, which is applicable to both shorter-lived species and those with intermediate and longer lifetimes, such as hydrogen. Using this methodology, we determine a 100-year global warming potential for hydrogen of 12 ± 6. Based on this GWP and hydrogen leakage rates of 1 % and 10 %, we find that hydrogen leakage offsets approximately 0.4 % and 4 % respectively of total equivalent CO2 emission reductions in our global hydrogen economy scenario. To maximise the benefit of hydrogen as an energy source, emissions associated with hydrogen leakage and emissions of the ozone precursor gases need to be minimised.

Changes in tropospheric ozone over India: Variability, long-term trends and climate forcing

At higher concentrations, tropospheric ozone can cause respiratory difficulties, premature human mortality and can harm vegetation by reducing photosynthesis and its growth. It is an oxidant and also an important greenhouse gas with positive feedback to temperature. It is produced as a byproduct of chemical reactions involving nitrogen oxides (NOx) and volatile organic compounds (VOCs) in the presence of sunlight, rather than being emitted directly to the atmosphere. Here, we analyse the seasonal and inter-annual variability, long-term trends and radiative forcing of the tropospheric column ozone (TPO) in India for the period of 2005–2020 using satellite and ground-based data. The analysis shows very high annual averaged TPO in the Indo-Gangetic Plain (IGP) and North West India, about 45–50 DU. Our findings reveal a significant increase of TPO in India, with the highest trend in the peninsular region (0.295 ± 0.0617 DU/year) and the lowest in North West (0.179 ± 0.048 DU/year). The increase in tropospheric ozone reveals a warming of about 0.5 °C in the troposphere as there is an associated radiative forcing of about 0.2–0.5 W/m2 at the tropopause (125 hPa); indicating that the increasing tropospheric ozone is a great concern for regional warming, public health and ecosystem dynamics.

Rapid increase in tropospheric ozone over Southeast Asia attributed to changes in precursor emission source regions and sectors

Observations indicate that tropospheric ozone (O3) concentrations over Southeast Asia have been increasing rapidly since the 1990s. Here, we quantify source contributions from geographical regions and emission sectors of the two distinct types of O3 precursors, i.e., nitrogen oxides (NOx) and volatile organic compounds (VOCs), to the increase in tropospheric O3 in Southeast Asia during 1990–2019 using an O3 source tagging technique implemented in a global chemistry-climate model. The results show that although local anthropogenic emission of NOx in Southeast Asia only contributes 18% of the annual averaged near-surface O3 concentration, the increase in local NOx emission dominates the increasing trend of O3 concentration in Southeast Asia, accounting for 107% of the regional averaged trend of 1.07 ppb decade−1. Increases in NOx emissions from East Asia and South Asia explain 29% of the increasing trend, but 9% is offset by the emission reduction in North America. The vertical O3 trends in the troposphere contributed by individual source regions are consistent with those near the surface. Ground transportation is responsible for 79% of the rapid O3 increase, followed by 39% contribution from international shipping. Because an increase in anthropogenic NOx emissions enhances the O3 production efficiency by VOCs, the increase in O3 concentrations in Southeast Asia is thereby largely contributed by methane and biogenic VOCs.

Air pollution as a substantial threat to the improvement of agricultural total factor productivity: Global evidence

ObjectiveThis study aims to provide empirical evidence about whether and to what extent air pollution affects the global agricultural total factor productivity (TFP). MethodsThe research sample covers 146 countries all over the world during 2010–2019. Two-way fixed effects panel regression models are used to estimate air pollution’s impacts. A random forest analysis is conducted to assess the relative importance of independent variables. ResultsThe results show that, on average, a 1% increase in fine particulate matter (PM2.5) and tropospheric ozone (O3) concentration would cause the agricultural TFP to decline by 0.104% and 0.207%, respectively. Air pollution’s adverse impact widely exists in various countries with different development levels, pollution degrees, and industrial structures. This study also finds that temperature has a moderating effect on the relationship between PM2.5 and agricultural TFP. PM2.5 pollution’s detrimental impact is weaker (stronger) in a warmer (cooler) climate. In addition, the random forest analysis confirms that air pollution is among the most crucial predictors of agricultural productivity. ConclusionsAir pollution is a substantial threat to the improvement of global agricultural TFP. Worldwide actions should be taken to ameliorate air quality, for the sake of agricultural sustainability and global food security.

The historical ozone trends simulated with the SOCOLv4 and their comparison with observations and reanalyses

Abstract. There is evidence that the ozone layer has begun to recover owing to the ban on the production of halogenated ozone-depleting substances (hODS) accomplished by the Montreal Protocol and its amendments and adjustments (MPA). However, recent studies, while reporting an increase in tropospheric ozone from the anthropogenic NOx and CH4 and confirming the ozone recovery in the upper stratosphere from the effects of hODS, also indicate a continuing decline in the lower tropical and mid-latitudinal stratospheric ozone. While these are indications derived from observations, they are not reproduced by current global chemistry–climate models (CCMs), which show positive or near-zero trends for ozone in the lower stratosphere. This makes it difficult to robustly establish ozone evolution and has sparked debate about the ability of contemporary CCMs to simulate future ozone trends. We applied the new Earth system model (ESM) SOCOLv4 (SOlar Climate Ozone Links, version 4) to calculate long-term ozone trends between 1985–2018 and compare them with trends derived from the BAyeSian Integrated and Consolidated (BASIC) ozone composite and MERRA-2, ERA-5, and MSRv2 reanalyses. We designed the model experiment with a six-member ensemble to account for the uncertainty of the natural variability. The trend analysis is performed separately for the ozone depletion (1985–1997) and ozone recovery (1998–2018) phases of the ozone evolution. Within the 1998–2018 period, SOCOLv4 shows statistically significant positive ozone trends in the mesosphere, upper and middle stratosphere, and a steady increase in the tropospheric ozone. The SOCOLv4 results also suggest slightly negative trends in the extra-polar lower stratosphere, yet they barely agree with the BASIC ozone composite in terms of magnitude and statistical significance. However, in some realizations of the SOCOLv4 experiment, the pattern of ozone trends in the lower stratosphere resembles much of what is observed, suggesting that SOCOLv4 may be able to reproduce the observed trends in this region. Thus, the model results reveal marginally significant negative ozone changes in parts of the low-latitude lower stratosphere, which agrees in general with the negative tendencies extracted from the satellite data composite. Despite the slightly smaller significance and magnitude of the simulated ensemble mean, we confirm that modern CCMs such as SOCOLv4 are generally capable of simulating the observed ozone changes, justifying their use to project the future evolution of the ozone layer.

Multidecadal increases in global tropospheric ozone derived from ozonesonde and surface site observations: can models reproduce ozone trends?

Abstract. Despite decades of effort, the drivers of global long-term trends in tropospheric ozone are not well understood, impacting estimates of ozone radiative forcing and the global ozone budget. We analyze tropospheric ozone trends since 1980 using ozonesondes and remote surface measurements around the globe and investigate the ability of two atmospheric chemical transport models, GEOS-Chem and MERRA2-GMI, to reproduce these trends. Global tropospheric ozone trends measured at 25 ozonesonde sites from 1990–2017 (nine sites since 1980s) show increasing trends averaging 1.8 ± 1.3 ppb per decade across sites in the free troposphere (800–400 hPa). Relative trends in sondes are more pronounced closer to the surface (3.5 % per decade above 700 hPa, 4.3 % per decade below 700 hPa on average), suggesting the importance of surface emissions (anthropogenic, soil NOx, impacts on biogenic volatile organic compounds (VOCs) from land use changes, etc.) in observed changes. While most surface sites (148 of 238) in the United States and Europe exhibit decreases in high daytime ozone values due to regulatory efforts, 73 % of global sites outside these regions (24 of 33 sites) show increases from 1990–2014 that average 1.4 ± 0.9 ppb per decade. In all regions, increasing ozone trends both at the surface and aloft are at least partially attributable to increases in 5th percentile ozone, which average 1.8 ± 1.3 ppb per decade and reflect the global increase of baseline ozone in rural areas. Observed ozone percentile distributions at the surface have shifted notably across the globe: all regions show increases in low tails (i.e., below 25th percentile), North America and Europe show decreases in high tails (above 75th percentile), and the Southern Hemisphere and Japan show increases across the entire distribution. Three model simulations comprising different emissions inventories, chemical schemes, and resolutions, sampled at the same locations and times of observations, are not able to replicate long-term ozone trends either at the surface or free troposphere, often underestimating trends. We find that ∼75 % of the average ozone trend from 800–400 hPa across the 25 ozonesonde sites is captured by MERRA2-GMI, and <20 % is captured by GEOS-Chem. MERRA2-GMI performs better than GEOS-Chem in the northern midlatitude free troposphere, reproducing nearly half of increasing trends since 1990 and capturing stratosphere–troposphere exchange (STE) determined via a stratospheric ozone tracer. While all models tend to capture the direction of shifts in the ozone distribution and typically capture changes in high and low tails, they tend to underestimate the magnitude of the shift in medians. However, each model shows an 8 %–12 % (or 23–32 Tg) increase in total tropospheric ozone burden from 1980 to 2017. Sensitivity simulations using GEOS-Chem and the stratospheric ozone tracer in MERRA2-GMI suggest that in the northern midlatitudes and high latitudes, dynamics such as STE are most important for reproducing ozone trends in models in the middle and upper troposphere, while emissions are more important closer to the surface. Our model evaluation for the last 4 decades reveals that the recent version of the GEOS-Chem model underpredicts free tropospheric ozone across this long time period, particularly in winter and spring over midlatitudes to high latitudes. Such widespread model underestimation of tropospheric ozone highlights the need for better understanding of the processes that transport ozone and promote its production.

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

AbstractTropospheric 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−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 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.

Data for "Rapid increase in tropospheric ozone over Southeast Asia attributed to changes in precursor emission source regions and sectors"

Data for "Rapid increase in tropospheric ozone over Southeast Asia attributed to changes in precursor emission source regions and sectors"

Apportionment of the Pre‐Industrial to Present‐Day Climate Forcing by Methane Using UKESM1: The Role of the Cloud Radiative Effect

AbstractThe Year 1850 to 2014 increase in methane from 808 to 1831 ppb leads to an effective radiative forcing (ERF) of 0.97 ± 0.04 W m−2 in the United Kingdom's Earth System Model, UKESM1. The direct methane contribution is 0.54 ± 0.04 W m−2. It is better represented in UKESM1 than in its predecessor model HadGEM2 due to shortwave and longwave absorption improvements and the absence of an anomalous dust response in the UKESM1 simulations. An indirect ozone ERF of 0.13–0.20 W m−2 is due to the tropospheric ozone increase outweighing that of the stratospheric decrease. The indirect water vapor ERF of 0.02–0.07 W m−2 is consistent with previous estimates. The methane increase also leads to a cloud radiative effect of 0.12 ± 0.02 W m−2 from thermodynamic adjustments and aerosol‐cloud interactions (aci). Shortwave and longwave contributions of 0.23 and −0.35 W m−2 to the cloud forcing arise from radiative heating and stabilization of the upper troposphere, reducing convection and global cloud cover. The aerosol‐mediated contribution (0.28–0.30 W m−2) is due to changes in oxidants reducing new particle formation (−8%), shifting the aerosol size distribution toward fewer but larger particles. Cloud droplet number concentration decreases and cloud droplet effective radius increases. This reduction in the Twomey effect switches the cloud forcing sign (−0.14 to 0.12 W m−2) and is due to chemistry‐aerosol‐cloud coupling in UKESM1. Despite uncertainties in rapid adjustments and process representation in models, these results highlight the potential importance of chemistry‐aerosol‐cloud interactions and dynamical adjustments in climate forcing.

Air Pollution and COVID-19: Any Causal Link?

Abstract Several studies have amply proved that air pollution negatively impacts human health. The nature of its effects on COVID-19 has, of late, become an area for investigation across the world. The present study reviews reports in the literature that centred on whether the presence and impact of air pollutants magnified the symptoms and actions of COVID-19 and whether preventive measures taken, starting with lockdown, affected air pollution levels. This may help to establish causality, if any, between pollution and COVID-19. Studies were chosen to ensure representation of all continents with diverse climatic conditions with the exception of Australia. Most of the studies concluded that air pollutants declined as a result of the lockdowns imposed to constrain the spread of COVID-19. A significant reduction in NO2 is observed along with the resultant increase in tropospheric ozone in the atmosphere. The inference is untrue in hostile meteorological conditions. According to some studies, reduction in pollutants aided in contracting the spread and severity of COVID-19. On the other hand, hostile weather conditions incited the spread and magnitude of COVID-19. A governmental policy inference could be that government intervention through imposing a lockdown would reduce air pollution and ensure the health safety of the people, but economic growth considerations need to be balanced against the benefit for public health.

Analysis of Ozone Pollution Characteristics and Influencing Factors in Northeast Economic Cooperation Region, China

The increase in tropospheric ozone (O3) concentration has become one of the factors restricting urban development. This paper selected the important economic cooperation areas in Northeast China as the research object and collected the hourly monitoring data of pollutants and meteorological data in 11 cities from 1 January 2015 to 31 December 2019. The temporal and spatial variation trend of O3 concentration and the effects of meteorological factors and other pollutants, including CO (carbon monoxide), SO2 (sulfur dioxide), NO2 (nitrogen dioxide), and PM2.5 and PM10 (PM particles with aerodynamic diameters less than 2.5 μm and 10 μm) on ozone concentration were analyzed. At the same time, the variation period of O3 concentration was further analyzed by Morlet wavelet analysis. The results showed that the O3 pollution in the study area had a significant spatial correlation. The spatial distribution showed that the O3 concentration was relatively high in the south and low in the northeast. Seasonally, the O3 concentration was the highest in spring, followed by summer, and the lowest in winter. The diurnal variation of O3 concentration presented a “single peak” pattern. O3 concentration had a significant positive correlation with temperature, sunshine duration, and wind speed and a significant anticorrelation with CO, NO2, SO2, and PM2.5 concentration. Under the time scale of a = 9, 23, O3 had significant periodic fluctuation, which was similar to those of wind speed and temperature.

Numerical Study of Meteorological Factors for Tropospheric Nocturnal Ozone Increase in the Metropolitan Area of São Paulo

One of the central problems in large cities is air pollution, mainly caused by vehicular emissions. Tropospheric ozone is an atmospheric oxidizing gas that forms in minimal amounts naturally, affecting peoples’ health. This pollutant is formed by the NO2 photolysis, creating a main peak during the day. Nighttime secondary peaks occur in several parts of the world, but their intensity and frequency depend on the local condition. In this sense, this works aims to study the local characteristics for tropospheric nocturnal ozone levels in the Metropolitan Area of São Paulo, in Brazil, using the Simple Photochemical Module coupled to the Brazilian Developments on the Regional Atmospheric Modeling System. For this, three different situations of nocturnal occurrence were studied. The results show that the nocturnal maximum of ozone concentrations is related to the vertical transport of this pollutant from higher levels of the atmosphere to the surface and is not related to the synoptic condition.

Slow feedbacks resulting from strongly enhanced atmospheric methane mixing ratios in a chemistry–climate model with mixed-layer ocean

Abstract. In a previous study the quasi-instantaneous chemical impacts (rapid adjustments) of strongly enhanced methane (CH4) mixing ratios have been analysed. However, to quantify the influence of the respective slow climate feedbacks on the chemical composition it is necessary to include the radiation-driven temperature feedback. Therefore, we perform sensitivity simulations with doubled and quintupled present-day (year 2010) CH4 mixing ratios with the chemistry–climate model EMAC (European Centre for Medium-Range Weather Forecasts, Hamburg version – Modular Earth Submodel System (ECHAM/MESSy) Atmospheric Chemistry) and include in a novel set-up a mixed-layer ocean model to account for tropospheric warming. Strong increases in CH4 lead to a reduction in the hydroxyl radical in the troposphere, thereby extending the CH4 lifetime. Slow climate feedbacks counteract this reduction in the hydroxyl radical through increases in tropospheric water vapour and ozone, thereby dampening the extension of CH4 lifetime in comparison with the quasi-instantaneous response. Changes in the stratospheric circulation evolve clearly with the warming of the troposphere. The Brewer–Dobson circulation strengthens, affecting the response of trace gases, such as ozone, water vapour and CH4 in the stratosphere, and also causing stratospheric temperature changes. In the middle and upper stratosphere, the increase in stratospheric water vapour is reduced with respect to the quasi-instantaneous response. We find that this difference cannot be explained by the response of the cold point and the associated water vapour entry values but by a weaker strengthening of the in situ source of water vapour through CH4 oxidation. However, in the lower stratosphere water vapour increases more strongly when tropospheric warming is accounted for, enlarging its overall radiative impact. The response of the stratosphere adjusted temperatures driven by slow climate feedbacks is dominated by these increases in stratospheric water vapour as well as strongly decreased ozone mixing ratios above the tropical tropopause, which result from enhanced tropical upwelling. While rapid radiative adjustments from ozone and stratospheric water vapour make an essential contribution to the effective CH4 radiative forcing, the radiative impact of the respective slow feedbacks is rather moderate. In line with this, the climate sensitivity from CH4 changes in this chemistry–climate model set-up is not significantly different from the climate sensitivity in carbon-dioxide-driven simulations, provided that the CH4 effective radiative forcing includes the rapid adjustments from ozone and stratospheric water vapour changes.

Increased tropospheric ozone levels enhance pathogen infection levels of amphibians

As a result of anthropogenic activities, changes to the chemistry of Earth's atmosphere pose a threat to ecosystem health and biodiversity. One such change is the increase in tropospheric ozone (O3), which is particularly severe in the Mediterranean basin area, where the levels of this pollutant are chronically high during spring and summer time. Within this region, Mediterranean mountain ecosystems are hot spots for biodiversity which may be especially vulnerable to changes in O3 levels. Declines in montane amphibian populations have been recorded worldwide, including the Mediterranean basin. A significant driver of these declines is the emerging infection disease, chytridiomycosis, caused by the aquatic fungus Batrachochytrium dendrobatidis (Bd). Chytridiomycosis has negatively affected populations of several amphibian species in the Spanish Central Range, including in the Sierra Guadarrama, and interactions with other biotic and abiotic factors are an important part of these declines. However, there is little evidence or knowledge of whether tropospheric O3 levels may be another factor in the outbreaks of this disease. To test the hypothesis that O3 levels are another interactive driver of Bd infection dynamics, two different approaches were followed: 1) an experimental study in open top chambers was used to quantify the aspects of how Bd infection progressed throughout the metamorphic process under four different O3 levels; and 2) a field epidemiological study was used to analyse the relationship between the Bd infection load in the Sierra de Guadarrama and tropospheric O3 levels during a 9 year period. Our results suggest that high O3 levels significantly delayed the rate of development of tadpoles and increased Bd infection, providing empirical evidence of two new separate ways that may explain population declines of montane amphibians.

Sub micron aerosol variability and its ageing process at a high altitude site in India: Impact of meteorological conditions

The effect of relative humidity and temperature on the submicron aerosol variability and its ageing process was studied over a high altitude site, Mahabaleshwar in south-west India. The mass composition of non-refractory particulate matter of 1 μm (NR-PM1) size was obtained using Time of Flight Aerosol Chemical Speciation Monitor (ToF-ACSM) along with the measurements on a few trace gases during winter (December 2017–February 2018) and summer season (20th March - 5th May 2018). Sulfate exhibited strong dependence on the relative humidity (RH) as its mass fraction increased with the increase in RH. The Sulfate oxidation ratio (SOR) calculated during summer season also showed an increasing trend with RH indicating the influence of aqueous phase oxidation on sulfate fraction. On the other hand, OOA showed remarkable enhancement in its mass fraction with the increase in temperature along with the corresponding increase in f44 and tropospheric ozone. OOA, ozone and f44 ratio increased 14–34%, 8–26% and 25–43% respectively with the increase in temperature from 18 to 30 °C. This is indicative of the dominance of photochemical ageing processes during high temperature conditions. The extent of photochemical ageing was found to be higher during summer season (mean temperature ∼25.4 ± 2.6 °C) as compared to winter season (mean temperature ∼20.5 ± 2.6 °C). The nitrate diurnal was majorly governed by gas to particle partitioning process during winter season, whereas the summertime nitrate diurnal was influenced primarily by its formation rate. The non parametric wind regression analysis revealed that the mass concentration during winter was majorly contributed by distant sources from north east direction while during summer the local sources were more dominant.

Update and evaluation of the ozone dry deposition in Oslo CTM3 v1.0

Abstract. High concentrations of ozone in ambient air are hazardous not only to humans but to the ecosystem in general. The impact of ozone damage on vegetation and agricultural plants in combination with advancing climate change may affect food security in the future. While the future scenarios in themselves are uncertain, there are limiting factors constraining the accuracy of surface ozone modeling also at present: the distribution and amount of ozone precursors and ozone-depleting substances, the stratosphere–troposphere exchange, as well as scavenging processes. Removal of any substance through gravitational settling or by uptake by plants and soil is referred to as dry deposition. The process of dry deposition is important for predicting surface ozone concentrations and understanding the observed amount and increase of tropospheric background ozone. The conceptual dry deposition velocities are calculated following a resistance-analogous approach, wherein aerodynamic, quasi-laminar, and canopy resistance are key components, but these are hard to measure explicitly. We present an update of the dry deposition scheme implemented in Oslo CTM3. We change from a purely empirical dry deposition parameterization to a more process-based one which takes the state of the atmosphere and vegetation into account. We examine the sensitivity of the scheme to various parameters, e.g., the stomatal conductance-based description of the canopy resistance and the choice of ozone surface resistance, and evaluate the resulting modeled ozone dry deposition with respect to observations and multi-model studies. Individual dry deposition velocities are now available for each land surface type and agree generally well with observations. We also estimate the impact on the modeled ozone concentrations at the surface. We show that the global annual total ozone dry deposition decreases with respect to the previous model version (−37 %), leading to an increase in surface ozone of more than 100 % in some regions. While high sensitivity to changes in dry deposition to vegetation is found in the tropics and the Northern Hemisphere, the largest impact on global scales is associated with the choice of prescribed ozone surface resistance over the ocean and deserts.

Isotopic constraint on the twentieth-century increase in tropospheric ozone.

Tropospheric ozone (O3) is a key component of air pollution and an important anthropogenic greenhouse gas1. During the twentieth century, the proliferation of the internal combustion engine, rapid industrialization and land-use change led to a global-scale increase in O3 concentrations2,3; however, the magnitude of this increase is uncertain. Atmospheric chemistry models typically predict4-7 an increase in the tropospheric O3 burden of between 25 and 50 per cent since 1900, whereas direct measurements made in the late nineteenth century indicate that surface O3 mixing ratios increased by up to 300 per cent8-10 over that time period. However, the accuracy and diagnostic power of these measurements remains controversial2. Here we use a record of the clumped-isotope composition of molecular oxygen (18O18O in O2) trapped in polar firn and ice from 1590 to 2016 AD, as well as atmospheric chemistry model simulations, to constrain changes in tropospheric O3 concentrations. We find that during the second half of the twentieth century, the proportion of 18O18O in O2 decreased by 0.03±0.02 parts per thousand (95 per cent confidence interval) below its 1590-1958 AD mean, which implies that tropospheric O3 increased by less than 40 per cent during that time. These results corroborate model predictions of global-scale increases in surface pollution and vegetative stress caused by increasing anthropogenic emissions of O3 precursors4,5,11. We also estimate thatthe radiative forcing of tropospheric O3 since 1850 AD is probably less than +0.4 watts per square metre, consistent with results from recent climate modelling studies12.

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.

Simulated Global Climate Response to Tropospheric Ozone‐Induced Changes in Plant Transpiration

AbstractTropospheric ozone (O3) pollution is known to damage vegetation, reducing photosynthesis and stomatal conductance, resulting in modified plant transpiration to the atmosphere. We use an Earth system model to show that global transpiration response to near‐present‐day surface tropospheric ozone results in large‐scale global perturbations to net outgoing long‐wave and incoming shortwave radiation. Our results suggest that the radiative effect is dominated by a reduction in shortwave cloud forcing in polluted regions, in response to ozone‐induced reduction in land‐atmosphere moisture flux and atmospheric humidity. We simulate a statistically significant response of annual surface air temperature of up to ~ +1.5 K due to this ozone effect in vegetated regions subjected to ozone pollution. This mechanism is expected to further increase the net warming resulting from historic and future increases in tropospheric ozone.