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Horowitz, L.

Publications and source records attributed to Horowitz, L..

Global Distribution and Trends of Tropospheric Ozone: An Observation-Based Review

Tropospheric 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.

Mixing ratios↗

Long-Term Changes in Lower Tropospheric Baseline Ozone Concentrations:

Two recent papers have quantified long-term ozone (O3) changes observed at northernmidlatitude sites that are believed to represent baseline (here understood as representative of continental to hemispheric scales) conditions. Three chemistry-climate models (NCAR CAM-chem, GFDL-CM3, and GISS-E2-R) have calculated retrospective tropospheric O3 concentrations as part of the Atmospheric Chemistry and Climate Model Intercomparison Project and Coupled Model Intercomparison Project Phase 5 model intercomparisons. We present an approach for quantitative comparisons of model results with measurements for seasonally averaged O3 concentrations. There is considerable qualitative agreement between the measurements and the models, but there are also substantial and consistent quantitative disagreements. Most notably, models (1) overestimate absolute O3 mixing ratios, on average by approximately 5 to 17 ppbv in the year 2000, (2) capture only approximately 50% of O3 changes observed over the past five to six decades, and little of observed seasonal differences, and (3) capture approximately 25 to 45% of the rate of change of the long-term changes. These disagreements are significant enough to indicate that only limited confidence can be placed on estimates of present-day radiative forcing of tropospheric O3 derived from modeled historic concentration changes and on predicted future O3 concentrations. Evidently our understanding of tropospheric O3, or the incorporation of chemistry and transport processes into current chemical climate models, is incomplete. Modeled O3 trends approximately parallel estimated trends in anthropogenic emissions of NO(sub x), an important O3 precursor, while measured O3 changes increase more rapidly than these emission estimates.

atmospheric composition↗

Radiative Forcing in the ACCMIP Historical and Future Climate Simulations

A primary goal of the Atmospheric Chemistry and Climate Model IntercomparisonProject (ACCMIP) was to characterize the short-lived drivers of preindustrial to 2100climate change in the current generation of climate models. Here we evaluate historicaland 5 future radiative forcing in the 10 ACCMIP models that included aerosols, 8 of whichalso participated in the Coupled Model Intercomparison Project phase 5 (CMIP5).The models generally reproduce present-day climatological total aerosol opticaldepth (AOD) relatively well. components to this total, however, and most appear to underestimate AOD over East10 Asia. The models generally capture 1980-2000 AOD trends fairly well, though theyunderpredict AOD increases over the YellowEastern Sea. They appear to strongly underestimate absorbing AOD, especially in East Asia, South and Southeast Asia, SouthAmerica and Southern Hemisphere Africa.We examined both the conventional direct radiative forcing at the tropopause (RF) and the forcing including rapid adjustments (adjusted forcing AF, including direct andindirect effects). The models calculated all aerosol all-sky 1850 to 2000 global meanannual average RF ranges from 0.06 to 0.49 W m(sup -2), with a mean of 0.26 W m(sup -2) and a median of 0.27 W m(sup -2. Adjusting for missing aerosol components in some modelsbrings the range to 0.12 to 0.62W m(sup -2), with a mean of 0.39W m(sup -2). Screen20ing the models based on their ability to capture spatial patterns and magnitudes ofAOD and AOD trends yields a quality-controlled mean of 0.42W m(sup -2) and range of0.33 to 0.50 W m(sup -2) (accounting for missing components). The CMIP5 subset of ACCMIPmodels spans 0.06 to 0.49W m(sup -2), suggesting some CMIP5 simulations likelyhave too little aerosol RF. A substantial, but not well quantified, contribution to histori25cal aerosol RF may come from climate feedbacks (35 to 58). The mean aerosol AF during this period is 1.12W m(sup -2) (median value 1.16W m(sup -2), range 0.72 to1.44W m(sup -2), indicating that adjustments to aerosols, which include cloud, water vaporand temperature, lead to stronger forcing than the aerosol direct RF.

Climate Models↗

Tropospheric Ozone Changes, Radiative Forcing and Attribution to Emissions in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (+/-1 standard deviation) in RFs of +/-17%. Three different radiation schemes were used - we find differences in RFs between schemes (for the same ozone fields) of +/-10 percent. Applying two different tropopause definitions gives differences in RFs of +/-3 percent. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of +/-30 percent for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44+/-12 percent), nitrogen oxides (31 +/- 9 percent), carbon monoxide (15 +/- 3 percent) and non-methane volatile organic compounds (9 +/- 2 percent); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m(−2) DU(−1), a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m(−2); relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. Climate change has relatively small impacts on global mean tropospheric ozone RF.

climate change↗