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A Modeling Study of Effective Radiative Forcing and Climate Response Due to Tropospheric Ozone


doi: 10.1007/s00376-016-5193-0

  • This study simulates the effective radiative forcing (ERF) of tropospheric ozone from 1850 to 2013 and its effects on global climate using an aerosol-climate coupled model, BCC_AGCM2.0.1_CUACE/Aero, in combination with OMI (Ozone Monitoring Instrument) satellite ozone data. According to the OMI observations, the global annual mean tropospheric column ozone (TCO) was 33.9 DU in 2013, and the largest TCO was distributed in the belts between 30°N and 45°N and at approximately 30°S; the annual mean TCO was higher in the Northern Hemisphere than that in the Southern Hemisphere; and in boreal summer and autumn, the global mean TCO was higher than in winter and spring. The simulated ERF due to the change in tropospheric ozone concentration from 1850 to 2013 was 0.46 W m-2, thereby causing an increase in the global annual mean surface temperature by 0.36°C, and precipitation by 0.02 mm d-1 (the increase of surface temperature had a significance level above 95%). The surface temperature was increased more obviously over the high latitudes in both hemispheres, with the maximum exceeding 1.4°C in Siberia. There were opposite changes in precipitation near the equator, with an increase of 0.5 mm d-1 near the Hawaiian Islands and a decrease of about -0.6 mm d-1 near the middle of the Indian Ocean.
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  • Antõn M., M. Lõpez, J. M. Vilaplana, M. Kroon, R. McPeters, M. Ba\ nõn, A. Serrano, 2009: Validation of OMI-TOMS and OMI-DOAS total ozone column using five Brewer spectroradiometers at the Iberian Peninsula. J. Geophys. Res.: Atmos., 114, D14307.10.1029/2009JD012003642649881575399311905722febefdaahttp%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2F2009JD012003%2Fabstracthttp://onlinelibrary.wiley.com/doi/10.1029/2009JD012003/abstractThis article focuses on the comparison of the total ozone column data from the Ozone Monitoring Instrument (OMI) flying aboard the NASA EOS-Aura satellite platform with ground-based measurement recorded by Brewer spectroradiometers located at five Spanish remote sensing ground stations between January 2005 and December 2007. The satellite data are derived from two algorithms: OMI Total Ozone Mapping Spectrometer (OMI-TOMS) and OMI Differential Optical Absorption Spectroscopy (OMI-DOAS). The largest relative differences between these OMI total ozone column estimates reach 5% with a significant seasonal dependence. The agreement between OMI ozone data and Brewer measurements is excellent. Total ozone columns from OMI-TOMS are on average a mere 2.0% lower than Brewer data. For OMI-DOAS data the bias is a mere 1.4%. However, the relative difference between OMI-TOMS and Brewer measurements shows a notably lower seasonal dependence and variability than the differences between OMI-DOAS and ground-based data. For both OMI ozone data products these relative differences show significant dependence on the satellite ground pixel solar zenith angle for cloud-free cases as well as for cloudy conditions. However, the OMI ozone data products are shown to reveal opposite behavior with respect to the two antagonistic sky conditions. No significant dependency of the ground-based to satellite-based differences with respect to the satellite cross-track position is seen for either OMI retrieval algorithm.
    Buchard V., C. Brogniez, F. Auriol, B. Bonnel, J. Lenoble, A. Tanskanen, B. Bojkov, and P. Veefkind, 2008: Comparison of OMI ozone and UV irradiance data with ground-based measurements at two French sites. Atmos. Chem. Phys., 8, 4517- 4528.10.5194/acp-8-4517-2008ea62473eea51a5946a4cfcdf1890a8f7http%3A%2F%2Fwww.oalib.com%2Fpaper%2F1371315http://www.oalib.com/paper/1371315Ozone Monitoring Instrument (OMI), launched in July 2004, is dedicated to the monitoring of the Earth's ozone, air quality and climate. OMI provides among other things the total column of ozone (TOC), the surface ultraviolet (UV) irradiance at several wavelengths, the erythemal dose rate and the erythemal daily dose. The main objective of this work is to validate OMI data with ground-based instruments in order to use OMI products (collection 2) for scientific studies. The Laboratoire d'Optique Atmosph0108rique (LOA) located in Villeneuve d'Ascq in the north of France performs solar UV measurements using a spectroradiometer and a broadband radiometer. The site of Brian01§on in the French Southern Alps is also equipped with a spectroradiometer operated by Interaction Rayonnement Solaire Atmosph01¨re (IRSA). The instrument belongs to the Centre Europ0108en M0108dical et Bioclimatologique de Recherche et d'Enseignement Sup0108rieur. The comparison between the TOC retrieved with ground-based measurements and OMI TOC shows good agreement at both sites for all sky conditions. Comparisons of spectral UV on clear sky conditions are also satisfying whereas results of comparisons of the erythemal daily doses and erythemal dose rates for all sky conditions and for clear sky show that OMI overestimates significantly surface UV doses at both sites.
    Chang W.-Y., H. Liao, and H.-J. Wang, 2009: Climate responses to direct radiative forcing of anthropogenic aerosols,tropospheric ozone, and long-lived greenhouse gases in eastern China over 1951-2000. Adv. Atmos.Sci. , 26, 748-762, doi: 10.1007/s00376-009-9032-4.10.1007/s00376-009-9032-456b4aadb4b2ce72484b365ee7a9ee3cdhttp%3A%2F%2Fwww.cqvip.com%2FMain%2FDetail.aspx%3Fid%3D30867379http://d.wanfangdata.com.cn/Periodical_dqkxjz-e200904015.aspxA unified chemistry-aerosol-climate model is applied in this work to compare climate responses to changing concentrat, ions of long-lived greenhouse gases (GHGs, CO2, CH4, N2O, tropospheric O3, and aerosols during the years 1951--2000. Concentrations of sulfate, nitrate, primary organic carbon (POA), secondary organic carbon (SOA), black carbon (BC) aerosols, and tropospheric O3 for the years 1950 and 2000 are obtained a priori by coupled chemistry-aerosol-GCM simulations, and then monthly concentrations are interpolated linearly between 1951 and 2000. The annual concentrations of GHGs are taken from the IPCC Third Assessment Report. BC aerosol is internally mixed with other aerosols. Model results indicate that the simulated climate change over 1951--2000 is sensitive to anthropogenic changes in atmospheric components. The predicted year 2000 global mean surface air temperature can differ by 0.8o with different forcings. Relative to the climate simulation without changes in GHGs, O3, and aerosols, anthropogenic forcings of SO2-4, BC, BC+SO2-4, BC+SO2-4+POA, BC+SO2-4+POA+SOA+NO-3, O3, and GHGs are predicted to change the surface air temperature averaged over 1971--2000 in eastern China, respectively, by -0.40oC, +0.62oC, +0.18oC, +0.15oC, -0.78oC, +0.43oC, and +0.85oC, and to change the precipitation, respectively, by -0.21, +0.07, -0.03, +0.02, -0.24, -0.08, and +0.10 mm d-1. The authors conclude that all major aerosols are as important as GHGs in influencing climate change in eastern China, and tropospheric O3 also needs to be included in studies of regional climate change in China.
    Conley A. J., J. F. Lamarque, F. Vitt, W. D. Collins, and J. Kiehl, 2013: PORT, a CESM tool for the diagnosis of radiative forcing. Geoscientific Model Development, 6, 469- 476.10.5194/gmd-6-469-2013e4750b2f-1bd5-412d-9cc3-c1cd1af46775WOS:00031843860001330ff569cee55a104cd4e3fa4b9c9aeb6http%3A%2F%2Fwww.oalib.com%2Fpaper%2F2158338refpaperuri:(874f860fe272a31e299223f3f03c7a1c)http://www.oalib.com/paper/2158338The Parallel Offline Radiative Transfer (PORT) model is a stand-alone tool, driven by model-generated datasets, that can be used for any radiation calculation that the underlying radiative transfer schemes can perform, such as diagnosing radiative forcing. In its present distribution, PORT isolates the radiation code from the Community Atmosphere Model (CAM4) in the Community Earth System Model (CESM1). The current configuration focuses on CAM4 radiation with the constituents as represented in present-day conditions in CESM1, along with their optical properties. PORT includes an implementation of stratospheric temperature adjustment under the assumption of fixed dynamical heating, which is necessary to compute radiative forcing in addition to the more straightforward instantaneous radiative forcing. PORT can be extended to use radiative constituent distributions from other models or model simulations. Ultimately, PORT can be used with various radiative transfer models. As illustrations of the use of PORT, we perform the computation of radiative forcing from doubling of carbon dioxide, from the change of tropospheric ozone concentration from the year 1850 to 2000, and from present-day aerosols. The radiative forcing from tropospheric ozone (with respect to 1850) generated by a collection of model simulations under the Atmospheric Chemistry and Climate Model Intercomparison Project is found to be 0.34 (with an intermodel standard deviation of 0.07) W m(-2). Present-day aerosol direct forcing (relative to no aerosols) is found to be -1.3 W m(-2).
    Crutzen P. J., 1974: Photochemical reactions initiated by and influencing ozone in unpolluted tropospheric air. Tellus, 26, 47- 57.10.1111/j.2153-3490.1974.tb01951.x5bf2b27965bbe0738db5166c079daacdhttp%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1111%2Fj.2153-3490.1974.tb01951.x%2Ffullhttp://onlinelibrary.wiley.com/doi/10.1111/j.2153-3490.1974.tb01951.x/fullABSTRACT This paper presents theoretical arguments in favour of OH-concentrations larger than 10 6 molecules cm 613 in the sunlit lower troposphere even if allowance is made for heterogeneous removal of OH, HO 2 and HNO 3 molecules. The OH-concentrations, presented in this paper, were calculated considering for the first time the photochemical effect of both scattered and direct radiation at ground levels and adopting recent accurate data for the quantum efficiency of O( 1 D) production in the ozone photolysis near 310 nm. The significant role played by OH in the atmospheric carbon, nitrogen and possibly sulphur cycles is discussed. Low background mixing ratios of NO x molecules (< 10 619 ) in the unpolluted atmosphere are calculated. The oxidation of NH 3 , initiated by the reaction with OH, may provide a significant source of tropospheric NO x -molecules, if its rate constant is about 10 6113 cm 3 s 611 near the ground. The conversion of NO 2 into HNO 3 , followed by heterogeneous removal of HNO 3 , is the most important tropospheric sink for NO x -molecules. The photodissociation of ozone in ultraviolet light between 300 and 330 nm, which leads to the formation of the excited O( 1 D) atom, “drives” several sequences of reactions treated in this study. Several chains of reactions, involving carbon and nitrogen compounds, lead to large rates of formation and destruction of ozone in the troposphere. These rates partly balance each other. Whether there is a net production or destruction of ozone in the troposphere cannot be determined at present. Ozone is a very active, catalytic component in the tropospheric chemical systems. Globally, the combustion source of CO for the year 1970 is more than 20% of the natural source of CO as provided by the oxidation of biologically produced CH 4 . For middle latitudes of the Northern Hemisphere the combustion source is about equal to the natural source. However, too little is known about homogeneous and heterogeneous reactions affecting the methane oxidation products.
    Derwent R. G., M. E. Jenkin, and S. M. Saunders, 1996: Photochemical ozone creation potentials for a large number of reactive hydrocarbons under European conditions. Atmos. Environ., 30, 181- 199.10.1016/1352-2310(95)00303-G7b97ad403c1d077ac0bdb1e17c21b5dahttp%3A%2F%2Fwww.sciencedirect.com%2Fscience%2Farticle%2Fpii%2F135223109500303Ghttp://www.sciencedirect.com/science/article/pii/135223109500303GA photochemical trajectory model is used to describe the ozone production from the oxidation of methane and 95 other hydrocarbons in the presence of sunlight and NOin air parcels advected across north west Europe towards the British Isles. By adding a small additional mass emission of each hydrocarbon in turn, additional ozone production was stimulated. A photochemical ozone creation potential (POCP) index was generated from the model results showing the relative importance of each hydrocarbon in ozone formation, on a mass emitted basis. Aromatic and olefinic hydrocarbons showed the highest POCP values with halocarbons the lowest. Using the POCP index, motor vehicle exhaust is seen to exhibit the highest ozone-forming potential of all the hydrocarbon emission source categories evaluated. Toluene, -butane, ethylene and the xylenes, alone, account for over one third of the ozone forming potential of European emissions. Certain hydrocarbons, including acetone and methyl acetate, show significantly lower POCPs and have considerable potential as candidates for substitution in industrial or chemical processes and as solvents.
    Forster P., Coauthors, 2007: Changes in atmospheric constituents and in radiative forcing. Chapter 2. Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, Intergovernmental Panel on Climate Change, Ed., Cambridge University Press.933127c5dda06d2497fd85aba324b609http%3A%2F%2Fcore.ac.uk%2Fdisplay%2F23498085http://core.ac.uk/display/23498085Archer, D., 2007: Methane hydrate stability and anthropogenic
    Fowler D., Coauthors, 2009: Atmospheric composition change: Ecosystems-Atmosphere interactions. Atmos. Environ., 43, 5193- 5267.10.1016/j.atmosenv.2009.07.0686ef0de17-7a9a-45fa-b011-54dd69791ee90802239d2fb9f26da2c941ee0c065df7http%3A%2F%2Fwww.sciencedirect.com%2Fscience%2Farticle%2Fpii%2FS1352231009006633refpaperuri:(9fa3ce0f2e9d23673dfbb5b0c5e6135e)http://www.sciencedirect.com/science/article/pii/S1352231009006633Some important developments of the science have been applied to assist in addressing policy questions, which have been the main driver of the research agenda, while other developments in understanding have not been applied to their wider field especially in chemistry-transport models through deficiencies in obtaining appropriate data to enable application or inertia within the modelling community. The paper identifies applications, gaps and research questions that have remained intractable at least since 2000 within the specialized sections of the paper, and where possible these have been focussed on research questions for the coming decade.
    Gao L. J., M. G. Zhang, and Z. W. Han, 2009: Model analysis of seasonal variations in tropospheric ozone and carbon monoxide over East Asia. Adv. Atmos. Sci.,26, 312-318, doi: 10.1007/s00376-009-0312-9.10.1007/s00376-009-0312-97f785aaa861697f93acaa5863f243d33http%3A%2F%2Flink.springer.com%2F10.1007%2Fs00376-009-0312-9http://d.wanfangdata.com.cn/Periodical_dqkxjz-e200902014.aspxTemporal-spatial variations in tropospheric ozone concentrations over East Asia in the period from 1 January 2000 to 31 December 2004 were simulated by using the Models-3 Community Multi-scale Air Quality (CMAQ) modeling system with meteorological fields calculated by the Regional Atmospheric Modeling System (RAMS). The simulated concentrations of ozone and carbon monoxide were compared with ground level observations at two remote sites, Ryori (39.03°N, 141.82°E) and Yonagunijima (24.47°N, 123.02°E). The comparison shows that the model reproduces their seasonal variation patterns reasonably well, and simulated ozone levels are generally in good agreement with the observed ones, but carbon monoxide concentrations are underestimated. Analysis of horizontal distributions of monthly averaged ozone mixing ratios in the surface layer indicates that ozone concentrations have noticeable differences among the four seasons; they are generally higher in the spring and summer while lower in the winter, reflecting the seasonal variation of solar intensity and photochemical activity and the fact that the monsoons over East Asia are playing an important role in ozone distributions.
    Heath D. F., A. J. Krueger, H. A. Roeder, and B. D. Henderson, 1975: The solar backscatter ultraviolet and total ozone mapping spectrometer (SBUV/TOMS) for NIMBUS G. Optical Engineering, 14, 323- 331.
    Hsu J., M. J. Prather, 2009: Stratospheric variability and tropospheric ozone. J. Geophys. Res.: Atmos.,114(D6), doi: 10.1029/2008JD010942.10.1029/2008JD01094222f454483046b3228bf2673cd6b9d3cbhttp%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2F2008JD010942%2Fpdfhttp://onlinelibrary.wiley.com/doi/10.1029/2008JD010942/pdfChanges in the stratosphere-troposphere exchange (STE) of ozone over the last few decades have altered the tropospheric ozone abundance and are likely to continue doing so in the coming century as climate changes. Combining an updated linearized stratospheric ozone chemistry (Linoz v2) with parameterized polar stratospheric clouds (PSCs) chemistry, a 5-year (2001-2005) sequence of the European Centre for Medium-Range Weather Forecasts (ECMWF) meteorology data, and the University of California, Irvine (UCI) chemistry transport model (CTM), we examined variations in STE Oflux and how it perturbs tropospheric O. Our estimate for the current STE ozone flux is 290 Tg/a in the Northern Hemisphere (NH) and 225 Tg/a in the Southern Hemisphere (SH). The 2001-2005 interannual root-mean-square (RMS) variability is 25 Tg/a for the NH and 30 Tg/a for the SH. STE drives a seasonal peak-to-peak NH variability in tropospheric ozone of about 7-8 Dobson unit (DU). Of the interannual STE variance, 20% and 45% can be explained by the quasi-biennial oscillation (QBO) in the NH and SH, respectively. The CTM matches the observed QBO variations in total column ozone, and the STE Oflux shows negative anomalies over the midlatitudes during the easterly phases of the QBO. When the observed column ozone depletion from 1979 to 2004 is modeled with Linoz v2, we predicted STE reductions of at most 10% in the NH, corresponding to a mean decrease of 1 ppb in tropospheric O.
    Hurrell J. W., J. J. Hack, D. Shea, J. M. Caron, and J. Rosinski, 2008: A new sea surface temperature and sea ice boundary dataset for the community atmosphere model. J.Climate, 21, 5145- 5153.0ff603cbc3bfb3d5101e80534d7908a6http%3A%2F%2Ficesjms.oxfordjournals.org%2Fexternal-ref%3Faccess_num%3D10.1175%2F2008JCLI2292.1%26link_type%3DDOIhttp://icesjms.oxfordjournals.org/external-ref?access_num=10.1175/2008JCLI2292.1&amp;link_type=DOI
    Isaksen, I. S. A., Coauthors, 2009: Atmospheric composition change: Climate-Chemistry interactions. Atmos. Environ., 43, 5138- 5192.10.1016/j.atmosenv.2009.08.003f6f00f11-b4b4-45b8-8630-e94686a633f7468e5c79de21c210facc06e7cda3a876http%3A%2F%2Fwww.sciencedirect.com%2Fscience%2Farticle%2Fpii%2FS1352231009006943refpaperuri:(2ebab25734d855fd38d0f3cae625a90a)http://www.sciencedirect.com/science/article/pii/S1352231009006943Chemically active climate compounds are either primary compounds like methane (CH 4 ), removed by oxidation in the atmosphere, or secondary compounds like ozone (O 3 ), sulfate and organic aerosols, both formed and removed in the atmosphere. Man-induced climate-hemistry interaction is a two-way process: Emissions of pollutants change the atmospheric composition contributing to climate change through the aforementioned climate components, and climate change, through changes in temperature, dynamics, the hydrological cycle, atmospheric stability, and biosphere-atmosphere interactions, affects the atmospheric composition and oxidation processes in the troposphere. Here we present progress in our understanding of processes of importance for climate-hemistry interactions, and their contributions to changes in atmospheric composition and climate forcing. A key factor is the oxidation potential involving compounds like O 3 and the hydroxyl radical (OH). Reported studies represent both current and future changes. Reported results include new estimates of radiative forcing based on extensive model studies of chemically active climate compounds like O 3 , and of particles inducing both direct and indirect effects. Through EU projects like ACCENT, QUANTIFY, and the AeroCom project, extensive studies on regional and sector-wise differences in the impact on atmospheric distribution are performed. Studies have shown that land-based emissions have a different effect on climate than ship and aircraft emissions, and different measures are needed to reduce the climate impact. Several areas where climate change can affect the tropospheric oxidation process and the chemical composition are identified. This can take place through enhanced stratospheric-ropospheric exchange of ozone, more frequent periods with stable conditions favoring pollution build up over industrial areas, enhanced temperature induced biogenic emissions, methane releases from permafrost thawing, and enhanced concentration through reduced biospheric uptake. During the last 5-10 years, new observational data have been made available and used for model validation and the study of atmospheric processes. Although there are significant uncertainties in the modeling of composition changes, access to new observational data has improved modeling capability. Emission scenarios for the coming decades have a large uncertainty range, in particular with respect to regional trends, leading to a significant uncertainty range in estimated regional composition changes and climate impact.
    Johnson C. E., D. S. Stevenson, W. J. Collins, and R. G. Derwent, 2001: Role of climate feedback on methane and ozone studied with a coupled ocean-atmosphere-chemistry model. Geophys. Res. Lett., 28, 1723- 1726.
    Kim J. H., H. Lee, 2010: What causes the springtime tropospheric ozone maximum over Northeast Asia? Adv. Atmos. Sci.,27, 543-551, doi: 10.1007/s00376-009-9098-z.10.1007/s00376-009-9098-z1cf1c483fce403096227b8847da128d7http%3A%2F%2Fd.wanfangdata.com.cn%2FPeriodical_dqkxjz-e201003007.aspxhttp://d.wanfangdata.com.cn/Periodical_dqkxjz-e201003007.aspxScientists have long debated the relative importance of tropospheric photochemical production versus stratospheric influx as causes of the springtime tropospheric ozone maximum over northern mid-latitudes. This paper investigates whether or not stratospheric intrusion and photochemistry play a significant role in the springtime ozone maximum over Northeast Asia, where ozone measurements are sparse. We examine how tropospheric ozone seasonalities over Naha (26oN, 128oE), Kagoshima (31oN, 131oE), and Pohang (36oN, 129oE), which are located on the same meridional line, are related to the timing and location of the jet stream. The ozone seasonality shows a gradual increase from January to the maximum ozone month, which corresponds to April at Naha, May at Kagoshima, and June at Pohang. In order to examine the occurrence of stratospheric intrusion, we analyze a correlation between jet stream activity and tropospheric ozone seasonality. From these analyses, we did not find any favorable evidence supporting the hypothesis that the springtime enhancement may result from stratospheric intrusion. According to trajectory analysis for vertical and horizontal origins of the airmass, a gradual increasing tendency in ozone amounts from January until the onset of monsoon was similar to the increasing ozone formation tendency from winter to spring over mainland China, which has been observed during the build-up of tropospheric ozone over Central Europe in the winter--spring transition period due to photochemistry. Overall, the analyses suggest that photochemistry is the most important contributor to observed ozone seasonality over Northeast Asia.
    Kristjánsson, J. E., T. Iversen, A. Kirkevg, . Seland, J. Debernard, 2005: Response of the climate system to aerosol direct and indirect forcing: Role of cloud feedbacks. J. Geophys. Res.: Atmos.,110(D24), doi: 10.1029/ 2005JD006299.10.1029/2005JD006299b31e7e4dfcdd9fe22ecb7899ccd66047http%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2F2005JD006299%2Ffullhttp://onlinelibrary.wiley.com/doi/10.1029/2005JD006299/fullIn this study, the response of the climate system to aerosol direct and indirect radiative forcing is investigated. Several multidecadal equilibrium simulations are carried out, using the NCAR CCM3 framework coupled to a separately developed aerosol treatment. The aerosol treatment includes, e.g., a life cycle scheme for particulate sulfate and black carbon (natural and anthropogenic), calculations of aerosol size distributions and CCN activation, as well as computations of direct and indirect forcing (1st and 2nd indirect effect). In all the simulations the full aerosol treatment is run online, hence responding interactively to changes in climate. By far the largest response is caused by the indirect forcing, with a globally averaged cooling of -1.25 K due to anthropogenic aerosols. The largest temperature reduction is found in the Northern Hemisphere because of a larger aerosol burden there. As a result of this cooling pattern, the Intertropical Convergence Zone is displaced southward by a few hundred kilometers. Interestingly, a similar, though less significant displacement is also found in the experiments with the direct effect alone, even though the globally averaged aerosol induced cooling is much weaker in that case, i.e., -0.08 K. The direct radiative forcing is much stronger at the surface than at the top of the atmosphere, and this leads to a slight weakening of the hydrological cycle. Comparing simulations with direct and indirect forcing combined to those with indirect and direct forcing separately, a residual, caused by nonlinear model feedbacks, is manifested through a reduction in precipitation. This reduction amounts to -0.5% in a global average and exceeds -2.5% in the Arctic, highlighting the role of high-latitude climate feedbacks. Globally, cloud feedback is negative in the sense that in the colder climate resulting from anthropogenic aerosol forcing, net cloud forcing is reduced by 15% compared to the original climate state. This is caused by a general cloud thinning, especially at high latitudes, while in the most polluted regions, clouds are thicker through the 2nd indirect effect. The 1st indirect effect, on the other hand, remains intact in the presence of climate feedbacks, yielding a similar signature of cloud droplet reduction as in the pure forcing simulations.
    Lacis A. A., D. J. Wuebbles, and J. A. Logan, 1990: Radiative forcing of climate by changes in the vertical distribution of ozone. J. Geophys. Res.: Atmos., 95, 9971- 9981.10.1029/JD095iD07p09971d63114522656b359470c33d4a8ee54d0http%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2FJD095iD07p09971%2Ffullhttp://onlinelibrary.wiley.com/doi/10.1029/JD095iD07p09971/fullWe describe a simple method for evaluating the radiative forcing of surface temperature caused by changes in the vertical distribution of ozone. The method employs a parameterization based on one-dimensional radiative-convective equilibrium calculations; these calculations predict that the surface temperature should warm in response to both decreases in ozone above 30 km and increases in ozone below 30 km. The parameterization is used to investigate the response of surface temperature to observed changes in the vertical distribution of ozone at northern mid-latitudes. We show that the observed ozone trends, taken at face value, suggest a cooling of the surface temperature at northern mid-latitudes during the 1970s equal in magnitude to about half the warming predicted for CO 2 for the same time period. However, the measurement uncertainty of the observed trends is large, with the best estimates for mid-latitude cooling being 610.05±0.05°C. The surface cooling is caused by ozone decreases in the lower stratosphere, which outweigh the warming effects of ozone increases in the troposphere. The results obtained differ from predictions based on one-dimensional photochemical model simulations of ozone trends for the 1970s, which suggest a warming of the surface temperature equal to 6520% of the warming contributed by CO 2 . Also, the ozone decreases observed in the lower stratosphere during the 1970s produce atmospheric cooling by several tenths of a degree in the 12- to 20-km altitude region over the northern mid-latitudes. This temperature decrease is larger than the cooling due to CO 2 and thus may obscure the expected stratospheric CO 2 greenhouse signature.
    Lamarque, J. F., Coauthors, 2010: Historical (1850-2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols: methodology and application. Atmospheric Chemistry and Physics, 10, 7017- 7039.
    Lamarque, J. F., Coauthors, 2013: The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Overview and description of models, simulations and climate diagnostics. Geoscientific Model Development, 6, 179- 206.10.5194/gmd-6-179-201360311e1c323b07af3409fb93a43cf18dhttp%3A%2F%2Fwww.oalib.com%2Fpaper%2F1376958http://www.oalib.com/paper/1376958The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) consists of a series of time slice experiments targeting the long-term changes in atmospheric composition between 1850 and 2100, with the goal of documenting composition changes and the associated radiative forcing. In this overview paper, we introduce the ACCMIP activity, the various simulations performed (with a requested set of 14) and the associated model output. The 16 ACCMIP models have a wide range of horizontal and vertical resolutions, vertical extent, chemistry schemes and interaction with radiation and clouds. While anthropogenic and biomass burning emissions were specified for all time slices in the ACCMIP protocol, it is found that the natural emissions are responsible for a significant range across models, mostly in the case of ozone precursors. The analysis of selected present-day climate diagnostics (precipitation, temperature, specific humidity and zonal wind) reveals biases consistent with state-of-the-art climate models. The modelto- model comparison of changes in temperature, specific humidity and zonal wind between 1850 and 2000 and between 2000 and 2100 indicates mostly consistent results. However, models that are clear outliers are different enough from the other models to significantly affect their simulation of atmospheric chemistry.
    Lin L., Q. Fu, H. Zhang, J. Su, Q. Yang, and Z. Sun, 2013: Upward mass fluxes in tropical upper troposphere and lower stratosphere derived from radiative transfer calculations. Journal of Quantitative Spectroscopy and Radiative Transfer, 117, 114- 122.10.1016/j.jqsrt.2012.11.016a2d86d4b553ecf570d0ad779916c5034http%3A%2F%2Fwww.sciencedirect.com%2Fscience%2Farticle%2Fpii%2FS0022407312005225http://www.sciencedirect.com/science/article/pii/S0022407312005225Yang et al. [1] quantified vertical velocity and upward mass fluxes in tropical lower stratosphere based on radiative heating rate calculations using the Fu-Liou radiation model along with 8-year Southern Hemisphere Additional Ozonesondes balloon-borne measurements of temperature and ozone and cryogenic frost-point hygrometer measured water vapor. The impact of tropospheric clouds on stratospheric heating rates was considered using cloud distributions from the International Satellite Cloud Climatology Project. Since the radiative heating rate in the lower stratosphere can be as small as 0.1–0.202K/day, an accurate radiative heating rate calculation including all radiatively active species is required. In this paper, we revisit the calculations in Yang et al. [1] by developing a line-by-line radiative transfer model (LBLRTM-D4S) for multiple scattering atmospheres. We consider the cloud impact using the cloud fields based on active lidar and radar observations from CALIPSO and CloudSat so that the quantification of upward mass fluxes in tropical lower stratosphere can be extended to tropical upper troposphere. The annual mean mass fluxes and vertical velocities from LBLRTM-D4S are 651402kg02m 612 day 611 and 0.7702mm02s 611 , respectively, at 12002hPa (15.502km), and 651.202kg02m 612 day 611 and 0.1302mm02s 611 at 6002hPa (19.502km). We examine the accuracy of three commonly used efficient radiation models including Fu-Liou, RRTM, and SBDART in estimating tropical upward mass fluxes against the LBLRTM-D4S results.
    Liu C. X., Y. Liu, Z. N. Cai, S. T. Gao, J. C. Bian, X. Liu, and K. Chance, 2010: Dynamic formation of extreme ozone minimum events over the Tibetan Plateau during northern winters 1987-2001. J. Geophys. Res.: Atmos. ,115(D18), doi:10.1029/2009JD013130.10.1029/2009JD01313029c99e74eb44c3129e7b3cdd14374b07http%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2F2009JD013130%2Fcitedbyhttp://onlinelibrary.wiley.com/doi/10.1029/2009JD013130/citedbyWintertime extreme ozone minima in the total column ozone over the Tibetan Plateau (TP) between 1978 and 2001 are analyzed using observations from the Total Ozone Mapping Spectrometer (TOMS), Global Ozone Monitoring Experiment (GOME), and reanalysis data from both National Centers for Environmental Prediction and European Centre for Medium-Range Weather Forecasts. Results show that total column ozone reduction in nine persistent (lasting for at least 2 days) and four transient events can be substantially attributed to ozone reduction in the upper troposphere and lower stratosphere region (below 25 km). This reduction is generally caused by uplift of the local tropopause and northward transport of tropical ozone-poor air associated with an anomalous anticyclone in the upper troposphere. These anticyclonic anomalies are closely related to anomalous tropical deep convective heating, which is, however, not necessarily phase locked with the tropical Madden-Julian Oscillation as in our earlier case study. Considering stratospheric processes, the selected 13 events can be combined into nine independent events. Moreover, five of the nine independent events, especially the persistent events, are coupled with contributions from stratospheric dynamics between 25 and 40 km, i.e., 15%-40% derived from GOME observations for events in November 1998, February 1999, and December 2001. On the basis of these events, stratospheric column ozone reduction over the TP region can be attributed to the dynamics (development and/or displacement) of the two main stratospheric systems, namely, the polar vortex and the Aleutian High. The effect of a "low-ozone pocket" inside the Aleutian High on the total column ozone in East Asia requires further study.
    Liu Y., W.-L. Li, X.-J. Zhou, I.-S.-A. Isaksen, J.-K. Sundet, and J.-H.-He, 2003: The possible influences of the increasing anthropogenic emissions in India on tropospheric ozone and OH. Adv. Atmos. Sci.,20, 968-977, doi: 10.1007/ BF02915520.10.1007/BF029155204209acb6b6d2b642f96450160d278e28http%3A%2F%2Flink.springer.com%2F10.1007%2FBF02915520http://d.wanfangdata.com.cn/Periodical_dqkxjz-e200306012.aspxA 3-D chemical transport model (OSLO CTM2) is used to investigate the influences of the increasing anthropogenic emission in India. The model is capable of reproducing the observational results of the INDOEX experiment and the measurements in summer over India well. The model results show that when Nox and CO emissions in India are doubled, ozone concentration increases, and global average OH decreases a little. Under the effects of the Indian summer monsoon, Nox and CO in India are efficiently transported into the middle and upper troposphere by the upward current and the convective activities so that the Nox, CO, and ozone in the middle and upper troposphere significantly increase with the increasing Nox and CO emissions. These increases extensively influence a part of Asia, Africa, and Europe, and persist from June to September.
    Miyazaki K., H. J. Eskes, K. Sudo, M. Takigawa, M. van Weele and K. F. Boersma, 2012: Simultaneous assimilation of satellite NO2, O3, CO, and HNO3 data for the analysis of tropospheric chemical composition and emissions. Atmos. Chem. Phys., 12, 9545- 9579.
    Myhre G., Coauthors, 2013a: Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations. Atmospheric Chemistry and Physics, 13, 1853- 1877.10.5194/acp-13-1853-2013d673fc74-0d8e-458a-9219-cc86ab0db90aWOS:000315406600010707ccfedd9353d90fd80d00b27a511a5http%3A%2F%2Fwww.oalib.com%2Fpaper%2F1366726refpaperuri:(145d9d8824aace30efe62ab8757d90bb)http://www.oalib.com/paper/1366726We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 16 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from -0.58 to -0.02 Wm(-2), with a mean of -0.27 Wm(-2) for the 16 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of -0.35 Wm(-2). Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study. We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results.
    Myhre G., Coauthors, 2013b: Anthropogenic and natural radiative forcing. Climate Change 2013: The Physical Science Basis. Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, IPCC, Ed., Cambridge University Press.
    Nakajima T., A. Higurashi, K. Kawamoto, and J. Penner, 2000: A possible correlation between satellite-derived cloud and aerosol microphysical parameters. Geophys. Res. Lett., 28: 1171- 1174.e87624a1a85a4376095294db1e0a6441http%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2F2000GL012186%2Fpdf/s?wd=paperuri%3A%28609de6e512963f152078fd1d5ed6dca8%29&filter=sc_long_sign&tn=SE_xueshusource_2kduw22v&sc_vurl=http%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2F2000GL012186%2Fpdf&ie=utf-8&sc_us=1332370395424549545
    Pincus R., H. W. Barker, and J. J. Morcrette, 2003: A fast, flexible, approximate technique for computing radiative transfer in inhomogeneous cloud fields. J. Geophys. Res.: Atmos.,108(D13), doi: 10.1029/2002JD003322.10.1029/2002JD003322b92efa2ddaeb39c1411c1efff8edb8d1http%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2F2002JD003322%2Freferenceshttp://onlinelibrary.wiley.com/doi/10.1029/2002JD003322/referencesCiteSeerX - Scientific documents that cite the following paper: 2003: A fast, flexible, approximate technique for computing radiative transfer in inhomogeneous clouds
    Shindell D., G. Faluvegi, A. Lacis, J. Hansen, R. Ruedy, and E. Aguilar, 2006: Role of tropospheric ozone increases in 20th-century climate change. J. Geophys. Res., 111, D08302.10.1029/2005JD00634821898423dc5c6b81fd42d3d6a8851ad3http%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2F2005JD006348%2Fpdfhttp://onlinelibrary.wiley.com/doi/10.1029/2005JD006348/pdfCiteSeerX - Scientific documents that cite the following paper: The role of tropospheric ozone increases in 20th century climate change
    Shindell D., Coauthors, 2013: Attribution of historical ozone forcing to anthropogenic emissions. Nature Climate Change, 3, 567- 570.10.1038/nclimate1835b1b03b65550ce04546051ef1b7cdc6cdhttp%3A%2F%2Fwww.nature.com%2Fnclimate%2Fjournal%2Fv3%2Fn6%2Ffull%2Fnclimate1835.htmlhttp://www.nature.com/nclimate/journal/v3/n6/full/nclimate1835.htmlAnthropogenic ozone radiative forcing is traditionally separately attributed to tropospheric and stratospheric changes assuming that these have distinct causes. Using the interactive composition-climate model GISS-E2-R we find that this assumption is not justified. Our simulations show that changes in emissions of tropospheric ozone precursors have substantial effects on ozone in both regions, as do anthropogenic halocarbon emissions. On the basis of our results, further simulations with the NCAR-CAM3.5 model, and published studies, we estimate industrial era (1850-2005) whole-atmosphere ozone forcing of ~0.5Wmdue to anthropogenic tropospheric precursors and about -0.2Wmdue to halocarbons. The net troposphere plus stratosphere forcing is similar to the net halocarbon plus precursor ozone forcing, but the latter provides a more useful perspective. The halocarbon-induced ozone forcing is roughly two-thirds the magnitude of the halocarbon direct forcing but opposite in sign, yielding a net forcing of only ~0.1Wm. Thus, the net effect of halocarbons has been smaller, and the effect of tropospheric ozone precursors has been greater, than generally recognized.
    Skeie R. B., T. K. Berntsen, G. Myhre, K. Tanaka, M. M. Kvalevg, and C. R. Hoyle, 2011: Anthropogenic radiative forcing time series from pre-industrial times until 2010. Atmospheric Chemistry and Physics, 11, 11 827- 11 857.10.5194/acpd-11-22545-20112fd87e095248d231eaaa14d2318c41d8http%3A%2F%2Fwww.oalib.com%2Fpaper%2F2696244http://www.oalib.com/paper/2696244In order to use knowledge of past climate change to improve our understanding of the sensitivity of the climate system, detailed knowledge about the time development of radiative forcing (RF) of the earth atmosphere system is crucial. In this study, time series of anthropogenic forcing of climate from pre-industrial times until 2010, for all well established forcing agents, are estimated. This includes presentation of RF histories of well mixed greenhouse gases, tropospheric ozone, direct- and indirect aerosol effects, surface albedo changes, stratospheric ozone and stratospheric water vapour. For long lived greenhouse gases, standard methods are used for calculating RF, based on global mean concentration changes. For short lived climate forcers, detailed chemical transport modelling and radiative transfer modelling using historical emission inventories is performed. For the direct aerosol effect, sulphate, black carbon, organic carbon, nitrate and secondary organic aerosols are considered. For aerosol indirect effects, time series of both the cloud lifetime effect and the cloud albedo effect are presented. Radiative forcing time series due to surface albedo changes are calculated based on prescribed changes in land use and radiative transfer modelling. For the stratospheric components, simple scaling methods are used. Long lived greenhouse gases (LLGHGs) are the most important radiative forcing agent with a RF of 2.83 0.28 W min year 2010 relative to 1750. The two main aerosol components contributing to the direct aerosol effect are black carbon and sulphate, but their contributions are of opposite sign. The total direct aerosol effect was -0.48 0.14 W min year 2010. Since pre-industrial times the RF of LLGHGs has been offset by the direct and indirect aerosol effects, especially in the second half of the 20th century, which possibly lead to a decrease in the total anthropogenic RF in the middle of the century. We find a total anthropogenic RF in year 2010 of 1.4 W m. However, the uncertainties in the negative RF from aerosols are large, especially for the cloud lifetime effect.
    Svde O. A., C. R. Hoyle, G. Myhre, and I. S. A. Isaksen, 2011: The HNO3 forming branch of the HO2 + NO reaction: Pre-industrial-to-present trends in atmospheric species and radiative forcings. Atmospheric Chemistry and Physics, 11, 8929- 8943.
    Stevenson, D. S., Coauthors, 2006: Multimodel ensemble simulations of present-day and near-future tropospheric ozone. J. Geophys. Res.: Atmos. (1984-2012), 111( D8), D08301.10.1029/2005JD00633883ec1eb542ffdbbaa178e296674ce44dhttp%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2F2005JD006338%2Fcitedbyhttp://onlinelibrary.wiley.com/doi/10.1029/2005JD006338/citedbyGlobal tropospheric ozone distributions, budgets, and radiative forcings from an ensemble of 26 state-of-the-art atmospheric chemistry models have been intercompared and synthesized as part of a wider study into both the air quality and climate roles of ozone. Results from three 2030 emissions scenarios, broadly representing “optimistic,” “likely,” and “pessimistic” options, are compared to a base year 2000 simulation. This base case realistically represents the current global distribution of tropospheric ozone. A further set of simulations considers the influence of climate change over the same time period by forcing the central emissions scenario with a surface warming of around 0.7K. The use of a large multimodel ensemble allows us to identify key areas of uncertainty and improves the robustness of the results. Ensemble mean changes in tropospheric ozone burden between 2000 and 2030 for the 3 scenarios range from a 5% decrease, through a 6% increase, to a 15% increase. The intermodel uncertainty (±1 standard deviation) associated with these values is about ±25%. Model outliers have no significant influence on the ensemble mean results. Combining ozone and methane changes, the three scenarios produce radiative forcings of 6150, 180, and 300 mW m612, compared to a CO2 forcing over the same time period of 800–1100 mW m612. These values indicate the importance of air pollution emissions in short- to medium-term climate forcing and the potential for stringent/lax control measures to improve/worsen future climate forcing. The model sensitivity of ozone to imposed climate change varies between models but modulates zonal mean mixing ratios by ±5 ppbv via a variety of feedback mechanisms, in particular those involving water vapor and stratosphere-troposphere exchange. This level of climate change also reduces the methane lifetime by around 4%. The ensemble mean year 2000 tropospheric ozone budget indicates chemical production, chemical destruction, dry deposition and stratospheric input fluxes of 5100, 4650, 1000, and 550 Tg(O3) yr611, respectively. These values are significantly different to the mean budget documented by the Intergovernmental Panel on Climate Change (IPCC) Third Assessment Report (TAR). The mean ozone burden (340 Tg(O3)) is 10% larger than the IPCC TAR estimate, while the mean ozone lifetime (22 days) is 10% shorter. Results from individual models show a correlation between ozone burden and lifetime, and each model's ozone burden and lifetime respond in similar ways across the emissions scenarios. The response to climate change is much less consistent. Models show more variability in the tropics compared to midlatitudes. Some of the most uncertain areas of the models include treatments of deep tropical convection, including lightning NO x production; isoprene emissions from vegetation and isoprene's degradation chemistry; stratosphere-troposphere exchange; biomass burning; and water vapor concentrations.
    Stevenson, D. S., Coauthors, 2013: Tropospheric ozone changes,radiative forcing and attribution to emissions in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). Atmos. Chem. Phys., 13, 3063- 3085.
    Stohl, A., Coauthors, 2003: Stratosphere-troposphere exchange: A review, and what we have learned from staccato. J. Geophys. Res.: Atmos. (1984-2012),108(D12), doi: 10.1029/ 2002JD002490.10.1029/2002JD0024909f48eee307e345ac62dfa729e7dc0e9ahttp%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2F2002JD002490%2Ffullhttp://onlinelibrary.wiley.com/doi/10.1029/2002JD002490/full[1] This paper provides a review of stratosphere-troposphere exchange (STE), with a focus on processes in the extratropics. It also addresses the relevance of STE for tropospheric chemistry, particularly its influence on the oxidative capacity of the troposphere. After summarizing the current state of knowledge, the objectives of the project Influence of Stratosphere-Troposphere Exchange in a Changing Climate on Atmospheric Transport and Oxidation Capacity (STACCATO), recently funded by the European Union, are outlined. Several papers in this Journal of Geophysical Research - Atmospheres special section present the results of this project, of which this paper gives an overview. STACCATO developed a new concept of STE in the extratropics, explored the capacities of different types of methods and models to diagnose STE, and identified their various strengths and shortcomings. Extensive measurements were made in central Europe, including the first monitoring over an extended period of time of beryllium-10 ( 10 Be), to provide a suitable database for case studies of stratospheric intrusions and for model validation. Photochemical models were used to examine the impact of STE on tropospheric ozone and the oxidizing capacity of the troposphere. Studies of the present interannual variability of STE and projections into the future were made using reanalysis data and climate models.
    Stordal, F., Coauthors, 2003: Climate impact of tropospheric ozone changes. Ozone-Climate Interactions, I. S. A. Isaksen, Ed., European Commission Air Pollution research report No. 81.1b7fb390ca7e601ea47ed2a2e3e973e4http%3A%2F%2Fadsabs.harvard.edu%2Fabs%2F2013PhDT.......281Lhttp://adsabs.harvard.edu/abs/2013PhDT.......281LTropospheric ozone (O) is one of the most important trace gases in the atmosphere as it plays an important role in atmospheric chemistry, climate and air quality. The changed climate and stratosphere Ohave great potential impact on tropospheric Owhich could lead broad environmental impacts. We carried out modelling study to investigate: (1) The tropospheric Oresponse to past changes in GHGs and ODSs, (2) The tropospheric Oresponse to stratospheric Ochange through UV and STE pathway and (3) The response of summer cyclone to climate change.
    Veefkind J. P., J. F. de Haan, E. J. Brinksma, M. Kroon, and P. F. Levelt, 2006: Total ozone from the ozone monitoring instrument (OMI) using the DOAS technique. IEEE Trans. Geosci. Remote Sens., 44( 5), 1239- 1244.10.1109/TGRS.2006.871204d2c0cfadfdfde5b39182f28317eb4db9http%3A%2F%2Fieeexplore.ieee.org%2Fxpls%2Fabs_all.jsp%3Farnumber%3D1624602http://ieeexplore.ieee.org/xpls/abs_all.jsp?arnumber=1624602Not Available
    Wang Z.-L., H. Zhang, X.-W. Jing, and X.-D. Wei, 2013a: Effect of non-spherical dust aerosol on its direct radiative forcing. Atmos. Res.,120-121, 112- 126.10.1016/j.atmosres.2012.08.006c42f6374-aa7a-499e-baa0-345a4092571b03333671976803f2c8bca19731964428http%3A%2F%2Fwww.sciencedirect.com%2Fscience%2Farticle%2Fpii%2FS0169809512002736refpaperuri:(dabf303ce334e72b4a80ec7138afb390)http://cpfd.cnki.com.cn/Article/CPFDTOTAL-ZGQX201209005054.htmThe optical properties of spherical and non-spherical dust aerosols are calculated using the Lorenz-Mie theory and the combination of T-matrix method and an improved geometric optics method.The resulting optical properties are then applied in an interactive system that coupled a general circulation model with an aerosol model to quantitatively analyze the effect of non-spherical dust aerosol on its direct radiative forcing(DRF).Our results show that the maximum difference in dust instantaneous radiative forcing(IRF) between spherical and non-spherical particles is 0.27 W m-2 at the top of the atmosphere(TOA) and appears over the Sahara Desert due to enhanced absorption of solar radiation by non-spherical dust.The global annual means of shortwave(longwave) IRFs due to spherical and non-spherical dust aerosols at the TOA for all sky are-0.62(0.074) W m-2 and-0.61(0.073) W m-2,respectively,and the corresponding values for clear sky are-1.16(0.092) W m-2 and-1.14(0.093) W m-2,which indicates that the non-spherical effect of dust has almost no effect on their global annual mean IRFs.However,non-spherical dust displays more evident influences than above on its atmospheric-and land-temperature adjusted radiative forcing(ARF) at the TOA over the Saharan Desert,West Asia,and northern China,with an approximate maximum increase of 3.0 and decrease of 0.5 W m-2.The global annual means of shortwave(longwave) ARFs due to spherical and non-spherical dust aerosols are-0.55(0.052) W m-2 and-0.48(0.049) W m-2 at the TOA for all sky,respectively,and the corresponding values for clear sky are-1.07(0.066) W m-2 and-0.95(0.062) W m-2.All ARFs of dust become much weaker than their corresponding IRFs.The absolute values of annual mean ARF for non-spherical dust are approximately 13%(11.2%) and 6%(6%) less than those of spherical dust for the shortwave and longwave for all sky(clear sky),respectively.The results indicate that the non-spherical effect of dust can reduce their ARFs more obviously than do their IRFs.
    Wang Z.-L., H. Zhang, J.-N. Li, X.-W. Jing, and P. Lu, 2013b: Radiative forcing and climate response due to the presence of black carbon in cloud droplets. J. Geophys. Res.: Atmos., 118, 3662- 3675.10.1002/jgrd.50312037024cd585836b3533bba8040a9c7d1http%3A%2F%2Fcpfd.cnki.com.cn%2FArticle%2FCPFDTOTAL-ZGQX201409001003.htmhttp://cpfd.cnki.com.cn/Article/CPFDTOTAL-ZGQX201409001003.htm[1]Optical properties of clouds containing black carbon(BC)particles in their water droplets are calculated by using the Maxwell Garnett mixing rule and Mie theory.The obtained cloud optical properties were then applied to an interactive system by coupling an aerosol model with a General Circulation Model.This system is used to investigate the radiative forcing and the equilibrium climate response due to BC in cloud droplets.The simulated global annual mean radiative forcing at the top of the atmosphere due to the BC in cloud droplets is found to be 0.086 W m 2.Positive radiative forcing can be seen in Africa,South America,East and South Asia,and West Europe,with a maximum value of1.5 W m 2being observed in these regions.The enhanced cloud absorption is shown to increase the global annual mean values of solar heating rate,water vapor,and temperature,but to decrease the global annual mean cloud fraction.Finally,the global annual mean surface temperature is shown to increase by+0.08 K.The local maximum changes are found to be as low as 1.5 K and as high as+0.6 K.We show there has been a significant difference in surface temperature change in the Southern and Northern Hemisphere(+0.19 K and 0.04 K,respectively).Our results show that this interhemispheric asymmetry in surface temperature change could cause a corresponding change in atmospheric dynamics and precipitation.It is also found that the northern trade winds are enhanced in the Intertropical Convergence Zone(ITCZ).This results in northerly surface wind anomalies which cross the equator to converge with the enhanced southern trade winds in the tropics of Southern Hemisphere.This is shown to lead to an increase(a decrease)of vertical ascending motion and precipitation on the south(north)side of the equator,which could induce a southward shift in the tropical rainfall maximum related to the ITCZ.
    Wang Z. L., H. Zhang , and X. Y. Zhang, 2014: Black carbon reduction will weaken the aerosol net cooling effect. Atmos. Chem. Phys. Discuss,14, 33 117-33 141, doi: 10.5194/acpd-14-33117-2014.0d22490f491c03d1766ca6127434bf4dhttp%3A%2F%2Fadsabs.harvard.edu%2Fabs%2F2014ACPD...1433117W/s?wd=paperuri%3A%2857823dd94664cd4c7ac6373315411ab1%29&filter=sc_long_sign&tn=SE_xueshusource_2kduw22v&sc_vurl=http%3A%2F%2Fadsabs.harvard.edu%2Fabs%2F2014ACPD...1433117W&ie=utf-8&sc_us=10522755533932871014
    Wang Z. L., H. Zhang, and X. Y. Zhang, 2015: Simultaneous reductions in emissions of black carbon and co-emitted species will weaken the aerosol net cooling effect, Atmos. Chem. Phys., 15( 7), 3671- 3685.2905f16e66fa7f03c8f0cff9e89b2dbchttp%3A%2F%2Fadsabs.harvard.edu%2Fabs%2F2015acp....15.3671w/s?wd=paperuri%3A%2822cc09cd93f3d8b58b3893a3f575416d%29&filter=sc_long_sign&tn=SE_xueshusource_2kduw22v&sc_vurl=http%3A%2F%2Fadsabs.harvard.edu%2Fabs%2F2015acp....15.3671w&ie=utf-8&sc_us=14334290536011868934
    Wu, T. W., Coauthors, 2010: The Beijing Climate Center atmospheric general circulation model: description and its performance for the present-day climate. Climate Dyn., 34, 123- 147.10.1007/s00382-008-0487-2ed67c5acfd5a67cd1c2a184e1c216ab0http%3A%2F%2Fonlinelibrary.wiley.com%2Fresolve%2Freference%2FXREF%3Fid%3D10.1007%2Fs00382-008-0487-2http://onlinelibrary.wiley.com/resolve/reference/XREF?id=10.1007/s00382-008-0487-2The Beijing Climate Center atmospheric general circulation model version 2.0.1 (BCC_AGCM2.0.1) is described and its performance in simulating the present-day climate is assessed. BCC_AGCM2.0.1 originates from the community atmospheric model version 3 (CAM3) developed by the National Center for Atmospheric Research (NCAR). The dynamics in BCC_AGCM2.0.1 is, however, substantially different from the Eulerian spectral formulation of the dynamical equations in CAM3, and several new physical parameterizations have replaced the corresponding original ones. The major modification of the model physics in BCC_AGCM2.0.1 includes a new convection scheme, a dry adiabatic adjustment scheme in which potential temperature is conserved, a modified scheme to calculate the sensible heat and moisture fluxes over the open ocean which takes into account the effect of ocean waves on the latent and sensible heat fluxes, and an empirical equation to compute the snow cover fraction. Specially, the new convection scheme in BCC_AGCM2.0.1, which is generated from the Zhang and McFarlane- scheme but modified, is tested to have significant improvement in tropical maximum but also the subtropical minimum precipitation, and the modified scheme for turbulent fluxes are validated using EPIC2001 in situ observations and show a large improvement than its original scheme in CAM3. BCC_AGCM2.0.1 is forced by observed monthly varying sea surface temperatures and sea ice concentrations during 1949-2000. The model climatology is compiled for the period 1971-2000 and compared with the ERA-40 reanalysis products. The model performance is evaluated in terms of energy budgets, precipitation, sea level pressure, air temperature, geopotential height, and atmospheric circulation, as well as their seasonal variations. Results show that BCC_AGCM2.0.1 reproduces fairly well the present-day climate. The combined effect of the new dynamical core and the updated physical parameterizations in BCC_AGCM2.0.1 leads to an overall improvement, compared to the original CAM3.
    Xin X. G., T. W. Wu, J. L. Li, Z. Z. Wang, W. P. Li, and F. H. Wu, 2013: How well does BCC_CSM1.1 reproduce the 20th century climate change over China? Atmospheric and Oceanic Science Letters, 6( 1), 21- 26.8aee8a1c-1597-4b69-b80c-28d16cf96e6bmag452220136121d1cbb5cb36fe7603e2aedc3eac55167ahttp%3A%2F%2Fwww.cqvip.com%2FQK%2F89435X%2F201301%2F44519711.htmlhttp://d.wanfangdata.com.cn/Periodical_dqhhykxkb201301004.aspx
    Young, P. J., Coauthors, 2012: Pre-industrial to end 21st century projections of tropospheric ozone from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). Atmospheric Chemistry and Physics Discussions, 12, 21 615- 21 677.10.5194/acp-13-2063-2013d4fc5e596bfdd58aafe37f427390d4a7http%3A%2F%2Fwww.oalib.com%2Fpaper%2F1367894http://www.oalib.com/paper/1367894Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75 %) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337 脗 23 Tg, the ensemble mean burden for 1850 time slice is ~30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: -4% (-16 %) for RCP2.6, 2% (-7 %) for RCP4.5, 1% (-9 %) for RCP6.0, and 7% (18 %) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40-150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A unified approach to ozone budget specifications and a rigorous investigation of the factors that drive tropospheric ozone is recommended to help future studies attribute ozone changes and inter-model differences more clearly.
    Zhang H., T. Nakajima, G. Y. Shi, T. Suzuki, and R. Imasu, 2003: An optimal approach to overlapping bands with correlated k distribution method and its application to radiative calculations. J. Geophys. Res.: Atmos. (1984-2012),108(D20), doi: 10.1029/2002JD003358.10.1029/2002JD0033581300b1423e021ced57675e31d9b06037http%3A%2F%2Fonlinelibrary.wiley.com%2Fdoi%2F10.1029%2F2002JD003358%2Ffullhttp://onlinelibrary.wiley.com/doi/10.1029/2002JD003358/full[1] It is found that the possibly achieved higher accuracy cannot be obtained for all overlapping bands if only one scheme is used to treat them in atmospheric absorption calculations. The commonly used multiplication transmittance scheme is not acceptable when correlation existing in the practical absorption spectra becomes strong. Therefore an optimized scheme to obtain k distribution parameters for overlapping bands is developed in this paper based on the completely uncorrelated, perfectly correlated, and partly correlated schemes. Two partial correlation formulae are given in the paper. Calculations of radiative flux and atmospheric heating (or cooling) rate are validated in detail using a line-by-line model described in the paper for six model atmospheres. The optimized scheme developed here has an accuracy in longwave clear skies of 0.07 K d 611 in the entire troposphere and 0.35 K d 611 above the tropopause; the accuracy of upward, downward, and net fluxes is 0.76 W m 612 at all altitudes. In shortwave region, the absolute errors of the heating rate are less than 0.05 K d 611 in the troposphere and less than 0.25 K d 611 above the tropopause; net flux errors are less than 0.9 W m 612 at all altitudes. For an ensemble of 42 diverse atmospheres, the new scheme guarantees an average maximum error of longwave heating rate of 0.068 K d 611 in troposphere, 0.22 K d 611 above tropopause, and an accuracy of 1.1 W m 612 of radiative net flux for all the levels. For a case of doubled CO 2 concentration, radiative forcing calculations hav
    Zhang M. G., Y. F. Xu, I. Uno, and H. Akimoto, 2004: A numerical study of tropospheric ozone in the springtime in East Asia. Adv. Atmos. Sci.,21, 163-170, doi: 10.1007/BF02915702.10.1007/0-306-47813-7_159cc11791fb4ad483ec6120bc6a284122http%3A%2F%2Fd.wanfangdata.com.cn%2FPeriodical%2Fdqkxjz-e200402002http://d.wanfangdata.com.cn/Periodical/dqkxjz-e200402002The Models-3 Community Multi-scale Air Quality modeling system (CMAQ) coupled with the Regional Atmospheric Modeling System (RAMS) is applied to East Asia to study the transport and photochemical transformation of tropospheric ozone in March 1998. The calculated mixing ratios of ozone and carbon monoxide are compared with ground level observations at three remote sites in Japan and it is found that the model reproduces the observed features very well. Examination of several high episodes of ozone and carbon monoxide indicates that these elevated levels are found in association with continental outflow,demonstrating the critical role of the rapid transport of carbon monoxide and other ozone precursors from the continental boundary layer. In comparison with available ozonesonde data, it is found that the model-calculated ozone concentrations are generally in good agreement with the measurements, and the stratospheric contribution to surface ozone mixing ratios is quite limited.
    Zhang H., G. Y. Shi, T. Nakajima, and T. Suzuki, 2006a: The effects of the choice of the k-interval number on radiative calculations. Journal of Quantitative Spectroscopy and Radiative Transfer, 98, 31- 43.10.1016/j.jqsrt.2005.05.0902c14eb54-8fc0-4fb8-a5a1-aa063fc0487d4b5021c29902ea506207f893bed1f64ehttp%3A%2F%2Fwww.sciencedirect.com%2Fscience%2Farticle%2Fpii%2FS0022407305002323refpaperuri:(641f287f753dc98e2a8a521b76d5da78)http://www.sciencedirect.com/science/article/pii/S0022407305002323The selection of the number of k -interval is a foundation to correlated k -distribution method and the problem of how to do it still remains unsettled. It is pointed out by numerical computation in this work that choosing the number of k -interval is a major factor affecting accuracy and speed in radiative calculation. To increase the number of k -interval is an efficient method to improve the accuracy. However, it is found by this study that there exists a saturation of the accuracy to an increase of the number. The optimal rules on the number of k -interval choosing are proposed in the paper. Then, five versions on atmospheric absorption by gases appropriate for GCMs are given according to them.
    Zhang H., T. Suzuki, T. Nakajima, G. Y. Shi, X. Y. Zhang, and Y. Liu, 2006b: Effects of band division on radiative calculations. Optical Engineering, 45, 016002.d75c76d1-4a36-457f-b136-9be34afe588ea9b3d5f34ff4ed34ce8641b46bbd60f8http%3A%2F%2Fscitation.aip.org%2Fgetabs%2Fservlet%2FGetabsServlet%3Fprog%3Dnormal%26id%3DOPEGAR000045000001016002000001%26idtype%3Dcvips%26gifs%3DYesrefpaperuri:(4c84d5e59ab56f21948e96cd6903d0ef)/s?wd=paperuri%3A%284c84d5e59ab56f21948e96cd6903d0ef%29&filter=sc_long_sign&tn=SE_xueshusource_2kduw22v&sc_vurl=http%3A%2F%2Fscitation.aip.org%2Fgetabs%2Fservlet%2FGetabsServlet%3Fprog%3Dnormal%26id%3DOPEGAR000045000001016002000001%26idtype%3Dcvips%26gifs%3DYes&ie=utf-8&sc_us=13613871562377111846
    Zhang H., Z. Shen, X.-D. Wei, M. Zhang, and Z. Li, 2012a: Comparison of optical properties of nitrate and sulfate aerosol and the direct radiative forcing due to nitrate in china. Atmos. Res., 113, 113- 125.10.1002/chin.200337218cd77d0be04ac2493ceb15d7969c9bd5bhttp%3A%2F%2Fwww.sciencedirect.com%2Fscience%2Farticle%2Fpii%2FS0169809512001330http://www.sciencedirect.com/science/article/pii/S0169809512001330Using model-simulated nitrate concentrations in China that reproduce observed features reasonably well, we found significant spatial and seasonal changes in DRFs due to nitrate aerosols. DRFs were stronger in winter, spring, and autumn, but much weaker in summer. The annual mean values of the forcings over China were 61024.5102W02m 61022 and 61020.9502W02m 61022 under clear-sky and all-sky conditions, respectively. Clouds play an important role in determining the DRF and can greatly reduce the forcing strength and its geographical extent.
    Zhang, H., Coauthors, 2012b: Simulation of direct radiative forcing of aerosols and their effects on East Asian climate using an interactive AGCM-aerosol coupled system. Climate Dyn., 38, 1675- 1693.10.1007/s00382-011-1131-0c32f63229d7da3b934d20193a4754102http%3A%2F%2Fcpfd.cnki.com.cn%2FArticle%2FCPFDTOTAL-KLQR201108002074.htmhttp://cpfd.cnki.com.cn/Article/CPFDTOTAL-KLQR201108002074.htmAn interactive system coupling the Beijing Climate Center atmospheric general circulation model (BCC_AGCM2.0.1) and the Canadian Aerosol Module (CAM) with updated aerosol emission sources was developed to investigate the global distributions of optical properties and direct radiative forcing (DRF) of typical aerosols and their impacts on East Asian climate. The simulated total aerosol optical depth (AOD), single scattering albedo, and asymmetry parameter were generally consistent with the ground-based measurements. Under all-sky conditions, the simulated global annual mean DRF at the top of the atmosphere was 0903’2.03 W m for all aerosols including sulfate, organic carbon (OC), black carbon (BC), dust, and sea salt; the global annual mean DRF was 0903’0.23 W m for sulfate, BC, and OC aerosols. The sulfate, BC, and OC aerosols led to decreases of 0.5800° and 0.14 mm day in the JJA means of surface temperature and precipitation rate in East Asia. The differences of land-sea surface temperature and surface pressure were reduced in East Asian monsoon region due to these aerosols, thus leading to the weakening of East Asian summer monsoon. Atmospheric dynamic and thermodynamic were affected due to the three types of aerosol, and the southward motion between 1500°N and 3000°N in lower troposphere was increased, which slowed down the northward transport of moist air carried by the East Asian summer monsoon, and moreover decreased the summer monsoon precipitation in south and east China.
    Zhang H., Q. Chen, B. Xie, and S. Y. Zhao, 2014a: PM2.5 and tropospheric ozone in china and pollutant emission controlling integrated analyses. Progressus Inquisitiones de Mutatione Climatis, 10, 289- 296. (in Chinese)27076975-474a-418e-8217-8bb7343685d84907cb4ff18b66afcb309f8a873c37e4http%3A%2F%2Fwww.climatechange.cn%2FEN%2FY2014%2FV10%2FI4%2F289http://www.climatechange.cn/EN/Y2014/V10/I4/289This work reviewed the observational status of PM2.5 and tropospheric ozone in China firstly; the distribution of the concentration of tropospheric ozone over the globe and China were given based on the satellite observation during the period of 2010-2013. The annual mean values are 29.78 DU and 33.97 DU in the globe and China region, respectively. Then, the distribution of PM2.5 concentration and their seasonal changes in China were simulated by an aerosol chemistry-climate coupled model system, with annual mean value of 0.51-10kg/m. The contributions from five kinds of aerosols to the simulated PM2.5 concentrations in different seasons were also analyzed. Then, the relations between the emissions of aerosol, greenhouse gases and their precursors and their radiative forcings were illustrated referring to the IPCC AR5. For these relations, the possible effects of controlling ozone precursors and particle matter on the climate were given, of which, the former is not totally clear, while reducing emissions of short lived greenhouse gases and black carbon is a secondary measure for short term (the future 50 years) climate change mitigation. Reducing emission of COis still our main strategy to promise the target of global average surface air temperature rise less than 2鈩. The strategies of pollutant emission control for near term and long term are all important for the prospects of both environment protection and climate change mitigation.
    Zhang H., X.-W. Jing, and J. Li, 2014b: Application and evaluation of a new radiation code under McICA scheme in BCC_AGCM2.0.1. Geoscientific Model Development, 7, 737- 754.10.5194/gmd-7-737-20148cf68c6dce16b5a50ccb56e217704588http%3A%2F%2Fadsabs.harvard.edu%2Fabs%2F2014GMD.....7..737Zhttp://adsabs.harvard.edu/abs/2014GMD.....7..737ZThis research incorporates the correlated k distribution BCC-RAD radiation model into the climate model BCC_AGCM2.0.1 and examines the change in climate simulation by implementation of the new radiation algorithm. It is shown that both clear-sky radiation fluxes and cloud radiative forcings (CRFs) are improved. The modeled atmospheric temperature and specific humidity are also improved due to changes in radiative heating rates, which most likely stem from the revised treatment of gaseous absorption. Subgrid cloud variability, including vertical overlap of fractional clouds and horizontal inhomogeneity in cloud condensate, is addressed by using the Monte Carlo Independent Column Approximation (McICA) method. In McICA, a cloud-type-dependent function for cloud fraction decorrelation length, which gives zonal mean results very close to the observations of CloudSat/CALIPSO, is developed. Compared to utilizing a globally constant decorrelation length, the maximum changes in seasonal CRFs by the new scheme can be as large as 10 and 20 W mfor longwave (LW) and shortwave (SW) CRFs, respectively, mostly located in the tropics. The inclusion of an observation-based horizontal inhomogeneity of cloud condensate has also a significant impact on CRFs, with global means of ~ 1.5 W mand ~ 3.7 Wmfor LW and SW CRFs at the top of atmosphere (TOA), respectively. Generally, incorporating McICA and horizontal inhomogeneity of cloud condensate in the BCC-RAD model reduces global mean TOA and surface SW and LW flux biases in BCC_AGCM2.0.1. These results demonstrate the feasibility of the new model configuration to be used in BCC_AGCM2.0.1 for climate simulations, and also indicate that more detailed real-world information on cloud structures should be obtained to constrain cloud settings in McICA in the future.
    Zhao S.Y., H. Zhang, S. Feng, and Q. Fu, 2015: Simulating direct effects of dust aerosol on arid and semi-arid regions using an aerosol_climate model system. Int. J. Climatol.,35, doi: 10.1002/joc.4093.
    Zhou X. J., C. Luo, W. L. Li, and J. E. Shi, 1995: Total ozone changes in China and low center over the Tibetan plateau. Chinese Science Bulletin, 40, 1396- 1398. (in Chinese)
    Zhou T. J., L. W. Zou, B. Wu, C. X. Jin, F. F. Song, X. L. Chen, and L. X. Zhang, 2014a: Development of earth/climate system models in China: A review from the Coupled Model Intercomparison Project perspective. Journal of Meteorological Research, 28( 5), 762- 779.10.1007/s13351-014-4501-968a6d0ec-1caf-4495-aab5-f355600c43c1mag4356520142857628857595832f9286cf509a49cbf678bb0http%3A%2F%2Fd.wanfangdata.com.cn%2FPeriodical_qxxb-e201405007.aspxhttp://d.wanfangdata.com.cn/Periodical_qxxb-e201405007.aspxThe development of coupled earth/climate system models in China over the past 20 years is reviewed,including a comparison with other international models that participated in the Coupled Model Intercomparison Project(CMIP) from phase 1(CMIPl) to phase 4(CMIP4).The Chinese contribution to CMIP is summarized,and the major achievements from CMIP1 to CMIP3 are listed as a reference for assessing the strengths and weaknesses of Chinese models.After a description of CMIP5 experiments,the five Chinese models that participated in CMIP5 are then introduced.Furthermore,following a review of the current status of international model development,both the challenges and opportunities for the Chinese climate modeling community are discussed.The development of high-resolution climate models,earth system models,and improvements in atmospheric and oceanic general circulation models,which are core components of earth/climate system models,are highlighted.To guarantee the sustainable development of climate system models in China,the need for national-level coordination is discussed,along with a list of the main components and supporting elements identified by the US National Strategy for Advancing Climate Modeling.
    Zhou, T. J., Coauthors, 2014b: Chinese contribution to CMIP5: An overview of five Chinese models' performances. Journal of Meteorological Research, 28( 4), 481- 509.10.1007/s13351-014-4001-y8f9f38b3-badd-4ffb-91cc-7428cf80da41mag435652014284481An overview of Chinese contribution to Coupled Model Intercomparison Project-Phase 5 (CMIP5) is presented. The performances of five Chinese Climate/Earth System Models that participated in the CMIP5 project are assessed in the context of climate mean states, seasonal cycle, intraseasonal oscillation, interan- nual variability, interdecadal variability, global monsoon, Asian-Australian monsoon, 20th-century historical climate simulation, climate change projection, and climate sensitivity. Both the strengths and weaknesses of the models are evaluated. The models generally show reasonable performances in simulating sea surface tem- perature (SST) mean state, seasonal cycle, spatial patterns of Madden-Julian oscillation (MJO) amplitude and tropical cyclone Genesis Potential Index (GPI), global monsoon precipitation pattern, El Ni&#241;o-Southern Oscillation (ENSO), and Pacific Decadal Oscillation (PDO) related SST anomalies. However, the perfor- mances of the models in simulating the time periods, amplitude, and phase locking of ENSO, PDO time periods, GPI magnitude, MJO propagation, magnitude of SST seasonal cycle, northwestern Pacific mon- soon and North American monsoon domains, as well as the skill of large-scale Asian monsoon precipitation need to be improved. The model performances in simulating the time evolution and spatial pattern of the 20th-century global warming and the future change under representative concentration pathways projection are compared to the multimodel ensemble of CMIP5 models. The model discrepancies in terms of climate sensitivity are also discussed.
    Ziemke J. R., S. Chand ra, G. J. Labow, P. K. Bhartia, L. Froidevaux, and J. C. Witte, 2011: A global climatology of tropospheric and stratospheric ozone derived from aura OMI and MLS measurements. Atmos. Chem. Phys., 11, 9237- 9251.10.5194/acpd-11-17879-2011802ce523-e505-4a3d-b9ec-9d5bb1c06ea310ccb81f053d19c9a51e1cfba1519a8dhttp%3A%2F%2Fwww.oalib.com%2Fpaper%2F1369742refpaperuri:(afb1f319b251c86039413e0ef42a44f3)http://www.oalib.com/paper/1369742ABSTRACT A global climatology of tropospheric and stratospheric column ozone is derived by combining six years of Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) ozone measurements for the period October 2004 through December 2010. The OMI/MLS tropospheric ozone climatology exhibits large temporal and spatial variability which includes ozone accumulation zones in the tropical south Atlantic year-round and in the subtropical Mediterranean/Asia region in summer months. High levels of tropospheric ozone in the Northern Hemisphere also persist in mid-latitudes over the Eastern North American and Asian continents extending eastward over the Pacific Ocean. For stratospheric ozone climatology from MLS, largest ozone abundance lies in the Northern Hemisphere in the latitude range 70 N-80 N in February-April and in the Southern Hemisphere around 40 S-50 S during months August-October. The largest stratospheric ozone abundances in the Northern Hemisphere lie over North America and Eastern Asia extending eastward across the Pacific Ocean and in the Southern Hemisphere south of Australia extending eastward across the dateline. With the advent of many newly developing 3-D chemistry and transport models it is advantageous to have such a dataset for evaluating the performance of the models in relation to dynamical and photochemical processes controlling the ozone distributions in the troposphere and stratosphere. The OMI/MLS ozone gridded climatology data, both calculated mean values and RMS uncertainties are made available to the science community via the NASA total ozone mapping spectrometer (TOMS) website http://toms.gsfc.nasa.gov.
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Manuscript received: 14 September 2015
Manuscript revised: 17 March 2016
Manuscript accepted: 11 April 2016
通讯作者: 陈斌, bchen63@163.com
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    沈阳化工大学材料科学与工程学院 沈阳 110142

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A Modeling Study of Effective Radiative Forcing and Climate Response Due to Tropospheric Ozone

  • 1. Key Laboratory for Semi-Arid Climate Change of the Ministry of Education, College of Atmosphere Science, Lanzhou University, Lanzhou 730000
  • 2. Laboratory for Climate Studies of China Meteorological Administration, National Climate Center, China Meteorological Administration, Beijing 100081
  • 3. Chinese Academy of Meteorological Sciences, Beijing 100081
  • 4. Department of Atmospheric Sciences, University of Washington, Seattle, 98195,USA

Abstract: This study simulates the effective radiative forcing (ERF) of tropospheric ozone from 1850 to 2013 and its effects on global climate using an aerosol-climate coupled model, BCC_AGCM2.0.1_CUACE/Aero, in combination with OMI (Ozone Monitoring Instrument) satellite ozone data. According to the OMI observations, the global annual mean tropospheric column ozone (TCO) was 33.9 DU in 2013, and the largest TCO was distributed in the belts between 30°N and 45°N and at approximately 30°S; the annual mean TCO was higher in the Northern Hemisphere than that in the Southern Hemisphere; and in boreal summer and autumn, the global mean TCO was higher than in winter and spring. The simulated ERF due to the change in tropospheric ozone concentration from 1850 to 2013 was 0.46 W m-2, thereby causing an increase in the global annual mean surface temperature by 0.36°C, and precipitation by 0.02 mm d-1 (the increase of surface temperature had a significance level above 95%). The surface temperature was increased more obviously over the high latitudes in both hemispheres, with the maximum exceeding 1.4°C in Siberia. There were opposite changes in precipitation near the equator, with an increase of 0.5 mm d-1 near the Hawaiian Islands and a decrease of about -0.6 mm d-1 near the middle of the Indian Ocean.

1. Introduction
  • Since the early 1970s, ozone has been receiving increasing attention as its concentrations are increasingly influenced by human activities. As a radiatively active gas, ozone has an effect on longwave and shortwave radiation in both the stratosphere and troposphere. Stratospheric ozone has strong absorption in solar UV radiation, leading to a surface cooling of the Earth, while tropospheric ozone causes a greenhouse effect by interacting with terrestrial longwave radiation. Any changes in the concentration of ozone can cause radiative forcing (RF) and therefore lead to climate change (Lacis et al., 1990; Forster et al., 2007).

    The concentration of tropospheric ozone has significantly increased since the industrial revolution. The main sources of tropospheric ozone include the downward transport of ozone from the stratosphere (Stohl et al., 2003; Hsu and Prather, 2009) and the photochemical oxidation of precursors. Methane (CH4), carbon monoxide (CO), and non-CH4 volatile organic compounds in the presence of nitrogen oxides (NOx) are the main anthropogenic precursors of ozone (Crutzen, 1974; Derwent et al., 1996; Zhang et al., 2004). When the emissions of NOx and CO double in India, tropospheric ozone can be increased up to 21 ppbv, with a relative change of more than 10% in the upper troposphere (Liu et al., 2003). Tropospheric ozone is depleted by several chemical reactions (Crutzen, 1974). Increases in absolute humidity (driven by global warming), changes in the ozone distribution itself, and changes of hydroxyl and peroxyl radicals, have influenced the rapid consumption of tropospheric ozone by chemical processes (Johnson et al., 2001; Stevenson et al., 2006; Isaksen et al., 2009). Tropospheric ozone can also be cleared by dry deposition, and it has an adverse effect on the photosynthesis of plants (Fowler et al., 2009). Anthropogenic precursor emissions are probably the main driver of changes in tropospheric ozone, and have increased dramatically since the industrial era (Lamarque et al., 2010).

    The global distribution of ozone in the atmosphere can be retrieved by satellite remote sensing, with early observational ozone data having been obtained from the Total Ozone Mapping Spectrometer (TOMS) and the Solar Backscatter Ultraviolet (SBUV) sensor (Heath et al., 1975). More recently, the Ozone Monitoring Instrument (OMI) onboard the Aura satellite has offered improvements by monitoring the UV/visible continuous spectrum with high spatial resolution (Miyazaki et al., 2012). Inversion methods have also been developed, including the continuously improving TOMS inversion method and a combination of TOMS and Differential Optical Absorption Spectroscopy (Antõn et al., 2009). To obtain the updated RF due to tropospheric ozone, the ozone observational data of the OMI in 2013 are utilized in this work.

    IPCC AR5 reported that the radiative forcing (RF) at the tropopause was 0.40 0.2 W m-2 due to the changes in tropospheric ozone since the industrial revolution. Tropospheric ozone is an important short-lived greenhouse gas, and controlling the emissions of its precursors can effectively slow down global warming (Zhang et al., 2014a). (Skeie et al., 2011) estimated that tropospheric ozone increased by about 11.4 DU from pre-industrial times to 2010. (Shindell et al., 2006) simulated the impact of tropospheric ozone on global mean surface temperature, and found that the increase in tropospheric ozone from pre-industrial times to 2000 could have contributed approximately 0.11°C to global warming. (Chang et al., 2009) simulated the climate responses to the direct RF due to tropospheric ozone in eastern China during 1951-2000, and found that the ozone forcing led to changes in the mean surface air temperature and precipitation in eastern China by +0.43°C and -0.08 mm d-1, respectively.

    The most recent estimation only reported RFs due to tropospheric ozone during 1850-2000 (Conley et al., 2013; Lamarque et al., 2013; Stevenson et al., 2013, Stordal et al., 2003), and very few studies have estimated the updated RF due to ozone from the pre-industrial era to the year 2013 and its climate effect. In this study, the updated tropospheric ozone observational data of 2013 were inputted into BCC_AGCM2.0.1, which had previously been coupled with the China Meteorological Administration Unified Atmospheric Chemistry Environment for Aerosols (CUACE/Aero) model (Wang et al., 2014; Zhang et al., 2014b), to simulate the effective RF (ERF) due to tropospheric ozone and its impact on the global climate. As defined in IPCC AR5, ERF is the net downward radiative flux change at the TOA allowing atmospheric temperatures, clouds and water vapor to adjust, but with surface or sea surface temperature and sea ice unchanged. Rapid tropospheric adjustments can influence the flux perturbations, leading to differences in long-term climate change due to the forcing agents. So, allowing the rapid adjustments in the troposphere can provide a relatively accurate characterization of the forcing due to tropospheric constituent changes.

    In section 2, the ozone data, model and ERF calculation method are briefly introduced. In section 3, the distribution of tropospheric ozone concentration and the ERF due to tropospheric ozone are analyzed, and then the climate effect of tropospheric ozone is discussed. A summary and discussion of the study is presented in section 4.

2. Data, model, and scheme description
  • The ozone profile data observed by the OMI in 2013 were used in this study. The OMI is one of the instruments onboard the Aura spacecraft (data available at: http://aura.gsfc.nasa.gov/), which was launched by NASA on 15 July 2004, as part of the EOS. The OMI is a nadir-scanning instrument, and it can measure column ozone in the UV (270-314 nm and 306-380 nm) and visible (350-500 nm) wavelengths. OMI has a global coverage (except polar night latitudes) at a spatial resolution of 13× 24 km, and a swath width of approximately 2600 km. According to the studies of (Buchard et al., 2008) and (Veefkind et al., 2006), the relative uncertainty of OMI data is about 3%. The ozone profile data are given in terms of the layer-columns of ozone in DU for an 18-layered atmosphere (about 2.5 km for each layer) (Miyazaki et al., 2012). NCEP daily mean tropopause data for 2013 (http://www.esrl.noaa.gov/) were also used in this study, for the calculation of tropospheric column ozone (TCO).

  • The aerosol-climate model BCC_AGCM2.0.1_CUACE/ Aero developed by (Zhang et al., 2012a), (Zhang et al., 2014b), and (Wang et al., 2014), was used in this study. The model has joined AeroCom Phase II (Myhre et al., 2013a), and it has been used to study the RFs of aerosols and the subsequent effects on climate (e.g., Zhang et al., 2012b; Wang et al., 2013a, 2013b, 2014, 2015; Zhao et al., 2015). BCC_AGCM is a general circulation model developed by the Beijing Climate Center of the China Meteorological Administration, and its main features have been described by (Wu et al., 2010). The CUACE/Aero aerosol model, developed by the Institute of Atmospheric Composition of the Chinese Academy of Meteorological Sciences, was coupled with BCC_AGCM by (Zhang et al., 2012b). The model employs a horizontal T42 spectral resolution (approximately 2.8° × 2.8°) and vertical hybrid δ-pressure coordinates, including 26 layers, with the top located at about 2.9 hPa. Recently, several revisions have been made to improve the physics of the model. First, several schemes were incorporated into BCC_AGCM (Zhang et al., 2014b), which included the cloud overlap scheme of the Monte Carlo independent column approximation (Pincus et al., 2003) and the radiation scheme BCC_RAD (Beijing Climate Center Radiation Transfer Mode) developed by Zhang et al. (2003, 2006a, 2006b). These schemes improved the accuracy of the sub-grid cloud structure and its radiative transfer process (Zhang et al., 2014b). Second, the methods of (Nakajima et al., 2000) and (Zhang et al., 2014a) were adopted to calculate the optical properties of water and ice clouds. More details about this coupled system can be found in (Zhang et al., 2012b) and (Wang et al., 2014). (Xin et al., 2013) estimated the sensitivity and general performance of the climate model, with their results showing the transient climate response (TCR) of the BCC model to be 1.94°C (the mean TCR was found to be 2.0°C for 16 climate models participating in CMIP5), and the model overestimating the global warming but underestimating the warming amplitude over China in the early 21st century. Furthermore, BCC_AGCM's participation in CMIP5 has shown reasonable performance in simulating important meteorological factors (Zhou et al., 2014a, 2014b).

  • Four experiments were performed in this study, named EXP1, EXP2, EXP3 and EXP4 (EXP1 and EXP2 were used to calculate ERF; EXP3 and EXP4 were for calculating the climate response; experiment configurations shown in Table 1). In EXP1, we used tropospheric ozone for the year 1850, given in (Lamarque et al., 2010); and the stratospheric ozone was from the OMI observational data for 2013. The tropopause in 1850 was defined as the height where the ozone concentration was 150 ppb, as used in (Young et al., 2012). In EXP2, everything was kept the same as in EXP1 except that the tropospheric ozone data from the OMI in 2013 were used. Each experiment was run for 15 years with prescribed SSTs. The last 10 years of results were analyzed to calculate the ERF due to the change in tropospheric ozone from 1850 to 2013. According to previous research (Kristjánsson et al., 2005), after a period of adjustment (generally five years for a model with prescribed SST), the global mean surface temperature will basically reach equilibrium (with small fluctuations). So, in this study, we just used the last 10 years of results of the 15-year runs of EXP1 and EXP2 to calculate the ERF due to the change in tropospheric ozone, as follows: $$ {ERF}=\Delta F_{EXP2}-\Delta F_{EXP1} , $$ where ∆ F was the net radiation flux (the difference between incoming and outgoing radiative flux, both shortwave and longwave) at the top of the model (for there is little difference in net radiation flux between the top of the model and the TOA). The ∆ F EXP1 (∆ F EXP2) was the net radiation flux of EXP1 (EXP2).

    The same tropospheric ozone data in EXP1/EXP2 were used in EXP3/EXP4. However, a coupled slab ocean model was used to replace the prescribed SST, in order to fully consider the climate response. EXP3 and EXP4 were run for 70 model years. In order to allow the global mean surface temperature to roughly reach equilibrium, the coupled slab ocean model needed 30 years of adjustment (Kristjánsson et al., 2005). So, we just used the last 40 years of results of the 70-year runs of EXP3 and EXP4 to facilitate discussion on the climate response due to the change in tropospheric ozone.

    The t-test was used on the model results to estimate their statistical significance. More specifically, the t-test used was the test for a difference between two sample means, as follows: $$ t=\dfrac{\overline{X_1}-\overline{X_2}}{\sqrt{\dfrac{(n_1-1)S_1^2+(n_2-1)S_2^2}{n_1+n_2-2}}\left(\dfrac{1}{n_1}+\dfrac{1}{n_2}\right)} , $$ where X and S was the average and variance of the sample, and n was sample size.

    Figure 1.  Seasonal mean distribution of TCO in 2013 from OMI observations: (a) DJF; (b) MAM; (c) JJA; (d) SON (units: DU).

3. Results
  • Figure 1 shows the seasonal mean distribution of TCO in 2013 from the OMI observation. The distribution of TCO varied both spatially and temporally. The largest TCO was mainly distributed in the belt between 30°N and 45°N, where the main emissions sources of anthropogenic ozone precursors were located. Additionally, another belt of peak TCO was located at approximately 30°S. Both belts of peak TCO in the NH and SH were due to some stratospheric ozone brought into the troposphere by the Brewer-Dobson circulation and latitudinal variations in the tropopause height (Lin et al., 2013). The area of high TCO in the SH was uniformly distributed in different seasons, with a maximum near the southern Indian Ocean. There were two low-TCO areas over the Tibetan Plateau and western North America. The TCO "trough" in the Tibetan Plateau is due to the increasing height of the tropopause over this region and dilution by low-ozone air from tropical areas (Zhou et al., 1995; Liu et al., 2010). The TCO was relatively low over the equator and polar areas, with a minimum in the Antarctic. The global mean TCO was higher in JJA (June-July-August) and SON (September-October-November), and lower in DJF (December-January-February) and MAM (March-April-May) (Table 2). The largest TCO (hemispheric mean: 40.74 DU) was recorded in MAM in the NH. The seasonal changes in the high-TCO areas in the SH were not as dramatic as in the NH, but there was also an obvious seasonal difference in the SH, with a maximum in SON (hemispheric mean: 36.94 DU). In China, the seasonal fluctuation of TCO was more notable, and the concentration reached a maximum in MAM (43.64 DU) before falling to a minimum in SON (30.98 DU). The temporal and spatial distributions of TCO were possibly a result of ozone generated by lightning discharges, fossil fuels and biomass burning, soil emissions, and seasonal transport due to planetary circulation (Ziemke et al., 2011).

    The global annual mean TCOs were 15.82 DU and 33.90 DU in 1850 and 2013, respectively [the TCO in 1850 given by (Lamarque et al., 2010) and the TCO in 2013 from the OMI observation). The spatial distributions of TCO in 1850 and 2013 were similar to some extent (Fig. 2). The TCO increased significantly in the midlatitudes (about 25 to 35 DU), where industrialized regions were located. The increase in TCO was less than 10 DU over high latitudes and less than 5 DU in the Antarctic. The TCO increased in the Tibetan Plateau and north of the Yangtze River in China (except northeastern China). Compared with other areas, the change in TCO was more apparent in China (increased by 20.99 DU in China and the global mean change in TCO was 18.06 DU). (Gao et al., 2009) showed that spatiotemporal variations in tropospheric ozone concentrations over East Asia were not only affected by the seasonal variation in solar intensity and photochemical activity [the most important contributor to ozone seasonality over Northeast Asia, as shown in (Kim and Lee, 2010)], but also influenced by the monsoons.

    Figure 2.  Global distribution of (a) annual mean TCO in 1850 and (b) the difference in TCO between 1850 and 2013 (units: DU). The TCO in 1850 is that given in Lamarque et al. (2010), while the TCO in 2013 is from the OMI observations.

    Figure 3.  The distribution of annual mean (a) shortwave ERF, (b) longwave ERF and (c) total ERF (units: W m$^-2$). The dots represent statistical significance according to the $t$-test at the $\ge 95%$ confidence level.

  • The increased emissions of ozone precursors into the atmosphere during the industrial era has led to a change in the ozone concentration and subsequently their ERF. However, for the effect of instant adjustment, the distributions of the change in tropospheric ozone and the consequent ERF did not agree very well. As shown in Fig. 3c, positive ERF occurred over the low latitudes of both hemispheres, such as Mexico, South Asia and the west coast of southern Africa. The ERF due to change in tropospheric ozone was negative over the midlatitudes of northern continents, such as northern Africa, Mongolia and especially northeastern China (approximately -5 W m-2) (see Fig. 3c). The shortwave ERF of tropospheric ozone was remarkably negative in eastern China, South Asia, and the Pacific region near the equator. However, in Southeast Asia and Siberia, the shortwave ERF was more notably positive. The most significantly negative and positive shortwave ERFs were in Southeast China (approximately -11 W m-2) and New Guinea (approximately 10 W m-2), respectively (see Fig. 3a). The distribution of longwave ERF was opposite to that of shortwave ERF, with the most significantly negative and positive longwave ERF in the Philippine basin (approximately -5 W m-2) and Arabian Sea (approximately 5.5 W m-2), respectively (see Fig. 3b). As IPCC AR5 reported, the difference between the ERF and RF for tropospheric ozone is likely to be small compared to the uncertainty in the RF (Shindell et al., 2013). The global annual mean total ERF was 0.46 W m-2 in this study, and the best estimate of tropospheric ozone RF reported in IPCC AR5 was 0.40 [0.20-0.60] W m-2. A comparison of our results and other model results is shown in Table 3.

    Figure 4.  Annual mean distributions of simulated differences in (a) surface temperature (units: $^\circ$C), (b) SNRF (units: W m$^-2$), (c) low cloud cover (units: %), (d) high cloud cover (units: %), and (e) zonal-mean total atmospheric meridional heat transport (units: K m s$^-1$) depicted by $VT$, where $V$ is the meridional velocity (units: m s$^-1$) and $T$ is the atmospheric temperature (units: K), and (f) wind field at 850 hPa (units: m s$^-1$) between EXP4 and EXP3. The dots represent statistical significance according to the $t$-test at the $\ge95%$ confidence level.

    Figure 5.  Simulated annual mean differences in (a) zonally averaged relative humidity (units: %), (b) cloud fraction (units: %), (c) precipitation (units: %), and (d) surface evaporation (units: %) between EXP4 and EXP3. The dots represent statistical significance according to the $t$-test at the $\ge 95%$ confidence level.

  • 3.3.1. Temperature

    Tropospheric ozone is an important short-lived greenhouse gas. The ERF of tropospheric ozone is generally positive, and leads to a warming effect on the near-surface climate. The simulations (EXP3 and EXP4) showed that the increase in tropospheric ozone since the industrial revolution caused an increase of 0.36°C in the global annual mean surface temperature, with a significance level above 95% on the global scale. As shown in Fig. 4a, the surface temperature was increased over most of the world, with a slight negative change in Alaska, in the southeastern and northwestern Pacific basin, and especially the Norwegian Sea (approximately -0.2°C). The warming over the middle and high latitudes of the boreal hemisphere was prominent, with a maximum exceeding 1.4°C, and it was also remarkable in the Antarctic Circle (approximately 1.0°C). Figure 4b shows the response of the surface net radiation flux (SNRF) to the change in tropospheric ozone. The distribution of SNRF was very consistent with surface temperature over the ocean areas, and there were significant increases in SNRF over the eastern Pacific Ocean near the equator, the west bank of southern Africa, the eastern sea near Japan and near the Antarctic Circle (with a significance level above 95% in these areas). The SNRF increased by more than 3.0 W m-2 in all the regions above, and the increase was particularly notable over the Tibetan Plateau where the increase reached approximately 8.0 W m-2. The increases in SNRF were also significant over the equatorial oceans, with a maximum increase of 3.52 W m-2. The SNRF decreased significantly over most of the Indian Ocean, South Pacific Ocean, west of the Ural Mountains, and the high latitudes of the SH (the decrease in the South Pacific Ocean had a significance level above 95%). The cooling in the North Pacific near the equator was most likely caused by the low-level cloud cover (below 680 hPa), which increased by around 2.0% (Fig. 4c) (with a significance level above 95%). The increase in low cloud resulted in a decrease in SNRF, thereby leading to a cooling effect at the surface. The increase in high-level cloud (above 440 hPa) can cause an increase in surface temperature. Therefore, the marked increase in high cloud might be the reason for the warming in the west near Greenland. Local temperature changes may not necessarily be explained by local processes (surface net radiation flux and cloud changes); they can be strongly influenced by changes in ambient heat transport. It should be noted that the surface temperature decreased in areas such as the southeastern Pacific basin and North Atlantic near the North Pole, but the total ERF was positive in these areas (Fig. 3c). This inconsistency might have been caused by the effect of air flow (Fig. 4f); there was cold advection from high latitudes in those areas. As shown in Fig. 4f, warm advection mainly caused the anomalous increasing of temperature in East Siberia, though the total ERF and SNRF there were both negative. Figure 4e shows the simulated annual mean difference in zonal-mean total atmospheric heat transport due to changes in the TCO. There was an increase in the total heat transport from high latitudes of the NH to regions near the North Pole. This increase also appeared at 30°S, and might have led to surface temperature increasing over Australia. Finally, the changes in total atmospheric heat transfer fed back to the changes in surface temperature.

    3.3.2. Evaporation, clouds and precipitation

    The increase in tropospheric ozone resulted in a warming effect on the atmosphere by positive ERF at the TOA, thereby causing an increase in surface evaporation (Fig. 5d). The spatial distributions of changes in surface evaporation and surface radiation flux were similar (Figs. 4b and 5d). The evaporation was dramatically increased at the sea surface over low and middle latitudes in both hemispheres, especially the Northwest and East Pacific (with a significance level above 95%), where evaporation was increased by more than 0.15 mm d-1. The surface evaporation was significantly weakened with the declining surface radiation flux in most areas.

    The increase in tropospheric ozone caused the amount of high, medium and low cloud to be reduced by 0.17%. In addition to surface evaporation, air flow convergence and divergence, changes in relative humidity and aerosol-cloud interactions also contribute to the changes in cloud cover. Thus, the changes in cloud cover and surface evaporation were not very consistent. Surface evaporation increased notably in the Pacific near 30°S, Yellow Sea and the Sea of Japan (Fig. 5d), with a significance level above 95%. However, the total cloud cover (mainly low cloud cover; Fig. 4c) decreased (with a significance level above 95%) due to the air divergence in the above regions (Fig. 4f).

    The vertical distribution of cloud was significantly influenced by relative humidity. As shown in Fig. 5a, the simulated annual mean differences in zonal mean relative humidity between EXP4 and EXP3 were consistent with that in zonal mean cloud fraction (Fig. 5b). The relative humidity was clearly reduced (maximum close to -1.0%) throughout the troposphere of the midlatitude NH, upper troposphere of the tropics in both hemispheres, and in most of the troposphere of the midlatitude SH, with a significance level above 95%. This might have been due to the decrease in surface evaporation and the air divergence. Because of the decrease in relative humidity, cloud cover was also reduced by about 0.2% to 0.8% in these areas (with a significance level above 95% in all the areas mentioned before), and led to a clear increase in SNRF, except in the Antarctic region. In contrast, the relative humidity and cloud cover increased remarkably throughout the troposphere near 60°S, the lower troposphere in the tropics, and the stratosphere in both hemispheres. There were significant increases of cloud cover in the lower troposphere over the high latitudes of both hemispheres, and these might have been due to the air convergence over these regions.

    The global distribution of changes in precipitation was similar to that of the changes in cloud cover. Near the equator, the changes in precipitation were notable, with a significance level above 95%. The precipitation and total cloud cover (mainly low cloud cover) increased significantly (over 0.5 mm d-1 and 4%) in the Hawaiian Islands, Philippines and Somalia. The precipitation and cloud cover were sharply reduced (over -0.6 mm d-1 and -4%) in the central Indian basin and Palau Islands. The total cloud cover and precipitation increased in the high latitudes of both hemispheres. The precipitation decreased in most of China, except the southeastern area.

4. Conclusions
  • This work studied the ERF and climate impact due to the tropospheric ozone concentration change since 1850 by using a coupling aerosol climate model, BCC_AGCM2.0.1_ CUACE/Aero, and OMI ozone concentration data in 2013. By analyzing the ozone data, we found that there were significant regional differences in TCO. The TCO was higher in the midlatitudes of the NH, mainly due to more emissions of ozone precursors from industry in this region. The maximum TCO was mainly located in the banded areas between 30°N to 45°N and around 30°S. The TCO was high in JJA and SON, and low in MAM and DJF. The maximum TCO was 36.58 DU in JJA, and the minimum was 30.46 DU in DJF. The TCO "trough" located over the Tibetan Plateau occurred in all seasons. The global mean TCO in 2013 (33.9 DU) was nearly double the value in 1850 (15.82 DU).

    The distribution of the simulated ERF due to the ozone concentration change since 1850 was dissimilar to that of TCO for the reason of instant adjustment. The annual mean ERF was 0.46 W m-2. A relatively positive ERF occurred in the low latitudes of both hemispheres, and a negative one in the mid-high latitudes of the NH.

    Tropospheric ozone, as an important short-lived greenhouse gas, has caused an average rise of 0.36°C in global temperature since 1850. The warming in the middle and high latitudes of both hemispheres was noticeable, and could exceed 0.8°C. The simulated annual mean difference in global surface evaporation and precipitation were both 0.02 mm d-1. Because of the change in tropospheric ozone concentrations, there were remarkable increases in the cloud cover near 60°S, the North Pole and the South Pacific, but the cloud cover decreased sharply near 40°N. The changes in the global distribution of precipitation and cloud cover were similar, especially near the equator. Precipitation increased significantly over the oceans from 10°N to 30°N, but was reduced (by about 0.6 mm d-1) over the central Indian basin and south of Guam.

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