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We use simultaneous observations of tropospheric ozone and outgoing longwave radiation (OLR) sensitivity to tropospheric ozone from the Tropospheric Emission Spectrometer (TES) to evaluate model tropospheric ozone and its effect on OLR simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5-20 ppb) in the Southern Hemisphere (SH) and modest high bias (5-10 ppb) in the Northern Hemisphere (NH) relative to TES ozone for 2005-2010. These ozone biases have a significant impact on the OLR. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean tropospheric ozone low bias leads up to 120mW/ sq. m OLR high bias locally but zonally compensating errors reduce the global OLR high bias to 39+/- 41mW/ sq. m relative to TES data. We show that there is a correlation (Sq. R = 0.59) between the magnitude of the ACCMIP OLR bias and the deviation of the ACCMIP preindustrial to present day (1750-2010) ozone radiative forcing (RF) from the ensemble ozone RF mean. However, this correlation is driven primarily by models whose absolute OLR bias from tropospheric ozone exceeds 100mW/ sq. m. Removing these models leads to a mean ozone radiative forcing of 394+/- 42mW/ sq. m. The mean is about the same and the standard deviation is about 30% lower than an ensemble ozone RF of 384 +/- 60mW/ sq. m derived from 14 of the 16 ACCMIP models reported in a companion ACCMIP study. These results point towards a profitable direction of combining satellite observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing.

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

The Climate Absolute Radiance and Refractivity Observatory (CLARREO) is a climate observation system that has been designed to monitor the Earth's climate with unprecedented absolute radiometric accuracy and SI traceability. Climate Observation System Simulation Experiments (OSSEs) have been generated to simulate CLARREO hyperspectral shortwave imager measurements to help define the measurement characteristics needed for CLARREO to achieve its objectives. To evaluate how well the OSSE-simulated reflectance spectra reproduce the Earth s climate variability at the beginning of the 21st century, we compared the variability of the OSSE reflectance spectra to that of the reflectance spectra measured by the Scanning Imaging Absorption Spectrometer for Atmospheric Cartography (SCIAMACHY). Principal component analysis (PCA) is a multivariate decomposition technique used to represent and study the variability of hyperspectral radiation measurements. Using PCA, between 99.7%and 99.9%of the total variance the OSSE and SCIAMACHY data sets can be explained by subspaces defined by six principal components (PCs). To quantify how much information is shared between the simulated and observed data sets, we spectrally decomposed the intersection of the two data set subspaces. The results from four cases in 2004 showed that the two data sets share eight (January and October) and seven (April and July) dimensions, which correspond to about 99.9% of the total SCIAMACHY variance for each month. The spectral nature of these shared spaces, understood by examining the transformed eigenvectors calculated from the subspace intersections, exhibit similar physical characteristics to the original PCs calculated from each data set, such as water vapor absorption, vegetation reflectance, and cloud reflectance.

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

As part of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), we evaluate the historical black carbon (BC) aerosols simulated by 8 ACCMIP models against observations including 12 ice core records, long-term surface mass concentrations, and recent Arctic BC snowpack measurements. We also estimate BC albedo forcing by performing additional simulations using offline models with prescribed meteorology from 1996-2000. We evaluate the vertical profile of BC snow concentrations from these offline simulations using the recent BC snowpack measurements. Despite using the same BC emissions, the global BC burden differs by approximately a factor of 3 among models due to differences in aerosol removal parameterizations and simulated meteorology: 34 Gg to 103 Gg in 1850 and 82 Gg to 315 Gg in 2000. However, the global BC burden from preindustrial to present-day increases by 2.5-3 times with little variation among models, roughly matching the 2.5-fold increase in total BC emissions during the same period.We find a large divergence among models at both Northern Hemisphere (NH) and Southern Hemisphere (SH) high latitude regions for BC burden and at SH high latitude regions for deposition fluxes. The ACCMIP simulations match the observed BC surface mass concentrations well in Europe and North America except at Ispra. However, the models fail to predict the Arctic BC seasonality due to severe underestimations during winter and spring. The simulated vertically resolved BC snow concentrations are, on average, within a factor of 2-3 of the BC snowpack measurements except for Greenland and the Arctic Ocean. For the ice core evaluation, models tend to adequately capture both the observed temporal trends and the magnitudes at Greenland sites. However, models fail to predict the decreasing trend of BC depositions/ice core concentrations from the 1950s to the 1970s in most Tibetan Plateau ice cores. The distinct temporal trend at the Tibetan Plateau ice cores indicates a strong influence from Western Europe, but the modeled BC increases in that period are consistent with the emission changes in Eastern Europe, the Middle East, South and East Asia. At the Alps site, the simulated BC suggests a strong influence from Europe, which agrees with the Alps ice core observations. At Zuoqiupu on the Tibetan Plateau, models successfully simulate the higher BC concentrations observed during the non-monsoon season compared to the monsoon season but overpredict BC in both seasons. Despite a large divergence in BC deposition at two Antarctic ice core sites, some models with a BC lifetime of less than 7 days are able to capture the observed concentrations. In 2000 relative to 1850, globally and annually averaged BC surface albedo forcing from the offline simulations ranges from 0.014 to 0.019Wm−2 among the ACCMIP models. Comparing offline and online BC albedo forcings computed by some of the same models, we find that the global annual mean can vary by up to a factor of two because of different aerosol models or different BC-snow parameterizations and snow cover. The spatial distributions of the offline BC albedo forcing in 2000 show especially high BC forcing (i.e., over 0.1W/sq. m) over Manchuria, Karakoram, and most of the Former USSR. Models predict the highest global annual mean BC forcing in 1980 rather than 2000, mostly driven by the high fossil fuel and biofuel emissions in the Former USSR in 1980.

Present 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+/-23 Tg, the ensemble mean burden for 1850 time slice is approx. 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.