ALBERT

Description: We present a sensitivity study on the effects of spatial and temporal resolution of atmospheric relative humidity (RH) on calculated aerosol optical thickness (AOT) and the aerosol direct radiative effects (DRE) in a global model. Using the same aerosol fields simulated in the Global Modeling Initiative (GMI) model, we find that, on a global average, the calculated AOT from RH in 1° latitude by 1.25° longitude spatial resolution is 11% higher than that in 2° by 2.5° resolution, and the corresponding DRE at the top of the atmosphere is 8–9% higher for total aerosols and 15% higher for only anthropogenic aerosols in the finer spatial resolution case. The difference is largest over surface escarpment regions (e.g. 〉200% over the Andes Mountains) where RH varies substantially with surface terrain. The largest zonal mean AOT difference occurs at 50–60°N (16–21%), where AOT is also relatively larger. A similar increase is also found when the time resolution of RH is increased. This increase of AOT and DRE with the increase of model resolution is due to the highly non-linear relationship between RH and the aerosol mass extinction efficiency (MEE) at high RH (〉80%). Our study suggests that caution should be taken in a multi-model comparison (e.g. AeroCom) since the comparison usually deals with results coming from different spatial/temporal resolutions.

Description: We examine the response of Arctic gas and aerosol concentrations to perturbations in pollutant emissions from Europe, East and South Asia, and North America using results from a coordinated model intercomparison. These sensitivities to regional emissions (mixing ratio change per unit emission) vary widely across models and species. Intermodel differences are systematic, however, so that the relative importance of different regions is robust. North America contributes the most to Arctic ozone pollution. For aerosols and CO, European emissions dominate at the Arctic surface but Asian emissions become progressively more important with altitude, and are dominant in the upper troposphere. Sensitivities show strong seasonality: surface sensitivities typically maximize during boreal winter for European and during spring for East Asian and North American emissions. Mid-tropospheric sensitivities, however, nearly always maximize during spring or summer for all regions. Deposition of black carbon (BC) onto Greenland is most sensitive to North American emissions. North America and Europe each contribute ~40% of total BC deposition to Greenland, with ~20% from East Asia. Elsewhere in the Arctic, both sensitivity and total BC deposition are dominated by European emissions. Model diversity for aerosols is especially large, resulting primarily from differences in aerosol physics and removal. Comparison of aerosols with observations indicates problems in either the models or interpretation of the measurements. For gas phase pollutants such as CO and O3, which are relatively well-simulated, the processes contributing most to uncertainties depend on the source region. Uncertainties in the Arctic surface CO response to emissions perturbations are dominated by emissions for East Asian sources, while uncertainties in transport, emissions, and oxidation are comparable for European and North American sources. At higher levels, model-to-model variations in transport and oxidation are most important. Differences in photochemistry appear to play the largest role in the intermodel variations in Arctic ozone sensitivity.

Description: Knowledge of the global distribution of tropospheric aerosols is important for studying the effects of aerosols on global climate. Chemical transport models rely on archived meteorological fields, accounting for aerosol sources, transport and removal processes can simulate the global distribution of atmospheric aerosols. However, the accuracy of global aerosol modeling is limited. Uncertainty in location and strength of aerosol emission sources is a major factor in limiting modeling accuracy. This paper describes an effort to develop an algorithm for retrieving global sources of aerosol from satellite observations by inverting the GOCART aerosol transport model. To optimize inversion algorithm performance, the inversion was formulated as a generalized multi-term least-squares-type fitting. This concept uses the principles of statistical optimization and unites diverse retrieval techniques into a single flexible inversion procedure. It is particularly useful for choosing and refining a priori constraints in the retrieval algorithm. For example, it is demonstrated that a priori limitations on the partial derivatives of retrieved characteristics, which are widely used in atmospheric remote sensing, can also be useful in inverse modeling for constraining time and space variability of the retrieved global aerosol emissions. The similarities and differences with the standard "Kalman filter" inverse modeling approach and the "Phillips-Tikhonov-Twomey" constrained inversion widely used in remote sensing are discussed. In order to retain the originally high space and time resolution of the global model in the inversion of a long record of observations, the algorithm was expressed using adjoint operators in a form convenient for practical development of the inversion from codes implementing forward model simulations. The inversion algorithm was implemented using the GOCART aerosol transport model. The numerical tests we conducted showed successful retrievals of global aerosol emissions with a 2°×2.5° resolution by inverting the GOCART output. For achieving satisfactory retrieval from satellite sensors such as MODIS, the emissions were assumed constant within the 24 h diurnal cycle and aerosol differences in chemical composition were neglected. Such additional assumptions were needed to constrain the inversion due to limitations of satellite temporal coverage and sensitivity to aerosol parameters. As a result, the algorithm was defined for the retrieval of emission sources of fine and coarse mode aerosols from the MODIS fine and coarse mode aerosol optical thickness data respectively. Numerical tests showed that such assumptions are justifiable, taking into account the accuracy of the model and observations and that it provides valuable retrievals of the location and the strength of the aerosol emissions. The algorithm was applied to MODIS observations during two weeks in August 2000. The global placement of fine mode aerosol sources retrieved from inverting MODIS observations was coherent with available independent knowledge. This was particularly encouraging since the inverse method did not use any a priori information about the sources and it was initialized under a "zero aerosol emission" assumption. The retrieval reproduced the instantaneous global MODIS observations with a standard deviation in fitting of aerosol optical thickness of ~0.04. The optical thickness during high aerosol loading events was reproduced with a standard deviation of ~48%. Applications of the algorithm for the retrieval of coarse mode aerosol emissions were less successful, mainly due to the currently existing lack of MODIS data over high reflectance desert dust sources. Possibilities for enhancing the global satellite data inversion by using diverse a priori constraints on the retrieval are demonstrated. The potential and limitations of applying our approach for the retrieval of global aerosol sources from aerosol remote sensing are discussed.

Description: The effects of unified aerosol sources on global aerosol fields simulated by different models are examined in this paper. We compare results from two AeroCom experiments, one with different (ExpA) and one with unified emissions, injection heights, and particle sizes at the source (ExpB). Surprisingly, harmonization of aerosol sources has only a small impact on the simulated diversity for aerosol burden, and consequently optical properties, as the results are largely controlled by model-specific transport, removal, chemistry (leading to the formation of secondary aerosols) and parameterizations of aerosol microphysics (e.g. the split between deposition pathways) and to a lesser extent on the spatial and temporal distributions of the (precursor) emissions. The burdens of black carbon and especially sea salt become more coherent in ExpB only, because the large ExpA diversity for these two species was caused by few outliers. The experiment also indicated that despite prescribing emission fluxes and size distributions, ambiguities in the implementation in individual models can lead to substantial differences. These results indicate the need for a better understanding of aerosol life cycles at process level (including spatial dispersal and interaction with meteorological parameters) in order to obtain more reliable results from global aerosol simulations. This is particularly important as such model results are used to assess the consequences of specific air pollution abatement strategies.

Description: The effect of aqueous versus crystalline sulfate-nitrate-ammonium tropospheric particles on global aerosol direct radiative forcing is assessed. A global three-dimensional chemical transport model predicts sulfate, nitrate, and ammonium aerosol mass. An aerosol thermodynamics model is called twice, once for the upper side (US) and once for lower side (LS) of the hysteresis loop of particle phase. On the LS, the sulfate mass budget is 40% solid ammonium sulfate, 12% letovicite, 11% ammonium bisulfate, and 37% aqueous. The LS nitrate mass budget is 26% solid ammonium nitrate, 7% aqueous, and 67% gas-phase nitric acid release due to increased volatility upon crystallization. The LS ammonium budget is 45% solid ammonium sulfate, 10% letovicite, 6% ammonium bisulfate, 4% ammonium nitrate, 7% ammonia release due to increased volatility, and 28% aqueous. LS aerosol water mass partitions as 22% effloresced to the gas-phase and 78% remaining as aerosol mass. The predicted US/LS global fields of aerosol mass are employed in a Mie scattering model to generate global US/LS aerosol optical properties, including scattering efficiency, single scattering albedo, and asymmetry parameter. Global annual average LS optical depth and mass scattering efficiency are, respectively, 0.023 and 10.7 m2 (g SO4-2)-1, which compare to US values of 0.030 and 13.9 m2 (g SO4-2)-1. Radiative transport is computed, first for a base case having no aerosol and then for the two global fields corresponding to the US and LS of the hysteresis loop. Regional, global, seasonal, and annual averages of top-of-the-atmosphere aerosol radiative forcing on the LS and US (FL and FU, respectively, in W m-2) are calculated. Including both anthropogenic and natural emissions, we obtain global annual averages of FL=-0.750, FU=-0.930, and DFU,L=24% for full sky calculations without clouds and FL=-0.485, FU=-0.605, and DFU,L=25% when clouds are included. Regionally, DFU,L=48% over the USA, 55% over Europe, and 34% over East Asia. Seasonally, DFU,L varies from 18% in DJF to 75% in SON over the USA. The global annual average contribution from anthropogenic aerosol is FL=-0.314 and FU=-0.404, which yield normalized direct radiative forcings (G) of GL=-205 W (g SO4-2)-1 and GU=-264 W (g SO4-2)-1.

Description: We use aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission to examine the distributions and source attributions of O3 and NOy in the Arctic and sub-Arctic region. Using a number of marker tracers, we distinguish various air masses from the background troposphere and examine their contributions to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has a mean O3 of ~60 ppbv and NOx of ~25 pptv throughout spring and summer with CO decreasing from ~145 ppbv in spring to ~100 ppbv in summer. These observed mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in emissions and stratospheric ozone layer in the past two decades that influence Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses, with mean O3 concentrations of 140–160 ppbv, are significant direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin displays net O3 formation in the Arctic due to its sustainable, high NOx (75 pptv in spring and 110 pptv in summer) and NOy (~800 pptv in spring and ~1100 pptv in summer). The air masses influenced by the stratosphere sampled during ARCTAS-B also show conversion of HNO3 to PAN. This active production of PAN is the result of increased degradation of ethane in the stratosphere-troposphere mixed air mass to form CH3CHO, followed by subsequent formation of PAN under high NOx conditions. These findings imply that an adequate representation of stratospheric NOy input, in addition to stratospheric O3 influx, is essential to accurately simulate tropospheric Arctic O3, NOx and PAN in chemistry transport models. Plumes influenced by recent anthropogenic and biomass burning emissions observed during ARCTAS show highly elevated levels of hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contain O3 higher than that in the Arctic tropospheric background except some aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.

Description: The Multi-Angle Imaging Spectro-Radiometer (MISR) instrument on NASA's Terra satellite can provide more reliable Aerosol Optical Depth (AOD, τ) and more particle information, such as constraints on particle size (Angström exponent or ANG, α), particle shape, and single-scattering albedo (SSA, ω), than many other satellite instruments. However, MISR's ability to retrieve aerosol properties is weakened at low AOD levels. When aerosol-type information content is low, many candidate aerosol mixtures can match the observed radiances. We propose an algorithm to improve MISR aerosol retrievals by constraining MISR mixtures' ANG and absorbing AOD (AAOD) with Goddard Chemistry Aerosol Radiation and Transport (GOCART) model-simulated aerosol properties. To demonstrate this approach, we calculated MISR aerosol optical properties over the contiguous US from 2006 to 2009. Sensitivities associated with the thresholds of MISR-GOCART differences were analyzed according to the agreement between our results (AOD, ANG, and AAOD) and AErosol RObotic NETwork (AERONET) observations. Overall, our AOD has a good agreement with AERONET because the MISR AOD retrieval is not sensitive to different mixtures under many retrieval conditions. The correlation coefficient (r) between our ANG and AERONET improves to 0.45 from 0.29 for the MISR Version 22 standard product and 0.43 for GOCART when all data points are included. However, when only cases having AOD 〉 0.2, the MISR product itself has r ~ 0.40, and when only AOD 〉 0.2 and the best-fitting mixture are considered, r ~ 0.49. So as expected, the ANG improvement occurs primarily when the model constraint is applied in cases where the particle type information content of the MISR radiances is low. Regression analysis for AAOD shows that MISR Version 22 and GOCART misestimate AERONET by a ratio (mean retrieved AAOD to mean AERONET AAOD) of 0.5; our method improves this ratio to 0.74. Large discrepancies are found through an inter-comparison of the spatial-temporal patterns of MISR, GOCART, and our adjusted aerosol optical properties. We attribute these differences to (1) GOCART underestimations of AOD and ANG in polluted regions due to the emissions inventories used, and not considering the fine particles such as nitrate, (2) a lack of certain aerosol mixtures in the Version 22 algorithm climatology, (3) a lack of sensitivity in the MISR radiances to particle type under some conditions, and (4) parameters and thresholds used in our method.