ALBERT

Description: We present a global aerosol assimilation system based on an Ensemble Kalman filter, which we believe leads to a significant improvement in aerosol fields. The ensemble allows realistic, spatially and temporally variable model covariances (unlike other assimilation schemes). As the analyzed variables are mixing ratios (prognostic variables of the aerosol transport model), there is no need for the extra assumptions required by previous assimilation schemes analyzing aerosol optical thickness (AOT). We describe the implementation of this assimilation system and in particular the construction of the ensemble. This ensemble should represent our estimate of current model uncertainties. Consequently, we construct the ensemble around randomly modified emission scenarios. The system is tested with AERONET observations of AOT and Angström exponent (AE). Particular care is taken in prescribing the observational errors. The assimilated fields (AOT and AE) are validated through independent AERONET, SKYNET and MODIS Aqua observations. We show that, in general, assimilation of AOT observations leads to improved modelling of global AOT, while assimilation of AE only improves modelling when the AOT is high.

Description: There is great uncertainty regarding the role of mineral dust aerosols in Earth's climate system. One reason for this uncertainty is that the optical properties of mineral dust, such as its single scattering albedo (the ratio of scattering to total extinction), are poorly constrained because ground observations are limited to a few locations and satellite standard products are not available due to the excessively bright surface of the desert in the visible wavelength, which makes robust retrievals difficult. Here, we develop a method to estimate the spatial distributions of the aerosol single scattering albedo (ω0) and optical depth (τa), with daily 1°×1° spatial resolution using data from the Moderate Resolution Imaging Spectroradiometer (MODIS) as well as model simulations of radiative transfer. This approach is based on the "critical surface reflectance" method developed in the literature, which estimates ω0 from the top of the atmospheric radiance. We estimate the uncertainties in ω0 over the Sahara (Asia) to be approximately 0.020 and 0.010 (0.023 and 0.017) for bands 9 and 1, respectively, while the uncertainty in τa is approximately 0.235 and 0.228 (0.464 and 0.370) for bands 9 and 1, respectively. The 5–95% range of the spatial distribution of ω0 over the Sahara (Asia) is approximately 0.90–0.94 and 0.96–0.99 (0.87–0.94 and 0.89–0.97) for bands 9 and 1, respectively, and that of τa over the Sahara (Asia) is approximately 0.8–1.4 and 0.8–1.7 (0.7–2.0 and 0.7–1.9) for bands 9 and 1, respectively. The results for the Sahara indicate a good correlation between ω0 and the surface reflectance, and between ω0 and τa. However, the relationships between ω0, τa, and surface reflectance are less clear in Asia than in the Sahara, and the ω0 values are smaller than those in the Sahara. The regions with small ω0 values are consistent with the regions where coal-burning smoke and carbonaceous aerosols are reported to be transported in previous studies. Because the coal-burning and carbonaceous aerosols are known to be more absorptive and have smaller ω0 values than dust aerosols, our results indicate that the dust aerosols in Asia are contaminated by these anthropogenic aerosols. The spatial distribution of dust optical properties obtained in our work could be useful in understanding the role of dust aerosols in Earth's climate system, most likely through future collaboration with regional and global modelling studies.

Description: We present sensitivity tests for a global aerosol assimilation system utilizing AERONET observations of AOT (aerosol optical thickness) and AAE (aerosol Ångström exponent). The assimilation system employs an ensemble Kalman filter which requires tuning of three numerical parameters: ensemble size nens, local patch size npatch and inflation factor ρ. In addition, experiments are performed to test the impact of various implementations of the system. For instance, we use a different prescription of the emission ensemble or a different combination of observations. The various experiments are compared against one-another and against independent AERONET and MODIS/Aqua observations. The assimilation leads to significant improvements in modelled AOT and AAE fields. Moreover remaining errors are mostly random while they are mostly systematic for an experiment without assimilation. In addition, these results do not depend much on our parameter or design choices. It appears that the value of the local patch size has by far the biggest impact on the assimilation, which has sufficiently converged for an ensemble size of nens=20. Assimilating AOT and AAE is clearly preferential to assimilating AOT at two different wavelengths. In contrast, initial conditions or a description of aerosol beyond two modes (coarse and fine) have only little effect. We also discuss the use of the ensemble spread as an error estimate of the analysed AOT and AAE fields. We show that a very common prescription of the emission ensemble (independent random modification in each grid cell) can have trouble generating sufficient spread in the forecast ensemble.

Description: The direct radiative forcing by sulfate aerosols is still uncertain, mainly because the uncertainties are largely derived from differences in sulfate column burdens and its vertical distributions among global aerosol models. One possible reason for the large difference in the computed values is that the radiative forcing delicately depends on various simplifications of the sulfur processes made in the models. In this study, therefore, we investigated impacts of different parts of the sulfur chemistry module in a global aerosol model, SPRINTARS, on the sulfate distribution and its radiative forcing. Important studies were effects of simplified and more physical-based sulfur processes in terms of treatment of sulfur chemistry, oxidant chemistry, and dry deposition process of sulfur components. The results showed that the difference in the aqueous-phase sulfur chemistry among these treatments has the largest impact on the sulfate distribution. Introduction of all the improvements mentioned above brought the model values noticeably closer to in-situ measurements than those in the simplified methods used in the original SPRINTARS model. At the same time, these improvements also brought the computed sulfate column burdens and its vertical distributions into good agreement with other AEROCOM model values. The global annual mean radiative forcing due to the direct effect of anthropogenic sulfate aerosol was thus estimated to be −0.26 W m−2 (−0.30 W m−2 with a different SO2 inventory), whereas the original SPRINTARS model showed −0.18 W m−2 (−0.21 W m−2 with a different SO2 inventory). The magnitude of the difference between original and improved methods was approximately 50% of the uncertainty among estimates by the world's global aerosol models reported by the IPCC-AR4 assessment report. Findings in the present study, therefore, may suggest that the model differences in the simplifications of the sulfur processes are still a part of the large uncertainty in their simulated radiative forcings.

Description: Using one month of the cloud-resolving Nonhydrostatic Icosahedral Atmospheric Model (NICAM) simulations, we examined the impact of different definitions of clear-sky flux on the determination of longwave cloud radiative forcing (CRF). Because the satellite-like cloud-free composite preferentially samples drier conditions relative to the all-sky mean state, the conventional clear-sky flux calculation using the all-sky mean state in the model may represent a more humid atmospheric state in comparison to the cloud-free state. The drier bias is evident for the cloud-free composite in the NICAM simulations, causing an overestimation of the longwave CRF by about 10% compared to the NICAM simulated longwave CRF. Overall, water vapor contributions of up to 10% of the total longwave CRF should be taken account for making model-generated cloud forcing comparable to the satellite measurements.

Description: Black carbon (BC) absorbs shortwave radiation more strongly than any other type of aerosol, and an accurate simulation of the aging processes of BC-containing particle is required to properly predict aerosol radiative forcing (ARF) and climate change. However, BC aging processes have been simplified in general circulation models (GCMs) due to limited computational resources. In particular, differences in the representation of the mixing states of BC-containing particles between GCMs constitute one of main reasons for the uncertainty in ARF estimates. To understand an impact of the BC aging processes and the mixing state of BC on the spatial distribution of BC and ARF caused by BC (BC-ARF), we implemented three different methods of incorporating BC aging processes into a global aerosol transport model, SPRINTARS: (1) the "AGV" method, using variable conversion rates of BC aging based on a new type of parameterization depending on both BC amount and sulfuric acid; (2) the "AGF" method, using a constant conversion rate used worldwide in GCMs; and (3) the "ORIG" method, which is used in the original SPRINTARS. First, we found that these different methods produced different BC burden within 10% over industrial areas and 50% over remote oceans. Second, a ratio of water-insoluble BC to total BC (WIBC ratio) was very different among the three methods. Near the BC source region, for example, the WIBC ratios were estimated to be 80–90% (AGV and AGF) and 50–60% (ORIG). Third, although the BC aging process in GCMs had small impacts on the BC burden, they had a large impact on BC-ARF through a change in both the WIBC ratio and non-BC compounds coating on BC cores. As a result, possible differences in the treatment of the BC aging process between aerosol modeling studies can produce a difference of approximately 0.3 Wm−2 in the magnitude of BC-ARF, which is comparable to the uncertainty suggested by results from a global aerosol modeling intercomparison project, AeroCom. The surface aerosol forcing efficiencies normalized by aerosol optical thickness and by BC burden varied greatly with region in the AGV method, which allowed for the existence of internally mixed BC and sulfate, whereas these were not varied with region in the AGF method. These results suggest that the efficiencies of BC-ARF obtained by previous studies using the AGF method are significantly underestimated.

Description: We present sensitivity tests for a global aerosol assimilation system utilizing AERONET observations of AOT (aerosol optical thickness) and AAE (aerosol Ångström exponent). The assimilation system employs an ensemble Kalman filter which requires optimization of three numerical parameters: ensemble size nens, local patch size npatch and inflation factor ρ. In addition, experiments are performed to test the impact of various implementations of the system. For instance, we use a different prescription of the emission ensemble or a different combination of observations. The various experiments are compared against one-another and against independent AERONET andMODIS/Aqua observations. The assimilation leads to significant improvements in modelled AOT and AAE fields. Moreover remaining errors are mostly random while they are mostly systematic for an experiment without assimilation. In addition, these results do not depend much on our parameter or design choices. It appears that the value of the local patch size has by far the biggest impact on the assimilation, which has sufficiently converged for an ensemble size of nens=20. Assimilating AOT and AAE is clearly preferential to assimilating AOT at two different wavelengths. In contrast, initial conditions or a description of aerosol beyond two modes (coarse and fine) have only little effect. We also discuss the use of the ensemble spread as an error estimate of the analysed AOT and AAE fields. We show that a very common prescription of the emission ensemble (independent random modification in each grid cell) can have trouble generating sufficient spread in the forecast ensemble.

Description: There is a great deal of uncertainty surrounding the role of mineral dust aerosols in the earth's climate system. One reason for this uncertainty is that the optical properties of mineral dust, such as its single scattering albedo (the ratio of scattering to total extinction), are poorly understood because ground observations are limited to several locations and the satellite standard products are not available due to the excessively bright surface of the desert in the visible wavelength. We develop a method in this paper to estimate the spatial distributions of the aerosol single scattering albedo (ω0) and optical depth (τa), with daily 1 degree latitude and 1 degree longitude resolution, using data from Moderate Resolution Imaging Spectroradiometer (MODIS), as well as model simulations of radiative transfer. This approach is based on the "critical surface reflectance" method developed in the literature, which estimates ω0 from the top of the atmospheric radiance. We confirm that the uncertainties in our estimation of ω0 and τa are suitably minor and that the characteristic spatial distributions estimated over the Sahara and Asia are significant. The results for the Sahara indicate good correlation between ω0 and the surface reflectance and between ω0 and τa. Therefore, ω0 is determined mainly by the mineral composition of surface dust and/or the optical depth of airborne dust in the Sahara. On the other hand, the relationships between ω0, τa, and the surface reflectance are less clear in Asia than in the Sahara, and the values of ω0 are smaller than those in the Sahara. The regions with small ω0 values are consistent with the regions where coal-burning smoke and carbonaceous aerosols are thought to be transported, as reported in previous studies. Because the coal-burning and carbonaceous aerosols are known to be more absorptive and have smaller ω0 values than dust aerosols, our results indicate that the dust aerosols in Asia are contaminated by these anthropogenic aerosols. The spatial distribution of dust optical properties obtained in our work could be useful in understanding the roles of dust aerosols in the earth's climate system, most likely through future collaboration with regional and global modelling studies.

Description: An aerosol-coupled global nonhydrostatic model with a stretched-grid system has been developed. Circulations over the global and target domains are simulated with a single model, which includes fine meshes covering the target region to calculate meso-scale circulations. The stretched global model involves lower computational costs to simulate atmospheric aerosols with fine horizontal resolutions compared with a global uniform nonhydrostatic model, whereas it may require higher computational costs compared with the general regional models, because the stretched-grid system calculates inside and outside the target domain. As opposed to general regional models, the stretched-grid system requires neither a nesting technique nor lateral boundary conditions. In this study, we developed a new-type regional model for the simulation of aerosols over Japan, especially in the Kanto areas surrounding Tokyo, with a maximum horizontal resolution of approximately 10 km. This model usually reproduces temporal variations and their averages of the observed weather around Japan. This model generally reproduces monthly mean distributions of the observed sulfate and SO2 over East Asia, with high correlations (R 〉 0.6), but the underestimation of the simulated concentrations by 40% (sulfate) and 50% (SO2). Their underestimation of the simulated sulfate and SO2 concentrations over East Asia are strongly affected by their underestimation in China and possibly by the uncertainty of the simulated precipitation around Japan. In the Kanto area, this model succeeds in simulating the wind patterns and the diurnal transitions around the center of the Kanto area, although it is inadequate to simulate the wind patterns and the diurnal transitions at some sites located at the edge of the Kanto area and surrounded on three sides by mountains, e.g., Maebashi, mainly due to the insufficient horizontal resolution. This model also generally reproduces both diurnal and synoptic variations of the observed and/or a regional aerosol-transport model, WRF-CMAQ, simulated EC, sulfate, and SO2 concentrations in the Kanto area, especially with their high correlation (R 〉 0.5) at Komae/Tokyo. Although the aerosol module used in this study is relatively simplified compared to the general regional aerosol models, this study reveals that our proposed model with the stretched-grid system can be applicable for the regional aerosol simulation.

Description: Various ice particle habits are investigated in conjunction with inferring the optical properties of ice cloud for the Global Change Observation Mission-Climate (GCOM-C) satellite program. A database of the single-scattering properties of five ice particle habits, namely, plates, columns, droxtals, bullet-rosettes, and Voronoi, is developed. The database is based on the specification of the Second Generation Global Imager (SGLI) sensor onboard the GCOM-C satellite, which is scheduled to be launched in 2017 by Japan Aerospace Exploration Agency (JAXA). A combination of the finite-difference time-domain (FDTD) method, Geometric Optics Integral Equation (GOIE) technique, and geometric optics method (GOM) are applied to compute the single-scattering properties of the selected ice particle habits at 36 wavelengths, from the visible-to-infrared spectral region, covering the SGLI channels for the size parameter, which is defined with respect to the equivalent-volume radius sphere, which ranges between 6 and 9000. The database includes the extinction efficiency, absorption efficiency, average geometrical cross-section, single-scattering albedo, asymmetry factor, size parameter of an equivalent volume sphere, maximum distance from the center of mass, particle volume, and six non-zero elements of the scattering phase matrix. The characteristics of the calculated extinction efficiency, single-scattering albedo, and asymmetry factor of the five ice particle habits are compared. Furthermore, the optical thickness and spherical albedo of ice clouds using the five ice particle habit models are retrieved from the Polarization and Directionality of the Earth's Reflectances-3 (POLDER-3) measurements on board the Polarization and Anisotropy of Reflectances for Atmospheric Sciences coupled with Observations from a Lidar (PARASOL). The optimal ice particle habit for retrieving the SGLI ice cloud properties was investigated by adopting the spherical albedo difference (SAD) method. It is found that the SAD, for bullet-rosette particle, with radii of equivalent volume spheres (r~) ranging between 6 to 10 μm, and the Voronoi particle, with r~ ranging between 28 to 38 μm, and 70 to 100 μm, is distributed stably as the scattering angle increases. It is confirmed that the SAD of small bullet rosette and all sizes of voronoi particles has a low angular dependence, indicating that the combination of the bullet-rosette and Voronoi models are sufficient for retrieval of the ice cloud spherical albedo and optical thickness as an effective habit models of the SGLI sensor. Finally, SAD analysis based on the Voronoi habit model with moderate particles (r~ = 30 μm) is compared to the conventional General Habit Mixture (GHM), Inhomogeneous Hexagonal Monocrystal (IHM), 5-plate aggregate and ensemble ice particle model. It is confirmed that the Voronoi habit model has an effect similar to the counterparts of some conventional models on the retrieval of ice cloud properties from space-borne radiometric observations.