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At least 37 records · Page 2

Measurements of aerosol microphysical and chemical properties in the central Arctic atmosphere during MOSAiC

The Arctic environment is transforming rapidly due to climate change. Aerosols’ abundance and physicochemical characteristics play a crucial, yet uncertain, role in these changes due to their influence on the surface energy budget through direct interaction with solar radiation and indirectly via cloud formation. Importantly, Arctic aerosol properties are also changing in response to climate change. Despite their importance, year-round measurements of their characteristics are sparse in the Arctic and often confined to lower latitudes at Arctic land-based stations and/or short high-latitude summertime campaigns. Here, we present unique aerosol microphysics and chemical composition datasets collected during the year-long Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition, in the central Arctic. These datasets, which include aerosol particle number concentrations, size distributions, cloud condensation nuclei concentrations, fluorescent aerosol concentrations and properties, and aerosol bulk chemical composition (black carbon, sulfate, nitrate, ammonium, chloride, and organics) will serve to improve our understanding of high-Arctic aerosol processes, with relevance towards improved modelling of the future Arctic (and global) climate.

54 ENVIRONMENTAL SCIENCES↗

Comparison of Modeled Backscatter using Measured Aerosol Microphysics with Focused CW Lidar Data over Pacific

During NASA's GLObal Backscatter Experiment (GLOBE) II flight mission over the Pacific Ocean in May-June 1990, extensive aerosol backscatter data sets from two continuous wave, focused CO2 Doppler lidars and an aerosol microphysics data set from a laser optical particle counter (LOPC) were obtained. Changes in aerosol loading in various air masses with associated changes in chemical composition, from sulfuric acid and sulfates to dustlike crustal material, significantly affected aerosol backscatter, causing variation of about 3 to 4 orders of magnitude. Some of the significant backscatter features encountered in different air masses were the low backscatter in subtropical air with even lower values in the tropics near the Intertropical Convergence Zone (ITCZ), highly variable backscatter in the ITCZ, mid-tropospheric aerosol backscatter background mode, and high backscatter in an Asian dust plume off the Japanese coast. Differences in aerosol composition and backscatter for northern and southern hemisphere also were observed. Using the LOPC measurements of physical and chemical aerosol properties, we determined the complex refractive index from three different aerosol mixture models to calculate backscatter. These values provided a well-defined envelope of modeled backscatter for various atmospheric conditions, giving good agreement with the lidar data over a horizontal sampling of approximately 18000 km in the mid-troposphere.

Srivastava, Vandana↗

Retrieval of Aerosol Microphysical Properties from AERONET Photo-Polarimetric Measurements. 2: A New Research Algorithm and Case Demonstration

A new research algorithm is presented here as the second part of a two-part study to retrieve aerosol microphysical properties from the multispectral and multiangular photopolarimetric measurements taken by Aerosol Robotic Network's (AERONET's) new-generation Sun photometer. The algorithm uses an advanced UNified and Linearized Vector Radiative Transfer Model and incorporates a statistical optimization approach.While the new algorithmhas heritage from AERONET operational inversion algorithm in constraining a priori and retrieval smoothness, it has two new features. First, the new algorithmretrieves the effective radius, effective variance, and total volume of aerosols associated with a continuous bimodal particle size distribution (PSD) function, while the AERONET operational algorithm retrieves aerosol volume over 22 size bins. Second, our algorithm retrieves complex refractive indices for both fine and coarsemodes,while the AERONET operational algorithm assumes a size-independent aerosol refractive index. Mode-resolved refractive indices can improve the estimate of the single-scattering albedo (SSA) for each aerosol mode and thus facilitate the validation of satellite products and chemistry transport models. We applied the algorithm to a suite of real cases over Beijing_RADI site and found that our retrievals are overall consistent with AERONET operational inversions but can offer mode-resolved refractive index and SSA with acceptable accuracy for the aerosol composed by spherical particles. Along with the retrieval using both radiance and polarization, we also performed radiance-only retrieval to demonstrate the improvements by adding polarization in the inversion. Contrast analysis indicates that with polarization, retrieval error can be reduced by over 50% in PSD parameters, 10-30% in the refractive index, and 10-40% in SSA, which is consistent with theoretical analysis presented in the companion paper of this two-part study.

aerosol retrieval algorithm↗

Intercomparison and Evaluation of Global Aerosol Microphysical Properties Among Aerocom Models of a Range of Complexity

Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multimodel- mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation an growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.

Cloud physics↗

Evaluation of the Global Aerosol Microphysical ModelE2-TOMAS Model Against Satellite and Ground-Based Observations

The TwO-Moment Aerosol Sectional (TOMAS) microphysics model has been integrated into the state-of-the- art general circulation model, GISS ModelE2. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the ModelE2-TOMAS model is compared to the default aerosol model in ModelE2, which is a one-moment aerosol (OMA) model (i.e. no aerosol microphysics). Overall, the ModelE2- TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement (mostly within a factor of 2) with observations of sulfur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as ModelE2-OMA) cannot capture the observed vertical distribution of sulfur dioxide over the Pacific Ocean, possibly due to overly strong convective transport and over-predicted precipitation. The ModelE2-TOMAS model simulates observed aerosol number concentrations and cloud condensation nuclei concentrations roughly within a factor of 2. Anthropogenic aerosol burdens in ModelE2-OMA differ from ModelE2-TOMAS by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. We observed larger differences for naturally emitted aerosols such as sea salt and mineral dust, as those emission rates are quite different due to different upper size cutoff assumptions.

Lee, Y. H.↗

A Fast and Efficient Version of the TwO-Moment Aerosol Sectional (TOMAS) Global Aerosol Microphysics Model

This study develops more computationally efficient versions of the TwO-Moment Aerosol Sectional (TOMAS) microphysics algorithms, collectively called Fast TOMAS. Several methods for speeding up the algorithm were attempted, but only reducing the number of size sections was adopted. Fast TOMAS models, coupled to the GISS GCM II-prime, require a new coagulation algorithm with less restrictive size resolution assumptions but only minor changes in other processes. Fast TOMAS models have been evaluated in a box model against analytical solutions of coagulation and condensation and in a 3-D model against the original TOMAS (TOMAS-30) model. Condensation and coagulation in the Fast TOMAS models agree well with the analytical solution but show slightly more bias than the TOMAS-30 box model. In the 3-D model, errors resulting from decreased size resolution in each process (i.e., emissions, cloud processing wet deposition, microphysics) are quantified in a series of model sensitivity simulations. Errors resulting from lower size resolution in condensation and coagulation, defined as the microphysics error, affect number and mass concentrations by only a few percent. The microphysics error in CN70CN100 (number concentrations of particles larger than 70100 nm diameter), proxies for cloud condensation nuclei, range from 5 to 5 in most regions. The largest errors are associated with decreasing the size resolution in the cloud processing wet deposition calculations, defined as cloud-processing error, and range from 20 to 15 in most regions for CN70CN100 concentrations. Overall, the Fast TOMAS models increase the computational speed by 2 to 3 times with only small numerical errors stemming from condensation and coagulation calculations when compared to TOMAS-30. The faster versions of the TOMAS model allow for the longer, multi-year simulations required to assess aerosol effects on cloud lifetime and precipitation.

Lee, Yunha↗

Advancements in the Representation of Cloud-Aerosol Microphysics in the GEOS-5 AGCM

Despite numerous challenges, the physical parameterization of cloud-aerosol interactions in atmospheric GCMs has become a top priority for advancement because of our need to simulate and understand past, current, and future indirect effects of aerosols on clouds. The challenges stem from the involvement of wide range of cloud-scale dynamics and aerosol activation physical processes. Cloud dynamics modulate cloud areal extent and condensate, while aerosol activation depends on aerosol mass load, size distribution, internal mixing state, and nucleating properties, and ultimately determines cloud optical properties via particle sizes. Both macro- and micro-scale processes are obviously important for cloud-radiation interactions. We will present the main features of cloud microphysical properties in the GEOS- 5 Atmospheric GCM (AGCM) as simulated by the McRAS-AC (Microphysics of Clouds with Relaxed Arakawa-Schubert and Aerosol-Cloud interaction) scheme. McRAS-AC uses Fountoukis and Nenes (2005) aerosol activation for liquid clouds, and has an option for either Liu and Penner (2005) or Barahona and Nenes (2008, 2009) aerosol activation for ice clouds. Aerosol loading (on-line or climatological) comes from GOCART, with an assumed log-normal size distribution. Other features of McRAS-AC are level-by-level cloud-scale thermodynamics, and Seifert-Beheng (2001)-type precipitation microphysics, particularly from moist convection. Results from Single-Column Model simulations will be shown to demonstrate how cloud radiative properties, lifetimes, and precipitation are influenced by different parameterization assumptions. Corresponding fields from year-long simulations of the full AGCM will also be presented with geographical distributions of cloud effective particle sizes compared to satellite retrievals. While the primary emphasis will be on current climate, simulation results with perturbed aerosol loadings will also be shown to expose the radiative sensitivity of the microphysical parameterization.

Lee, D.↗

Use of aerosol microphysical measurements to model IR backscatter in support of GLOBE

Data on the concentration and composition of free tropospheric aerosol over the Pacific Ocean, collected during the GAMETAG program in 1977-1978 (Davis, 1980 and Patterson et al., 1980) are used to model values of aerosol optical extinction coefficients (sigma) at two wavelengths (0.55 and 1 micron) and values of volume backscatter coefficients (beta) at four wavelengths (1 micron, 9.11 microns, 9.25 microns, and 10.6 microns) and to investigate the relationship between these parameters. The mass concentrations inferred from the GAMETAG measurements with optical particle spectrometers agreed with the results of simultaneous chemical measurements. The study of the relationships among the optical parameters indicates that visible and near-visible values of beta and sigma may be useful in predicting 9.11- and 10.6-micron backscatter.

Patterson, Edward M.↗

Representation of Nucleation Mode Microphysics in a Global Aerosol Model with Sectional Microphysics

In models, nucleation mode (1 nm<Dp <10 nm) particle microphysics can be represented explicitly with aerosol microphysical processes or can be parameterized to obtain the growth and survival of nuclei to the model's lower size boundary. This study investigates how the representation of nucleation mode microphysics impacts aerosol number predictions in the TwO-Moment Aerosol Sectional (TOMAS) aerosol microphysics model running with the GISS GCM II-prime by varying its lowest diameter boundary: 1 nm, 3 nm, and 10 nm. The model with the 1 nm boundary simulates the nucleation mode particles with fully resolved microphysical processes, while the model with the 10 nm and 3 nm boundaries uses a nucleation mode dynamics parameterization to account for the growth of nucleated particles to 10 nm and 3 nm, respectively.We also investigate the impact of the time step for aerosol microphysical processes (a 10 min versus a 1 h time step) to aerosol number predictions in the TOMAS models with explicit dynamics for the nucleation mode particles (i.e., 3 nm and 1 nm boundary). The model with the explicit microphysics (i.e., 1 nm boundary) with the 10 min time step is used as a numerical benchmark simulation to estimate biases caused by varying the lower size cutoff and the time step. Different representations of the nucleation mode have a significant effect on the formation rate of particles larger than 10 nm from nucleated particles (J10) and the burdens and lifetimes of ultrafinemode (10 nm≤Dp ≤70 nm) particles but have less impact on the burdens and lifetimes of CCN-sized particles. The models using parameterized microphysics (i.e., 10 nm and 3 nm boundaries) result in higher J10 and shorter coagulation lifetimes of ultrafine-mode particles than the model with explicit dynamics (i.e., 1 nm boundary). The spatial distributions of CN10 (Dp ≥10 nm) and CCN(0.2 %) (i.e., CCN concentrations at 0.2%supersaturation) are moderately affected, especially CN10 predictions above ∼700 hPa where nucleation contributes most strongly to CN10 concentrations. The lowermost-layer CN10 is substantially improved with the 3 nm boundary (compared to 10 nm) in most areas. The overprediction in CN10 with the 3 nm and 10 nm boundaries can be explained by the overprediction of J10 or J3 with the parameterized microphysics, possibly due to the instantaneous growth rate assumption in the survival and growth parameterization. The errors in CN10 predictions are sensitive to the choice of the lower size boundary but not to the choice of the time step applied to the microphysical processes. The spatial distribution of CCN(0.2 %) with the 3 nm boundary is almost identical to that with the 1 nm boundary, but that with the 10 nm boundary can differ more than 10-40% in some areas. We found that the deviation in the 10 nm simulations is partly due to the longer time step (i.e., 1 h time step used in the 10 nm simulations compared to 10 min time step used in the benchmark simulations), but, even with the same time step, the 10 nm cutoff showed noticeably higher errors than the 3 nm cutoff. In conclusion, we generally recommend using a lower diameter boundary of 3 nm for studies focused on aerosol indirect effects but down to 1 nm boundary for studies focused on CN10 predictions or nucleation.

microphysics↗

Signatures of aerosol-cloud interactions in GiOcean: a coupled global reanalysis with two-moment cloud microphysics

Aerosols influence the Earth's radiative balance through direct interactions with radiation and by affecting cloud properties. Anthropogenic aerosols have led to cooling during the industrial era through aerosol–cloud interactions (ACI), including aerosol effects on cloud microphysical properties and the subsequent adjustments. However, large uncertainties remain in Earth system models (ESMs) regarding the magnitude of this cooling. In part, ESMs substantially disagree on cloud properties, thermodynamics, the hydrological cycle, and general circulation. Reanalysis provides a useful avenue for exploring the impact of ACI on clouds and radiation because its atmosphere is forced to match realistic conditions through the assimilation of observations. Here, we explore the impact of ACI on clouds in the GiOcean reanalysis – the first to incorporate aerosol-cloud interactions. We contrast variables important for ACI between GiOcean and satellite observations and develop 2-dimensional lookup tables of ACI for both using a source-sink budget perspective to attribute the changes in cloud droplet number (Nd) and liquid water path (LWP) to aerosol and meteorology. A compositing analysis using lookup tables shows that GiOcean captures key aspects of aerosol–cloud–precipitation interactions, including (1) activation of aerosol into cloud droplets, (2) effective precipitation scavenging of Nd, (3) suppression of precipitation by high Nd in regions with heavy aerosol emissions. In contrast, satellite observations do not exhibit clear patterns for processes (2) and (3). Random Forest analysis shows that interannual variability in Nd and LWP over the Northern Hemisphere ocean in GiOcean is primarily driven by precipitation, consistent with satellite observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Improving the Performance of the OMPS Limb Profiling Instrument in Monitoring Aerosols in the Post-Pinatubo Stratosphere

The OMPS Limb Profiling (LP) instrument was launched on NOAA's Suomi NPP (SNPP) weather satellite in October 2011. The instrument measures limb-scattered radiation in the ultraviolet, visible and NIR wavelengths with high vertical resolution (~2 km) and relatively dense spatial and temporal sampling (several thousand measurements/day covering the entire sunlit globe). These measurements have very high sensitivity to stratospheric aerosols due to long path of the incoming solar photons through the aerosol layer. However, unlike the recently launched ISS/SAGE III that directly measures extinction of solar/lunar radiation by gases and particles along the line of sight (LOS) of the instrument, information content of OMPS LP measurements is complex. It consists of solar radiation singly scattered and attenuated by aerosols, air, and trace gases along the LOS of the instrument, as well as diffuse upwelling radiation from the lower atmosphere that also gets scattered and attenuated into the LOS. To unscramble this complex signal one needs to have good knowledge of aerosol size distribution (ASD) and their complex refractive index. We will describe our recent efforts in constraining the ASD parameters by analyzing in-situ balloon data from Laramie, Wyoming; aerosol microphysical model data from CARMA; and spectral information provided by OMPS LP. We will also discuss our proposed methodology to refine this information by adjusting the microphysical properties of the aerosols to make data from various occultation and scattering instruments internally consistent. This is a generalized version of the technique employed by AERONET in which solar extinction data are combined with scattered radiation measured by the almucantar technique to determine aerosol particle shape, complex refractive index and size distribution. We suggest that such closure studies are essential to develop confidence in space-based data to validate aerosol microphysical models, such as CARMA, and aerosol chemistry- transport models, such as GOCART, and for estimating radiative forcing due to stratospheric aerosols in both volcanic and quiescent time periods.

Bhartia, P. K.↗

A Satellite-Based Estimate of Combustion Aerosol Cloud Microphysical Effects over the Arctic Ocean

Climate predictions for the rapidly changing Arctic are highly uncertain, largely due to a poor understanding of the processes driving cloud properties. In particular, cloud fraction (CF) and cloud phase (CP) have major impacts on energy budgets, but are poorly represented in most models, often because of uncertainties in aerosol–cloud interactions. Here, we use over 10 million satellite observations coupled with aerosol transport model simulations to quantify large scale microphysical effects of aerosols on CF and CP over the Arctic Ocean during polar night, when direct and semi-direct aerosol effects are minimal. Combustion aerosols over sea ice are associated with very large (~10W/sq.m) differences in longwave cloud radiative effects at the sea ice surface. However, co-varying meteorological changes on factors such as CF likely explain the majority of this signal. For example, combustion aerosols explain at most 40% of the CF differences between the full dataset and the clean-condition subset, compared to between 57% and 91% of the differences that can be predicted by co-varying meteorology. After normalizing for meteorological regime, aerosol microphysical effects have small but significant impacts on CF, CP, and precipitation frequency on an Arctic-wide scale. These effects indicate that dominant aerosol–cloud microphysical mechanisms are related to the relative fraction of liquid-containing clouds, with implications for a warming Arctic.

Zamora, Lauren M.↗

Sensitivity of Multiangle Imaging to the Optical and Microphysical Properties of Biomass Burning Aerosols

The treatment of biomass burning (BB) carbonaceous particles in the Multiangle Imaging SpectroRadiometer (MISR) Standard Aerosol Retrieval Algorithm is assessed, and algorithm refinements are suggested, based on a theoretical sensitivity analysis and comparisons with near-coincident AERONET measurements at representative BB sites. Over the natural ranges of BB aerosol microphysical and optical properties observed in past field campaigns, patterns of retrieved Aerosol Optical Depth (AOD), particle size, and single scattering albedo (SSA) are evaluated. On the basis of the theoretical analysis, assuming total column AOD of 0.2, over a dark, uniform surface, MISR can distinguish two to three groups in each of size and SSA, except when the assumed atmospheric particles are significantly absorbing (mid-visible SSA approx.0.84), or of medium sizes (mean radius approx.0.13 pin); sensitivity to absorbing, medium-large size particles increases considerably when the assumed column AOD is raised to 0.5. MISR Research Aerosol Retrievals confirm the theoretical results, based on coincident AERONET inversions under BB-dominated conditions. When BB is externally mixed with dust in the atmosphere, dust optical model and surface reflection uncertainties, along with spatial variability, contribute to differences between the Research Retrievals and AERONET. These results suggest specific refinements to the MISR Standard Aerosol Algorithm complement of component particles and mixtures. They also highlight the importance for satellite aerosol retrievals of surface reflectance characterization, with accuracies that can be difficult to achieve with coupled surface-aerosol algorithms in some higher AOD situations.

Chen, Wei-Ting↗

Remote Sensing of Aerosol in the Terrestrial Atmosphere from Space: New Missions

The distribution and properties of atmospheric aerosols on a global scale are not well known in terms of determination of their effects on climate. This mostly is due to extreme variability of aerosol concentrations, properties, sources, and types. Aerosol climate impact is comparable to the effect of greenhouse gases, but its influence is more difficult to measure, especially with respect to aerosol microphysical properties and the evaluation of anthropogenic aerosol effect. There are many satellite missions studying aerosol distribution in the terrestrial atmosphere, such as MISR/Terra, OMI/Aura, AVHHR, MODIS/Terra and Aqua, CALIOP/CALIPSO. To improve the quality of data and climate models, and to reduce aerosol climate forcing uncertainties, several new missions are planned. The gap in orbital instruments for studying aerosol microphysics has arisen after the Glory mission failed during launch in 2011. In this review paper, we describe several planned aerosol space missions, including the Ukrainian project Aerosol-UA that obtains data using a multi-channel scanning polarimeter and wide-angle polarimetric camera. The project is designed for remote sensing of the aerosol microphysics and cloud properties on a global scale.

Aerosol↗