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At least 19 records

Southern Hemisphere tropospheric aerosol microphysics

Aerosol particle-size distribution data have been obtained in the Southern Hemisphere from approximately 4-deg S to 44-deg S and between ground level and 5 km, in the vicinity of eastern Australia. The relative shape of the free-tropospheric size distribution for particles with radii larger than approximately 0.04 micron was found to be remarkably stable with time, altitude, and location for the autumn-winter periods considered. This was despite some large concentration changes, which were found to be typical of the southeastern Australian coastal region. The majority of free-troposphere large particles were found to have sulfuric acid or lightly ammoniated sulfate morphology. Large particles in the boundary layer almost exclusively had a sea-salt morphology.

Gras, John L.↗

Three Years of Airborne Observations During NASA Activate: A Statistical Summary of Chemical, Optical, and Microphysical Aerosol Properties Over the Western North Atlantic Ocean

Airborne observations are critical to understanding Earth’s climate system and surface-level air quality by providing both spatial and vertical information that is not possible through ground measurement networks or satellite observations. Airborne platforms allow assessments of long-range transport, vertical redistribution, boundary-layer dynamics, and cloud-aerosol-interactions that are critical to model evaluation and satellite validation. Still, the high cost and effort of aircraft operations can limit measurement campaigns to short, focused time periods. Multiple deployments are often necessary for seasonal comparisons, and results can be limited if target phenomenon are infrequent. Subsequent analyses typically focus on case studies, especially if deployment conditions are climatologically anomalous. The NASA ACTIVATE (Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment) mission was designed to overcome these limitations by operating semi-continuously over multiple months during multiple seasons. Flight plans were intentionally simple, repetitive, and systematic to provide a statistically robust dataset that could be utilized similarly to a ground-network. Here, we present an overview of three years (2020-2022) of aerosol measurements from the NASA HU-25 Falcon aircraft supporting the ACTIVATE mission. Data from 179 flights were considered, the majority of which were based at NASA Langley Research Center and flown locally over the Wester North Atlantic Ocean just east of Hampton, VA, USA. Airmass characteristics tended to transition from continental outflow near the coast to mostly marine over the open ocean. Seasonal, diurnal, spatial, and vertical trends in aerosol microphysical, optical, and chemical properties are discussed in the context of synoptic scale meteorology. Statistical benefits of the ACTIVATE sampling strategy are discussed with regard to future model evaluation.

Luke D Ziemba↗

Intercomparison of Pulsed Lidar Data with Flight Level CW Lidar Data and Modeled Backscatter from Measured Aerosol Microphysics Near Japan and Hawaii

Aerosol backscatter coefficient data were examined from two nights near Japan and Hawaii undertaken during NASA's Global Backscatter Experiment (GLOBE) in May-June 1990. During each of these two nights the aircraft traversed different altitudes within a region of the atmosphere defined by the same set of latitude and longitude coordinates. This provided an ideal opportunity to allow flight level focused continuous wave (CW) lidar backscatter measured at 9.11-micron wavelength and modeled aerosol backscatter from two aerosol optical counters to be compared with pulsed lidar aerosol backscatter data at 1.06- and 9.25-micron wavelengths. The best agreement between all sensors was found in the altitude region below 7 km, where backscatter values were moderately high at all three wavelengths. Above this altitude the pulsed lidar backscatter data at 1.06- and 9.25-micron wavelengths were higher than the flight level data obtained from the CW lidar or derived from the optical counters, suggesting sample volume effects were responsible for this. Aerosol microphysics analysis of data near Japan revealed a strong sea-salt aerosol plume extending upward from the marine boundary layer. On the basis of sample volume differences, it was found that large particles were of different composition compared with the small particles for low backscatter conditions.

Cutten, D. R.↗

Global Influence of Organic Aerosol Volatility on Aerosol Microphysical Processes: Composition and Number

We present MATRIX-VBS, a new aerosol scheme that simulates organic partitioning in an aerosol microphysics model, as part of the NASA GISS ModelE Earth System Model. MATRIX-VBS builds on its predecessor aerosol microphysics model MATRIX (Bauer et al., 2008, https://doi.org/10.5194/acp-8-6003-2008) and was developed in the box model framework (Gao et al., 2017, https://doi.org/10.5194/gmd-10-751-2017). The scheme features the inclusion of organic partitioning between the gas and particle phases and the photochemical aging process using the volatility-basis set (Donahue et al., 2006, https://doi.org/10.1021/es052297c). To assess the performance of the new model, we compared its mass concentration, number concentration, and activated number concentration to the original scheme MATRIX, and evaluated its mass concentrations in four seasons against data from the NASA Atmospheric Tomography Mission (ATom) aircraft campaign. Results from MATRIX-VBS show that organics are transported further away from their source, and their mass concentration increases aloft and decreases at the surface compared to those in MATRIX. The mass concentration of organics at the surface agrees well with measurements, and there are discrepancies for vertical profiles aloft. In the new scheme, the global mass load of organic aerosols increased by 50%, there is also an increased number of particles at the surface and fewer activated ones in most regions. The new scheme presents advanced and more comprehensive capability in simulating aerosol processes.

aerosol modeling↗

Retrievals of Aerosol Microphysics from Simulations of Spaceborne Multiwavelength Lidar Measurements

In support of the Aerosol, Clouds, Ecosystems mission, simulations of a spaceborne multiwavelength lidar are performed based on global model simulations of the atmosphere along a satellite orbit track. The yield for aerosol microphysical inversions is quantified and comparisons are made between the aerosol microphysics inherent in the global model and those inverted from both the model's optical data and the simulated three backscatter and two extinction lidar measurements, which are based on the model's optical data. We find that yield can be significantly increased if inversions based on a reduced optical dataset of three backscatter and one extinction are acceptable. In general, retrieval performance is better for cases where the aerosol fine mode dominates although a lack of sensitivity to particles with sizes less than 0.1 microns is found. Lack of sensitivity to coarse mode cases is also found, in agreement with earlier studies. Surface area is generally the most robustly retrieved quantity. The work here points toward the need for ancillary data to aid in the constraints of the lidar inversions and also for joint inversions involving lidar and polarimeter measurements.

aerosols↗

PACE Microphysical Aerosol Properties from Polarimetry (PACE-MAPP)

We present the Plankton, Aerosols, Clouds and Ecosystems Microphysical Aerosol Properties from Polarimetry (PACE-MAPP) polarimetric remote sensing algorithm developed for the newly launched NASA PACE satellite observing system. The objective of PACE-MAPP is to retrieve detailed fine-mode (marine, pollution and smoke) and coarse-mode (sea-salt and dust) aerosol properties over the ocean for a range of light to heavy aerosol loadings using PACE’s polarimetric-imaging capabilities at multiple angles and wavelengths from the ultraviolet (UV) to the near-infrared (NIR). An additional objective for PACE-MAPP is to discriminate aerosols from thin clouds. The PACE-MAPP polarimetric remote sensing retrieval algorithm uses coupled atmosphere-ocean vector radiative transfer, optimal estimation, artificial intelligence and powerful inherent optical property look-up-tables for the Earth’s aerosol, cloud, and hydrosol particles. PACE-MAPP is the only retrieval algorithm designed to invert aerosol/ocean products using both polarimeters onboard PACE. We present results using PACE-MAPP to retrieve aerosol and ocean remote sensing products from measurements by the Hyper-Angular Rainbow Polarimeter #2 (HARP2) and Spectro-polarimeter for Planetary Exploration one (SPEXone) polarimeter instruments onboard PACE.

Snorre Stamnes↗

Spatial Distribution of Aerosol Microphysical and Optical Properties and Direct Radiative Effect from the China Aerosol Remote Sensing Network

Multi-year observations of aerosol microphysical and optical properties, obtained through ground-based remote sensing at 50 China Aerosol Remote Sensing Network (CARSNET) sites, were used to characterize the aerosol climatology for representative remote, rural, and urban areas over China to assess effects on climate. The annual mean effective radii for total particles (ReffT) decreased from north to south and from rural to urban sites, and high total particle volumes were found at the urban sites. The aerosol optical depth at 440 nm (AOD440 nm) increased from remote and rural sites (0.12) to urban sites (0.79), and the extinction Ångström exponent (EAE440–870 nm) increased from 0.71 at the arid and semi-arid sites to 1.15 at the urban sites, presumably due to anthropogenic emissions. Single-scattering albedo (SSA440 nm) ranged from 0.88 to 0.92, indicating slightly to strongly absorbing aerosols. Absorption AOD440 nm values were 0.01 at the remote sites versus 0.07 at the urban sites. The average direct aerosol radiative effect (DARE) at the bottom of atmosphere increased from the sites in the remote areas (−24.40 W m−2) to the urban areas (−103.28 W m−2), indicating increased cooling at the latter. The DARE for the top of the atmosphere increased from −4.79 W m−2 at the remote sites to −30.05 W m−2 at the urban sites, indicating overall cooling effects for the Earth–atmosphere system. A classification method based on SSA440 nm, fine-mode fraction (FMF), and EAE440–870 nm showed that coarse-mode particles (mainly dust) were dominant at the rural sites near the northwestern deserts, while light-absorbing, fine-mode particles were important at most urban sites. This study will be important for understanding aerosol climate effects and regional environmental pollution, and the results will provide useful information for satellite validation and the improvement of climate modelling.

Huizheng Che↗

MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

volatility-basis set↗

MATRIX-VBS Condensing Organic Aerosols in an Aerosol Microphysics Model

The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

Aerosols↗

A Global Modeling Study on Carbonaceous Aerosol Microphysical Characteristics and Radiative Effects

Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.

Bauer, S. E.↗

Simulations of Aerosol Microphysics in the NASA GEOS-5 Model

Aerosol-cloud-chemistry interactions have potentially large but uncertain impacts on Earth's climate. One path to addressing these uncertainties is to construct models that incorporate various components of the Earth system and to test these models against data. To that end, we have previously incorporated the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) module online in the NASA Goddard Earth Observing System model (GEOS-5). GEOS-5 provides a platform for Earth system modeling, incorporating atmospheric and ocean general circulation models, a land surface model, a data assimilation system, and treatments of atmospheric chemistry and hydrologic cycle. Including GOCART online in this framework has provided a path for interactive aerosol-climate studies; however, GOCART only tracks the mass of aerosols as external mixtures and does not include the detailed treatments of aerosol size distribution and composition (internal mixtures) needed for aerosol-cloud-chemistry-climate studies. To address that need we have incorporated the Community Aerosol and Radiation Model for Atmospheres (CARMA) online in GEOS-5. CARMA is a sectional aerosol-cloud microphysical model, capable of treating both aerosol size and composition explicitly be resolving the aerosol distribution into a variable number of size and composition groupings. Here we present first simulations of dust, sea salt, and smoke aerosols in GEOS-5 as treated by CARMA. These simulations are compared to available aerosol satellite, ground, and aircraft data and as well compared to the simulated distributions in our current GOCART based system.

Colarco, Peter↗

Optimized Profile Retrievals of Aerosol Microphysical Properties from Simulated Spaceborne Multiwavelength Lidar

This work is an expanded study of one previously published onretrievals of aerosol microphysical properties from space-borne multiwavelengthlidarmeasurements. The earlier studiesand this one weredone in the framework of the NASA Aerosol-Clouds-Ecosystems (now the Aerosol Clouds Convection and Precipitation) NASA mission. The focus here is on the capabilities of a simulated spacebornemultiwavelengthlidar system for retrieving aerosol complex refractive index (m = mr+ imi) and spectral single scattering albedo (SSA(λ)), although other bulk parameters such as effective (reff) radius and particle volume (V) and surface (S) concentrations are also studied. The novelty presented here is the use of recently published, case dependent optimized-constraints on the microphysical retrievals using three backscattering coefficients (β) at 355, 532 and 1064 nm and two extinction coefficients (α) at 355 and 532 nm, typically known as the stand-alone 3β+2α lidar inversion. Case-dependent optimized-constraints (CDOC) limit the ranges of refractive index, both real (mr) and imaginary (mi) parts, and of radii that are permitted in the retrievals. Such constraints are selected directly from the 3β+2α41measurements through an analysis of the relationship between spectral dependence of aerosol extinction-to-backscatter ratios (LR) and the Ångström exponent of extinction. The analyses presented here for different sets ofsize distributions and refractive indices reveal that the direct determination of CDOCareonly feasible for cases where the uncertaintiesin the input optical data areless than 15 %.Forthe same simulated spacebornesystem and yield than in Whiteman et al., (2018), we demonstrated that the use of CDOC as essential for the retrievals of refractive index and also largely improved retrieval of bulk parameters. A discussion of the global representativeness of CDOC is presented using simulated lidar data from a 24-hour satellite track using GEOS model output to initialize the lidar simulator.We found that CDOCare representative of many aerosol mixtures in spite of some outliers (e.g. highly hydrated particles) associatedwith the assumptions of bimodal size distributions and of the same refractive index for fine and coarse modes. Moreover, sensitivity tests performed using synthetic data reveal that retrievals of imaginary refractive index (mi) and SSA are extremely sensitive to β(355).

NASA Aerosol-Clouds-Ecosystems↗

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↗