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At least 181 records · Page 10

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↗

A history of Mars atmospheric opacity in the southern hemisphere during the Viking extended mission

A history of developing opacity in the Mars southern hemisphere during the Viking extended mission has been compiled using orbiter images obtained at high altitude. Observations of changing contrasts under similar viewing conditions have been modeled by multiple-scattering intensity transfer equations that have produced a temporal description of changes in optical depth and particle-scattering properties within a network of control points. The results are presented in the form of Mercator and perspective plots for various dates.

Thorpe, T. E.↗

Mars Odyssey THEMIS-VIS: Surface-Atmosphere Separation and Derivation of Aerosol Properties

Scattering by atmospheric aerosols can contribute a substantial fraction of the visible-light radiance observed in any remote sensing of Mars. Our objective is to develop techniques to separate this aerosol component from the surface-reflectance component in Mars Odyssey's THEMIS Visible Imaging Subsystem (THEMIS-VIS) dataset. The primary purpose of this study is the production of accurate surface reflectance data in order to allow for reliable color and mineralogical unit mapping. The second principal goal is to study the feasibility of using VIS measurements to derive quantitative information about ice and dust aerosol properties such as particle size and optical depth.

T H McConnochie↗

The Earth Surface Mineral Dust Source Investigation: An Earth Science Imaging Spectroscopy Mission

The Earth Surface Mineral Dust Source Investigation, EMIT, is planned to operate from the International Space Station starting no earlier than the fall of 2021. EMIT will use visible to short wavelength infrared imaging spectroscopy to determine the mineral composition of the arid land dust source regions of the Earth to advance our knowledge of the radiative forcing effect of these aerosols. Mineral dust emitted into the atmosphere under high wind conditions is an element of the Earth system with many impacts to the Earth’s energy balance, atmosphere, surface, and oceans. The Earth’s mineral dust cycle with source, transport, and deposition phases are studied with advanced Earth System Models. Because the chemical composition, optical and surface properties of soil particles vary strongly with the mineral composition of the source, these models require knowledge of surface soil mineral dust source composition knowledge to accurately understand dust impacts on the Earth system now and in the future. At present, compositional knowledge of the Earth’s mineral dust source regions from existing data sets is uncertain as a result of limited measurements. EMIT will use spectroscopically derived surface mineral composition to update the prescribe boundary conditions for state-of-the-art Earth System Models. The EMIT-initialized models will be used to investigate the impact of direct radiative forcing in the Earth system that depends strongly on the composition of the mineral dust aerosols emitted into the atmosphere. These new measurements and related products will be used to address the EMIT science objectives and made available to the science community for additional investigations. An overview of the EMIT science, development, and mission is presented in this paper.

Green, Robert O.↗

What we can Learn About Aerosols from EOS-MISR Multi-Angle Remote Sensing Observations

Multiangle, multispectral remote sensing observations, such as those anticipated from the Earth Observing System (EOS) Multiangle Imaging SpectroRadiometer (MISR), promise to significantly improve our ability to constrain aerosol properties from space. Recent advances in modeling the Earth's climate have brought us to a point where the contributions made by aerosols to the global radiation budget noticeably affect the results. Knowledge of both aerosol optical depth and the microphysical properties of particles is needed to adequately model aerosol effects. This talk explores the ability of multiangle, multi-spectral remote sensing observations anticipated from the EOS MISR instrument, to retrieve aerosol optical depth and information about mixes of particle types, globally, at 17.6 km spatial resolution. The instrument is scheduled for launch into a 10:30 AM, sun-synchronous polar orbit in 1999.

Kahn, Ralph↗

MISR Level 2 Aerosol parameters (MIL2ASAE_V1)

The Aerosol data contain aerosol optical depth, aerosol physical model, ancillary meteorological data, and related parameters. The aerosol data include tropospheric aerosol optical depth, Angstrom exponent and single scattering albedo on 17.6 km centers, aerosol mixture identifier and retrieval residuals, and ancillary data including assumed ozone optical depth and retrieval flags. For complete information about the aerosol mixtures, the user will need to order the MISR Aerosol Climatology Product (MIANACP) to obtain Aerosol Physical and Optical Properties (APOP) and the Mixture files. The Mixture files list up to 3 component models used in each mixture, with their relative compositional fractions, and includes ancillary information such as single scattering albedo. The APOP gives detailed information for the component particle models. [Location=GLOBAL] [Temporal_Coverage: Start_Date=2000-02-24; Stop_Date=] [Spatial_Coverage: Southernmost_Latitude=-90; Northernmost_Latitude=90; Westernmost_Longitude=-180; Easternmost_Longitude=180] [Data_Resolution: Latitude_Resolution=1.1 km - 17.6 km; Longitude_Resolution=1.1 km - 17.6 km; Horizontal_Resolution_Range=1 km - < 10 km or approximately .01 degree - < .09 degree; Temporal_Resolution=about 15 orbits/day].

CIRRUS OPTICAL DEPTH↗

Semimicroscopic description of isoscalar giant multipole resonances in medium-mass closed-shell nuclei

Main properties of isoscalar giant multipole resonances (up to L=3), including L=0,and 2 overtones, in medium-mass closed-shell nuclei are described within the semimicroscopic particle-hole dispersive optical model. Further, main properties are characterized by the energy-averaged strength distribution, projected (one-body) transition density, and probabilities of direct one-nucleon decay. Calculation results obtained for characteristics of the mentioned resonances in the 48 Ca, 90 Zr, and 132 Sn nuclei are compared with available experimental data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Intensive aerosol properties of boreal and regional biomass burning aerosol at Mt. Bachelor Observatory: larger and black carbon (BC)-dominant particles transported from Siberian wildfires

We characterize the aerosol physical and optical properties of 13 transported biomass burning (BB) events. BB events included long-range influence from fires in Alaskan and Siberian boreal forests transported to Mt. Bachelor Observatory (MBO) in the free troposphere (FT) over 8–14+ d and regional wildfires in northern California and southwestern Oregon transported to MBO in the boundary layer (BL) over 10 h to 3 d. Intensive aerosol optical properties and normalized enhancement ratios for BB events were derived from measured aerosol light scattering coefficients (σ scat ), aerosol light-absorbing coefficients (σ abs ), fine particulate matter (PM 1 ), and carbon monoxide (CO) measurements made from July to September 2019, with particle size distribution collected from August to September. The observations showed that the Siberian BB events had a lower scattering Ångström exponent (SAE), a higher mass scattering efficiency (MSE; Δσ scat /ΔPM 1 ), and a bimodal aerosol size distribution with a higher geometric mean diameter (D g ). We hypothesize that the larger particles and associated scattering properties were due to the transport of fine dust alongside smoke in addition to contributions from condensation of secondary aerosol, coagulation of smaller particles, and aqueous-phase processing during transport. Alaskan and Siberian boreal forest BB plumes were transported long distances in the FT and characterized by lower absorption Ångström exponent (AAE) values indicative of black carbon (BC) dominance in the radiative budget. Significantly elevated AAE values were only observed for BB events with <1 d transport, which suggests strong production of brown carbon (BrC) in these plumes but limited radiative forcing impacts outside of the immediate region.

54 ENVIRONMENTAL SCIENCES↗

Models Transport Saharan Dust too Low in the Atmosphere: a Comparison of the MetUM and CAMS Forecasts with Observations

We investigate the dust forecasts from two operational global atmospheric models in comparison with in situ and remote sensing measurements obtained during the AERosol properties – Dust (AER-D) field campaign. Airborne elastic backscatter lidar measurements were performed on board the Facility for Airborne Atmospheric Measurements during August 2015 over the eastern Atlantic, and they permitted us to characterise the dust vertical distribution in detail, offering insights on transport from the Sahara. They were complemented with airborne in situ measurements of dust size distribution and optical properties, as well as datasets from the Cloud–Aerosol Transport System (CATS) spaceborne lidar and the Moderate Resolution Imaging Spectroradiometer (MODIS). We compare the airborne and spaceborne datasets to operational predictions obtained from the Met Office Unified Model (MetUM) and the Copernicus Atmosphere Monitoring Service (CAMS). The dust aerosol optical depth predictions from the models are generally in agreement with the observations but display a low bias. However, the predicted vertical distribution places the dust lower in the atmosphere than highlighted in our observations. This is particularly noticeable for the MetUM, which does not transport coarse dust high enough in the atmosphere or far enough away from the source.We also found that both model forecasts underpredict coarse-mode dust and at times overpredict fine-mode dust, but as they are fine-tuned to represent the observed optical depth, the fine mode is set to compensate for the underestimation of the coarse mode. As aerosol–cloud interactions are dependent on particle numbers rather than on the optical properties, this behaviour is likely to affect their correct representation. This leads us to propose an augmentation of the set of aerosol observations available on a global scale for constraining models, with a better focus on the vertical distribution and on the particle size distribution. Mineral dust is a major component of the climate system; therefore, it is important to work towards improving how models reproduce its properties and transport mechanisms.

Debbie OSullivan↗

Thermal Characterization of Fe3O4 Nanoparticles Formed from Poorly Crystalline Siderite

Increasing interest in environmental geochemistry has led to the recognition that crystals with sizes in the nanometer range (e.g., colloids and nanoscale precipitates) and poorly crystalline compounds (e.g., ferrihydrites) may comprise the majority of reactive mineral surface area near the Earth s surface. When the diameters of individual particles are in the range of 100 nm or less, the surface energy contribution to the free energy modifies phase stability. This results in stabilization of polymorphs not normally encountered in the macrocrystal domain. These phases potentially have very different surface-site geometries, adsorptive properties, and growth mechanisms, and exhibit size-dependent kinetic behavior. Thus nanophases dramatically modify the physical and chemical properties of soils and sediments. In a more general sense, the characteristics of nanocrystals are of intense technological interest because small particle size confers novel chemical, optical, and electronic properties. Thus, nanocrystalline materials are finding applications as catalytic substrates, gas phase separation materials, and even more importantly in the field of medicine. This is an opportune time for mineral physicists working on nanocrystalline materials to develop collaborative efforts with materials scientists, chemists, and others working on nanophase materials of technological interest (e.g., for magnetic memories). Our objective in this study was to synthesize submicron (<200 nm) magnetite and to study their thermal and particle size properties.

Lauer, H. V., Jr.↗

Modeled Aerosol Optical Properties From Measurement-Based Mixtures of Chemical Species: Assessing the Impacts of Particle Morphology and Absorption

This report serves as the final report for the Colorado State University portion of this grant. The original grant was awarded to CSU under the direction of co-Principal Investigators Kirk Fuller and Sonia Kreidenweis. Upon Dr. Fuller's relocation to the University of Alabama - Huntsville, the major portion of the award was also relocated. The following summarizes only that work completed by Prof. Kreidenweis under her remaining award.

Kreidenweis, Sonia↗

Aerosol Optical Tweezers Elucidate the Chemistry, Acidity, Phase Separations, and Morphology of Atmospheric Microdroplets

Aerosol particles represent unique chemical environments because of their high surface area-to-volume ratio that promotes the effects of interfacial chemistry in confined environments. Properties such as viscosity, diffusivity, water content, pH, and morphology—following liquid–liquid phase separation—can strongly alter how a particle interacts with condensable vapors and reactive trace gases, thus modifying its continual evolution and environmental effects. Our understanding of this chemical evolution of atmospheric particulate matter and its environmental impacts is largely limited by our ability to directly observe how these critical particle properties respond to the addition or reactive uptake of new chemical components. Aerosol optical tweezers (AOT) stably trap particles in focused laser beams, providing positional control and the retrieval of many of these critical properties required to understand and predict the chemistry of aerosolized microdroplets. The analytical power of the AOT stems from the retrieval of the cavity-enhanced Raman spectrum induced by the trapping laser. Analysis of the whispering gallery modes (WGMs) that resonate as a standing wave around the droplet’s interface, provide high accuracy measurements of the droplet’s size, refractive index (and thus a measurement of composition), and can distinguish between core–shell, partially engulfed, and homogeneous morphologies. In this study, we have advanced the ability to determine the properties of the core and shell phases in biphasic droplets, including obtaining high-accuracy pH measurements. These capabilities were applied to perform AOT physical chemistry experiments on authentic secondary organic aerosol (SOA) produced directly in the AOT chamber by ozonolysis of terpene vapors. The propensity of the SOA to phase separate as a shell from a wide range of nonpolar to polar core phases was observed, along with the discovery of a stable emulsified state of SOA particles in an aqueous salt droplet. Micron-thick SOA shells did not impede the gain or loss of water or squalane from the core to the surrounding air, indicating no significant diffusional limitations to condensational growth or partitioning even under dry conditions. These experiments formed the foundation of a new framework that predicts how the phase-separated morphology of complex aerosols containing organic carbon evolves during continual atmospheric oxidation processes. Increases in oxidation state will quickly drive conversion from a partially engulfed to core–shell morphology that has dramatically different chemical reactivity since the core phase is completely concealed by the shell. The recent advances in the experimental capabilities of the AOT technique such as presented here enable novel experimental methodologies that provide insights into the chemistry and multidimensional properties of aerosol microdroplets, and how these coevolve and respond to continual chemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Laser Doppler anemometer diagnostics in unsteady flows

The application of the laser Doppler anemometer (LDA) to unsteady flows is discussed with respect to necessary features of the signal processor, properties of the optical system, and the character of the flow under investigation. The discussion of signal processors includes consideration of frequency trackers, counter-type processors, particle properties, data rates, and statistics. Secondly, diffraction limitations for an optical system are viewed with respect to spatial resolution. Finally, the total velocity field is decomposed into its subfields and the feasibility of, criteria for, and possible types of conditional sampling are defined. Several reported LDA experiments using conditional sampling are presented to demonstrate the different techniques that may be used.

Orloff, K. L.↗

Optical and microphysical properties of a cold cirrus cloud - Evidence for regions of small ice particles

An airborne lidar and a scanning radiometer aboard an ER-2 aircraft were used to observe a cold cirrus cloud, and a Forward Scattering Spectrometer Probe (FSSP) was used to obtain simultaneous in situ microphysical observations at two altitudes within the cloud. Lidar depolarization ratio data show that the clouds were composed predominantly of ice crystals. At an altitude where the temperature was -62.7 C, the lidar and radiometer analysis gave a visible extinction to infrared absorption ratio (alpha) of 2.3, while the cloud microphysics data provided an alpha value of 3.77. The discrepancy is attributed to undersizing of particles by the FSSP. Direct and remote measurements showed better agreement for a lower layer where the temperature was -47.3 C.

Platt, C. M. R.↗

Monitoring and characterization of particle contamination in the pulse compression chamber of the OMEGA EP laser system

The laser-damage performance of optics is known to be negatively affected by microscale particle contamination induced by the operational environment. This work investigates the properties of particles accumulating in various locations near critical optics inside the OMEGA EP grating compressor chamber during quarterly operational periods over a 2-year duration. The particles found were characterized using optical microscopy, scanning electron microscopy and energy dispersive X-ray spectroscopy. The analysis indicates significant concentrations of micrometer- to nanometer-scale particles inside the vacuum chamber, with higher values observed near the port leading to the OMEGA EP target chamber. The distribution of the chemical composition of these particles varies between collection periods. Although understanding of the mechanisms of particle generation and transport remains uncertain, the hypothesis is that this particle load represents a risk for contaminating the surfaces of high-value optics located inside the chamber, including the compression gratings and deformable mirrors, and therefore affecting their laser-damage resistance and overall operational lifetime.

47 OTHER INSTRUMENTATION↗

3+2+X: What Is the Most Useful Depolarization Input for Inverting Lidar Measurements of Non-Spherical Particles to Microphysical Properties?

The typical multiwavelength aerosol lidar data set for inversion of optical to microphysical parameters is composed of three backscatter coefficients (β ) at 355, 532, and 1064 nm and two extinction coefficients (α ) at 355 and 532 nm. This data combination is referred to as 3β +2α or 3+2 data set. This set of data is sufficient for retrieving some important microphysical particle parameters if the particles have spherical shape. Here, we investigate the effect of including the particle linear depolarization ratio (δ) as a third input parameter to the inversion of lidar data. The inversion algorithm is generally not used if measurements show values of δ that exceed 0.10 at 532 nm, i.e. in the presence of non-spherical particles such as desert dust, volcanic ash, and under special circumstances biomass-burning smoke.We use experimental data collected with instruments that are capable of measuring δ at all three lidar wavelengths with an inversion routine that uses the theory of light scattering by randomly oriented spheroids to replicate scattering properties of non-spherical particles. This is the first systematic test of the effect of using all theoretically possible combinations of δ taken at 355, 532, and 1064 nm as input in the lidar data inversion. We find that depolarization information at least at one wavelength already provides useful information in the in version of optical data that describe light-scattering by nonspherical particles. However, any choice of δ(λ) will give lower values of the single-scattering albedo than the traditional 3+2 data set. We find that input data sets that include 355 give a non-spherical fraction that closely resembles the dust ratio we obtain from using β(532) and δ(532) in a methodology applied in aerosol-type separation. The use of 355 in data sets of two or three reduces the fraction of non-spherical particles that is retrieved when using δ(532) and δ(1064). Use of the latter two without accounting for 355 generally leads to high fractions of non-spherical particles that we consider not trustworthy. The use of three δ(λ) instead of two δ(λ) including the constraint that one of these is measured at 355 nm does not provide any advantage over using 3+2+δ(355). Because of the technical challenges involved with accurately measuring δ(1064) we conclude that — depending on measurement capability — the future standard input for inversion using spheroid kernels might be 3+2+δ(355) or 3+2+δ(355)+δ(532).

Tesche, M.↗

The Use of Satellite-Measured Aerosol Optical Depth to Constrain Biomass Burning Emissions Source Strength in a Global Model GOCART

Small particles in the atmosphere, called "atmospheric aerosol" have a direct effect on Earth climate through scattering and absorbing sunlight, and also an indirect effect by changing the properties of clouds, as they interact with solar radiation as well. Aerosol typically stays in the atmosphere for several days, and can be transported long distances, affecting air quality, visibility, and human health not only near the source, but also far downwind. Smoke from vegetation fires is one of the main sources of atmospheric aerosol; other sources include anthropogenic pollution, dust, and sea salt. Chemistry transport models (CTMs) are among the major tools for studying the atmospheric and climate effects of aerosol. Due to the considerable variation of aerosol concentrations and properties on many temporal and spatial scales, and the complexity of the processes involved, the uncertainties in aerosol effects on climate are large, as is featured in the latest report of Intergovernmental Panel on Climate Change (IPCC) in 2007. Reducing this uncertainty in the models is very important both for predicting future climate scenarios and for regional air quality forecasting and mitigation. During vegetation fires, also called biomass burning (BB) events, complex mixture of gases and particles is emitted. The amount of BB emissions is usually estimated taking into account the intensity and size of the fire and the properties of burning vegetation. These estimates are input into CTMs to simulate BB aerosol. Unfortunately, due to large variability of fire and vegetation properties, the quantity of BB emissions is very difficult to estimate and BB emission inventories provide numbers that can differ by up to the order of magnitude in some regions. Larger uncertainties in data input make uncertainties in model output larger as well. A powerful way to narrow the range of possible model estimates is to compare model output to observations. We use satellite observations of aerosol properties, specifically aerosol optical depth, which is directly proportional to the amount of aerosol in the atmosphere, and compare it to the model output. Assuming the model represents aerosol transport and particle properties correctly, the amount of BB emissions determines the simulated aerosol optical depth. In this study, we explore the regional performance of 13 commonly used emission estimates. These are each input to global Goddard Chemistry Aerosol Radiation and Transport (GOCART) model. We then evaluate how well each emission estimate reproduces the smoke aerosol optical depth measured by the MODIS instrument. We compared GOCART-simulate aerosol optical depth with that measured from the satellite for 124 fire cases around the world during 2006 and 2007. We summarize the regional performance of each emission inventory and discuss reasons for their differences by considering the assumptions made during their development. We also show that because stronger wind disperses smoke plumes more readily, in cases with stronger wind, a larger increase in emission amount is needed to increase aerosol optical depth. In quiet, low-wind-speed environments, BB emissions produce a more significant increase in aerosol optical depth, other things being equal. Using the region-specific, quantitative relationships derived in our paper, together with the wind speed obtained from another source for a given fire case, we can constrain the amount of emission required in the model to reproduce the observations. The results of this paper are useful to the developers of BB emission inventories, as they show the strengths and weaknesses of individual emission inventories in different regions of the globe, and also for modelers who use these inventories and wish to improve their model results.

Petrenko, Mariya↗

Understanding Biases in Simulated Cloud Radiative Effects in E3SMv3

This study systematically investigates biases in cloud radiative effects (CREs) within the recently released Energy Exascale Earth System Model version 3 (E3SMv3). Compared to its previous version (E3SMv2), E3SMv3 shows excessively strong shortwave CRE over tropical and subtropical oceans, the Southern Ocean, and the Northern Hemisphere storm tracks, which is primarily caused by an overestimation of optically intermediate low clouds. The model also displays excessive longwave CRE over the Maritime Continent and other tropical deep convection regions, resulting from an overestimation of optically thick high clouds. Implementing the Predicted Particle Properties (P3) scheme for stratiform clouds played the most significant role in these cloud changes. In addition, using a double-moment scheme for convective clouds contributed to the increase in intermediate low clouds and optically thick clouds in tropical deep convection regions. Error metrics for total cloud amount (E TCA ), cloud properties (E ctp-τ ), and cloud properties weighted by their SW and LW radiative impacts (E SW and E LW ) indicate that E3SMv3's ability to reproduce observed cloud radiative effect of low, middle, and high clouds has not been improved compared to E3SMv2. Nevertheless, the performance of E3SMv3 remains well within the spread of CMIP6 models, with E SW and E LW values smaller than those in most CMIP6 models. This study underscores the importance of integrating diverse satellite observations for robust cloud evaluation and using cloud-radiation relationships as consistency check for model errors. It suggests that further model developments focus on improving cloud microphysics and their interactions with radiation.

Environmental sciences↗