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At least 199 records · Page 11

Preferential concentration of certain elements in smaller aerosols emitted from aircraft engines

Aerosols from aircraft engines were collected with an eight-stage cascade sampler for a period of 24 h. The aerosol samples from each stage were analyzed for their elemental composition using the proton-induced X-ray emission (PIXE) technique. Seventeen elements (Si, P, S, Cl, K, Ca, Ti, V, Fe, Ni, Cu, Zn, Br, Sr, Nb, Sn, and Pb) were positively identified and quantitated at each stage. Six elements (S, Ca, Fe, Zn, Sn, and Pb) showed a fractional concentration increase with decreasing aerosol size. Similar, but less well-defined, trends were also observed for V and Ni. Silicon and chlorine, on the other hand, showed an opposite trend. Neutron-activation analysis of bulk aerosol samples collected every 2 h over the same period showed a correlation between concentration of Si, Ca, V, Ti, Zn, Br, and Sn and the density of air traffic at the airport. Analysis of the aviation-fuel samples by PIXE indicates that major fractions of Pb, Sn, Br, Zn, Ni, Fe, V, Ca, and S observed in these aerosol studies come from the aircraft engine exhaust.

Jolly, R. K.↗

Aerosol Lidar and MODIS Satellite Comparisons for Future Aerosol Loading Forecast

Knowledge of the concentration and distribution of atmospheric aerosols using both airborne lidar and satellite instruments is a field of active research. An aircraft based aerosol lidar has been used to study the distribution of atmospheric aerosols in the California Central Valley and eastern US coast. Concurrently, satellite aerosol retrievals, from the MODIS (Moderate Resolution Imaging Spectroradiometer) instrument aboard the Terra and Aqua satellites, were take over the Central Valley. The MODIS Level 2 aerosol data product provides retrieved ambient aerosol optical properties (e.g., optical depth (AOD) and size distribution) globally over ocean and land at a spatial resolution of 10 km. The Central Valley topography was overlaid with MODIS AOD (5x5 sq km resolution) and the aerosol scattering vertical profiles from a lidar flight. Backward air parcel trajectories for the lidar data show that air from the Pacific and northern part of the Central Valley converge confining the aerosols to the lower valley region and below the mixed layer. Below an altitude of 1 km, the lidar aerosol and MODIS AOD exhibit good agreement. Both data sets indicate a high presence of aerosols near Bakersfield and the Tehachapi Mountains. These and other results to be presented indicate that the majority of the aerosols are below the mixed layer such that the MODIS AOD should correspond well with surface measurements. Lidar measurements will help interpret satellite AOD retrievals so that one day they can be used on a routine basis for prediction of boundary layer aerosol pollution events.

DeYoung, Russell↗

In Situ Aerosol Optical Thickness Collected by the SIMBIOS Program (1997-2000): Protocols, and and Data QC and Analysis

The purpose of this technical report is to provide current documentation of the Sensor Intercomparison and Merger for Biological and Interdisciplinary Oceanic Studies (SIMBIOS) Project Office activities on in situ aerosol optical thickness (i.e., protocols, and data QC and analysis). This documentation is necessary to ensure that critical information is related to the scientific community and NASA management. This critical information includes the technical difficulties and challenges of validating and combining ocean color data from an array of independent satellite systems to form consistent and accurate global bio-optical time series products. This technical report is not meant as a substitute for scientific literature. Instead, it will provide a ready and responsive vehicle for the multitude of technical reports issued by an operational project.

Fargion, Giulietta S.↗

A single-photon lidar observes atmospheric clouds at decimeter scales: resolving droplet activation within cloud base

Abstract Clouds, crucial for understanding climate, begin with droplet formation from aerosols, but observations of this fleeting activation step are lacking in the atmosphere. Here we use a time-gated time-correlated single-photon counting lidar to observe cloud base structures at decimeter scales. Results show that the air–cloud interface is not a perfect boundary but rather a transition zone where the transformation of aerosol particles into cloud droplets occurs. The observed distributions of first-arriving photons within the transition zone reflect vertical development of a cloud, including droplet activation and condensational growth. Further, the highly resolved vertical profile of backscattered photons above the cloud base enables remote estimation of droplet concentration, an elusive but critical property to understanding aerosol–cloud interactions. Our results show the feasibility of remotely monitoring cloud properties at submeter scales, thus providing much-needed insights into the impacts of atmospheric pollution on clouds and aerosol-cloud interactions that influence climate.

54 ENVIRONMENTAL SCIENCES↗

Stellar Energetic Particle-driven Production of Biologically Relevant Molecules in Atmospheres of Young Earth-like Exoplanets Around Active G-K Stars

The chemistry of N2, CO2, CH4-rich atmospheres of terrestrial-type exoplanets around active G-K stars is a complex problem: the star's ionizing radiation in the form of X-ray and Extreme UV radiation and the precipitating energetic particles accelerated in coronal mass ejection driven shocks can drive complex chemistry in the exoplanetary atmosphere, and ignite the production of complex molecules (Airapetian et al., 2016). We developed a set of atmospheric models to simulate the formation of organic molecules that can be considered as atmospheric pre-biosignatures from exoplanets around active stars. The model has recently been extended to account for the production of ions, their role in the enhanced chemistry in the lower atmosphere, as well as the interaction of these ions with the aerosols. We applied the photochemical-collisional model to simulate the chemistry of a young terrestrial-type exoplanets resembling the Hadean Earth to highlight the creation of atmospheric pre-biosignatures, relevant greenhouse gases, and the presence of aerosols driven by stellar activity sources. We also discuss the impact of that modified atmospheric chemistry on the exoplanetary climate.

Guillaume Philippe Gronoff↗

Development and testing of a continuous maritime monitor for radionuclide aerosols

Monitoring airborne concentrations of radionuclide activity may provide a timely warning to sea-based assets to avoid contamination from a radioactive plume. The development and testing of an automated aerosol monitoring system that can capture and detect radioactive particulate from marine air is presented. A custom electrostatic precipitator (ESP) was designed to capture particulate onto a reusable collection media. The collection efficiency of the ESP system for radon progeny was determined to be ~23%. A conservative calculation of the minimum detectable concentration of 214 Bi was estimated as 0.3-8 Bq/m 3 . The system was demonstrated in continuous operation, without consumables and limited maintenance, in a marine environment at the PNNL campus in Sequim, Washington. In conclusion, a successful 2-month deployment indicates the feasibility of the approach for continuous maritime monitoring for radionuclide aerosols.

Moore, Michael E. [Pacific Northwest National Labo↗

Circular Polarization in Atmospheric Aerosols

Recent technological advances have demonstrated the feasibility of deploying spaceborne optical detectors with full polarimetric capabilities. The measurement of all four Stokes coefficients opens significant new opportunities for atmospheric aerosol studies and applications. While considerable amounts of attention have been dedicated to sensors with sensitivity to the total intensity and linear polarization (represented by Stokes coefficients I, U, Q), there has been less attention to the additional information brought by measuring circular polarization (coefficient V). This report fills this gap in knowledge by providing an overview of aerosol sources of circular polarization in the atmosphere and discusses possible remote sensing signatures. In this manuscript, circularly polarized radiation that results from the interaction of incident unpolarized radiation are considered in three physical settings: optical activity originating in biogenic aerosols, alignment of non-spherical particles in the presence of electrical fields (such as dust, smoke, and volcanic ash) and aerosol multiple scattering effects. Observational and theoretical evidence of, and the settings and conditions for non-zero aerosol circular polarization generated from incident unpolarized radiation are here gathered and discussed. In addition, novel radiative transfer simulations are shown to illustrate notable spectral and other features where circular polarization may provide additional information that is possibly independent from total intensity and linear polarization only observations. Current techniques for detection of aerosol composition (also referred as aerosol type) from space provide limited information. Remote identification of aerosols such as smoke, volcanic ash, and dust particles can only be accomplished with some degree of confidence for moderate to high concentrations. When the same aerosols are found at lower concentrations (but still high enough to be of importance for air quality and cloud formation), these methods often produce ambiguous results. The circular polarization of aerosols is rarely utilized, and we explore its value for improved determination aerosol composition. This study is presented as an overview with a goal to provide a new perspective on an overlooked optical property and to trigger interest in further exploration of this subject.

Aerosol type↗

Polarimeter + Lidar–Derived Aerosol Particle Number Concentration

In this study, we propose a simple method to derive vertically resolved aerosol particle number concentration (Na) using combined polarimetric and lidar remote sensing observations. This method relies on accurate polarimeter retrievals of the fine-mode column-averaged aerosol particle extinction cross section and accurate lidar measurements of vertically resolved aerosol particle extinction coefficient such as those provided by multiwavelength high spectral resolution lidar. We compare the resulting lidar + polarimeter vertically resolved N(a) product to in situ N(a) data collected by airborne instruments during the NASA aerosol cloud meteorology interactions over the western Atlantic experiment (ACTIVATE). Based on all 35 joint ACTIVATE flights in 2020, we find a total of 32 collocated in situ and remote sensing profiles that occur on 11separate days, which contain a total of 322 cloud-free vertically resolved altitude bins of 150 m resolution. We demonstrate that the lidar + polarimeter N(a) agrees to within 106% for 90% of the 322 vertically resolved points. We also demonstrate similar agreement to within 121% for the polarimeter-derived column-averaged N(a). We find that the range-normalized mean absolute deviation (NMAD) for the polarimeter-derived column-averaged Na is 21%, and the NMAD for the lidar + polarimeter-derived vertically resolved Na is 16%. Taken together, these findings suggest that the error in the polarimeter-only column-averaged N(a) and the lidar + polarimeter vertically resolved N(a) are of similar magnitude and represent a significant improvement upon current remote sensing estimates of N(a).

RSP↗

Cloud and Radiation Mission with Active and Passive Sensing from the Space Station

A cloud and aerosol radiative forcing and physical process study involving active laser and radar profiling with a combination of passive radiometric sounders and imagers would use the space station as an observation platform. The objectives are to observe the full three dimensional cloud and aerosol structure and the associated physical parameters leading to a complete measurement of radiation forcing processes. The instruments would include specialized radar and lidar for cloud and aerosol profiling, visible, infrared and microwave imaging radiometers with comprehensive channels for cloud and aerosol observation and specialized sounders. The low altitude,. available power and servicing capability of the space station are significant advantages for the active sensors and multiple passive instruments.

Spinhirne, James D.↗

Characterization and Measurement of Spacecraft Airborne Particulate Matter

The International Space Station (ISS) gives a 6-member astronaut crew the ability to live and work in low Earth orbit. It is a unique indoor environment, which has served as both home and workplace to over 230 people since the year 2000. In this low gravity environment, smoke does not rise and cookie crumbs do not settle the way they do on Earth, causing airborne particulate matter, or aerosols, to behave differently and pose unique hazards for crew members. In its existence, virtually the same volume of ISS air has been continuously conditioned and ‘revitalized,’ including the removal of particles by filtration. While gaseous constituents of ISS air are monitored meticulously, sparse data exists on the indoor aerosols. The quantity and types of ISS airborne debris have been investigated in NASA’s Aerosol Sampling Experiment. Both active and passive samplers successfully collected airborne particulate matter in U.S. segments of the ISS, which were returned to Earth for characterization by microscopy and other techniques. The resulting data has informed the design of candidate particle instruments for spacecraft. In 2020, a reference-quality aerosol instrument will be flown to ISS, and will provide real-time data of particle concentrations in various modules. Smaller, more compact instruments will be necessary in future space missions, for example, in smaller vehicles, in habitats on lunar and planetary surfaces with ubiquitous dust, and also for use as wearable technology throughout missions. Miniaturized aerosol sensors, though lower fidelity than reference-quality instruments, can monitor the environment well when calibrated appropriately. Indoor air quality in spacecraft is fundamentally important to human health and comfort, and several particulate monitoring technologies will be at sufficient technology readiness levels for operational use within the next two years. Results of the Aerosol Sampling Experiment will be presented, along with the status of NASA’s aerosol instrument technology demonstrations on ISS.

Meyer, Marit E.↗

Modeling Macro- and Micro-Scale Turbulent Mixing and Chemistry in Engine Exhaust Plumes

Simulation of turbulent mixing and chemical processes in the near-field plume and plume-vortex regimes has been successfully carried out recently using a reduced gas phase kinetics mechanism which substantially decreased the computational cost. A detailed mechanism including gas phase HOx, NOx, and SOx chemistry between the aircraft exhaust and the ambient air in near-field aircraft plumes is compiled. A reduced mechanism capturing the major chemical pathways is developed. Predictions by the reduced mechanism are found to be in good agreement with those by the detailed mechanism. With the reduced chemistry, the computer CPU time is saved by a factor of more than 3.5 for the near-field plume modeling. Distributions of major chemical species are obtained and analyzed. The computed sensitivities of major species with respect to reaction step are deduced for identification of the dominant gas phase kinetic reaction pathways in the jet plume. Both the near field plume and the plume-vortex regimes were investigated using advanced mixing models. In the near field, a stand-alone mixing model was used to investigate the impact of turbulent mixing on the micro- and macro-scale mixing processes using a reduced reaction kinetics model. The plume-vortex regime was simulated using a large-eddy simulation model. Vortex plume behind Boeing 737 and 747 aircraft was simulated along with relevant kinetics. Many features of the computed flow field show reasonable agreement with data. The entrainment of the engine plumes into the wing tip vortices and also the partial detrainment of the plume were numerically captured. The impact of fluid mechanics on the chemical processes was also studied. Results show that there are significant differences between spatial and temporal simulations especially in the predicted SO3 concentrations. This has important implications for the prediction of sulfuric acid aerosols in the wake and may partly explain the discrepancy between past numerical studies (that employed parabolic or temporal approximations) and the measured data. Finally to address the major uncertainty in the near-field plume modeling related to the plume processing of sulfur compounds and advanced model was developed to evaluate its impact on the chemical processes in the near wake. A comprehensive aerosol model is developed and it is coupled with chemical kinetics and the axisymmetric turbulent jet flow models. The integrated model is used to simulate microphysical processes in the near-field jet plume, including sulfuric acid and water binary homogeneous nucleation, coagulation, non-equilibrium heteromolecular condensation, and sulfur-induced soot activation. The formation and evolution of aerosols are computed and analyzed. The computed results show that a large number of ultra-fine (0.3--0.6 nm in radius) volatile HSO4 - HO embryos are generated in the near-field plume. These embryos further grow in size by self coagulation and condensation. Soot particles can be activated by both heterogeneous nucleation and scavenging of H2SO4-H2O aerosols. These activated soot particles can serve as water condensation nuclei for contrail formation. Conditions under which ice contrails can form behind aircrafts are studied. The sensitivities of the threshold temperature for contrail formation with respect to aircraft propulsion efficiency, relative humidity, and ambient pressure are evaluated. The computed aerosol properties for different extent of fuel sulfur conversion to S(VI) (SO3 and H2SO4) in engine are examined and the results are found to be sensitive to this conversion fraction.

Menon, Suresh↗

Ground-based Validation of the EOS Multi-angle Imaging SpectroRadiometer (MISR) Aerosol Retrieval Algorithms and Science Data Products

A plan for the ground-based validation of MISR aerosol retrieval is outlined. Activities occur in two phases: (1) pre-launch, work is focused on technique development and MISR algorithm validation using conventional ground-base methods and a MISR simulator (AirMISR) operating from the ER-2 aircraft to simulate MISR on-orbit observations. (2) Post-launch, the validation program relies on ground campaigns, underflights wit the MISR simulator and the use of local measurements fo aerosol loading and properties and irradiance measurements derived from the AERONET and ISIS networks.

algorithm↗

Physical chemistry of the H2SO4/HNO3/H2O system - Implications for polar stratospheric clouds

Polar stratospheric clouds (PSCs) play a key role in stratospheric ozone depletion. Surface-catalyzed reactions on PSC particles generate chlorine compounds that photolyze readily to yield chlorine radicals, which in turn destroy ozone very efficiently. The most prevalent PSCs form at temperatures several degrees above the ice frost point and are believed to consist of HNO3 hydrates; however, their formation mechanism is unclear. Results of laboratory experiments are presented which indicate that the background stratospheric H2SO4/H2O aerosols provide an essential link in this mechanism: These liquid aerosols absorb significant amounts of HNO3 vapor, leading most likely to the crystallization of nitric acid trihydrate (NAT). The frozen particles then grow to form PSCs by condensation of additional amounts of HNO3 and H2O vapor. Furthermore, reaction probability measurements reveal that the chlorine radical precursors are formed readily at polar stratospheric temperatures not just on NAT and ice crystals, but also on liquid H2SO4 solutions and on solid H2SO4 hydrates. These results imply that the chlorine activation efficiency of the aerosol particles increases rapidly as the temperature approaches the ice frost point regardless of the phase or composition of the particles.

Molina, M. J.↗

Prognostic simulations of mixed-phase clouds with model AC-1D v1.0: the impact of aerosol types and freezing parameterizations on ice crystal budgets

Mixed-phase clouds at high latitudes contribute to the uncertainty in predicting cloud feedbacks and climate sensitivity, mainly due to the complexity of microphysical processes that influence the partitioning between the supercooled liquid and ice phases, and hence, cloud radiative effects on regional scales. Particularly in Arctic mixed-phase clouds, the activation of ice-nucleating particles (INPs) from various aerosol populations remains a leading source of uncertainty. We developed an aerosol-cloud one-dimensional (AC-1D) model, which provides a novel framework to prognostically treat INP and ice crystal budgets while explicitly accounting for polydisperse and multicomponent aerosol that activate INPs following different freezing parameterizations. The AC-1D model is informed by large-eddy simulations to probe the impact of INP representation on predicted ice crystal number concentrations (N i ) and ice crystal budgets in mixed-phase Arctic stratus. We apply three immersion freezing (IMF) parameterizations, two time-independent (singular) and one time-dependent (classical nucleation theory), to predict the evolution of the INP reservoir and resulting ice crystal budget from polydisperse mineral dust, organic (humic-like substances), and sea spray aerosol particle size distributions. Our analysis focuses on how variations in aerosol number concentration and cloud system parameters such as cloud cooling rate, cloud-top entrainment rate, and ice crystal fall speed influence the INP reservoir and ice crystal budgets. Furthermore, this study investigates the competitive ice nucleation dynamics in mixed aerosol environments and provides a process-level quantification of the INP budget terms, which directly controls ice crystal budgets. For all studied case scenarios, the aerosol types and associated particle size distributions significantly impact INP and N i , and the choice between a time-dependent and a singular freezing description yields orders-of-magnitude differences in the predicted INP and N i over the 10 h simulation time, reflecting typical cloud lifetimes. Our results show that the influence of cloud cooling, INP entrainment, and sedimentation varies significantly depending on the chosen freezing parameterization. These findings underscore the critical need for robust IMF parameterizations and precise cloud system observations to enhance the accuracy of models in predicting mixed-phase cloud structure and evolution.

Arctic clouds↗

A new method for operating a continuous flow diffusion chamber to investigate immersion freezing: assessment and performance study

Glaciation in mixed-phase clouds predominately occurs through the immersion freezing mode where ice nucleating particles (INPs) immersed within supercooled droplets induce nucleation of ice. Currently, model representations of this process are a large source of uncertainty in simulating cloud radiative properties, and to constrain these estimates, continuous flow diffusion chamber (CFDC)-style INP devices are commonly used to assess the immersion freezing efficiencies of INPs. In this study, a new approach was explored to operating such an ice chamber that provides maximum activation of particles without droplet breakthrough and correction factor ambiguity to obtain high-quality INP measurements in a manner that has not been demonstrated as possible previously. The conditioning section of the chamber was maintained at ~ –20 °C and water relative humidity (RH w ) ~ 113 % conditions to maximize the droplet activation, and the droplets were supercooled with an independently temperature-controlled nucleation section at a steady cooling rate (0.5 °C min –1 ) to induce the freezing of droplets and evaporation of unfrozen droplets. The performance of the modified ice chamber was evaluated using four INP species: K-feldspar, illite-NX, Argentinian soil dust, and airborne arable dust that had shown ice nucleation over a wide span of supercooled temperatures. Dry dispersed and size-selected K-feldspar particles were generated in the laboratory. Illite-NX and soil dust particles were sampled during the second phase of the Fifth International Ice Nucleation Workshop (FIN-02) campaign, and airborne arable dust particles were sampled from the aerosol inlet located on the rooftop of the laboratory. The measured ice nucleation efficiencies of model aerosols with a surface active site density (n s ) metric were higher, but mostly agreed within one order of magnitude compared to literature results.

54 ENVIRONMENTAL SCIENCES↗

Prescribing the aerosol effective radiative forcing in the Simple Cloud-Resolving E3SM Atmosphere Model v1

Aerosol effective radiative forcing critically influences climate projections but remains poorly constrained. Using the Simple Cloud-Resolving E3SM Atmosphere Model (SCREAM) v1 configuration, we assess the sensitivity of the radiative forcing due to anthropogenic aerosol changes using a simplified prescribed aerosol scheme (SPA) derived from E3SM v3. Nudged simulations at 3 and 12 km horizontal grid spacings reveal a more negative aerosol forcing than the reference 100 km E3SM v3 whence the SPA properties are derived. The resulting globally averaged aerosol forcing signal is largely due to aerosol–cloud interactions and exhibits little overall resolution sensitivity, while hints of resolution sensitivity appear regionally between the 3 and 12 km runs. While the default SPA scheme overestimates cloud droplet dependence on aerosols, parameterization adjustments in the activation process reconcile forcing estimates with the reference model. Our results demonstrate the ability to use a prescribed aerosol scheme to hold aerosol forcing to a desired strength across resolutions.

54 ENVIRONMENTAL SCIENCES↗