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At least 433 records · Page 24

Topical Issue on Optical Particle Characterization and Remote Sensing of the Atmosphere: Part I

Increasing our understanding of the Earth-atmosphere system has been a scientific and political priority for the last few decades. This system not only touches on environmental science, but it has applicability to our broader understanding of planetary atmospheres in general. While this issue focuses primarily on electromagnetics, other fundamental fields of science, including fluid and thermodynamics play major roles. In recent years, significant research efforts have led to advances in the fields of radiative transfer and electromagnetic scattering from irregularly shaped particles. Recently, several workshops and small conferences have taken place to promote the fusion of these efforts. Late in 2013, for instance, two such meetings took place. The Optical Characterization of Atmospheric Aerosols (OCAA) meeting took place in Smolenice, Slovakia to promote a better understanding of microphysical properties of aerosol particles, and the characterization of such atmospheric particles using optical techniques. A complementary conference was organized in Nagoya, Japan, the 3rd International Symposium on Atmospheric Light Scattering and Remote Sensing (ISALSaRS), whose goal is to fuse the advances achieved in particle characterization with remote-sensing techniques. While the focus of these meetings is slightly different, they represent the same aspects of this rapidly growing field. This Topical Issue is the first of two parts. Within this issue we analyze different aspects of the problem of atmospheric characterization and present a broad overview of the topical area. Research includes theory and experiment, ranging from fundamental microphysical properties of individual aerosol particles to broad characterizations of atmospheric properties. Since this is an active field, we also have encouraged the submission of ideas for new methodologies that may represent the future of the field.

aerosols↗

The Goddard Chemistry Aerosol Radiation and Transport Model

The Goddard Chemistry Aerosol Radiation and Transport (GOCART) model is one of the fourteen global models participating in the International AEROCOM activity. The Oslo workshop is the 4th AEROCOM workshop. In this workshop, we are going to show updated model results of global aerosol extinction and absorption, vertical profiles, and direct and indirect effects. We will also discuss with other participants on model similarities and discrepancies, issues related to comparisons with in-situ and remote sensing data, and future directions.

Chin, Mian↗

Elemental composition of aerosols in fourteen experiments of the Cloud Condensation Nuclei Workshop

Aeosols were collected with two Ci impactors and analyzed with proton induced X-ray emission (PIXE) for chemical composition and to detect if contamination was present. One of the impactors sampled the generated aerosols; the other impactor sampled droplets from a diffusion cloud chamber. The purpose of the experiments was to test the feasibility of a study of the transfer of chemical elements from the fine particle sizes to the coarse particle sizes, after CCN are activated and cloud droplets are formed. The data indicated that sulfur-containing aerosols did exhibit the expected transfer.

Mach, W. H.↗

Abrupt emissions reductions during COVID-19 contributed to record summer rainfall in China

Record rainfall and severe flooding struck eastern China in the summer of 2020. The extreme summer rainfall occurred during the COVID-19 pandemic, which started in China in early 2020 and spread rapidly across the globe. By disrupting human activities, substantial reductions in anthropogenic emissions of greenhouse gases and aerosols might have affected regional precipitation in many ways. Here, we investigate such connections and show that the abrupt emissions reductions during the pandemic strengthened the summer atmospheric convection over eastern China, resulting in a positive sea level pressure anomaly over northwestern Pacific Ocean. The latter enhanced moisture convergence to eastern China and further intensified rainfall in that region. Modeling experiments show that the reduction in aerosols had a stronger impact on precipitation than the decrease of greenhouse gases did. We conclude that through abrupt emissions reductions, the COVID-19 pandemic contributed importantly to the 2020 extreme summer rainfall in eastern China.

54 ENVIRONMENTAL SCIENCES↗

Improving GCM Predictability of Mixed-Phase Clouds and Aerosol Interactions at High Latitudes with ARM Observations

The overachieving goal of this project is to improve the predictability of mixed-phase clouds and aerosol interactions in the Community Atmosphere Model version 6 (CAM6) through comparison with the ARM observations. There are three main objectives of the proposed study: (1) Improve the representation of ice microphysical processes in mixed-phase clouds; (2) Test the performance of ice microphysics in CESM-CAM6 with the ARM observations in northern and southern high latitudes; and (3) Examine mixed-phase cloud microphysics-aerosol-turbulence-radiation interactions in CESM-CAM6. In this project, we have (1) Improved the representation of ice microphysical processes in mixed-phase clouds in CESM-CAM6 by implementing the marine organic aerosol (MOA) and treating the ice nucleating particles (INPs) from MOA and its impacts on mixed-phase clouds. We improved the treatment of ice depositional growth through the Wegener–Bergeron–Findeisen (WBF) process by considering the subgrid heterogeneous distributions between liquid droplets and ice crystals in mixed-phase clouds; (2) Tested the performance of ice microphysics in CESM-CAM6 with the ARM observations at high latitudes. We compared the simulated INP concentrations with the ARM observations, e.g., from M-PACE, ISDAC, INPOP, and other data (Mace Head, Zeppelin, CAPRICORN). We examined the impact of improved WBF treatment on model simulated Arctic mixed-phase clouds observed in the M-PACE field campaign. Seasonal variations of modeled mixed-phase cloud properties (LWO, IWP) are compared with the ground-based remote sensing retrievals at the ARM’s NSA $Utqia\dot{g}vik$ site; and (3) Examined mixed-phase cloud microphysics-aerosol-dynamics-radiation interactions in CESM-CAM6 that include the impacts of MOA INPs, and impacts of different model parameterizations (CLUBB versus UW turbulence & shallow convection schemes, MG2 versus MG1) on high-latitude mixed-phase cloud properties. Aerosol indirect effects of MOA through the liquid phase (droplet activation) and ice phase processes (e.g., the glaciation indirect effect) were investigated.

54 ENVIRONMENTAL SCIENCES↗

Enhanced Filter Material for Pathogen Removal

It was determined that spherical silver (Ag) nanoparticles either bound to 316 stainless-steel filter material or as unbound nanomaterials in deionized water had anti-microbial activity on Escherichia coli K-12 (E. coli) cultures when aerosolized or waterborne. This effect however was attenuated when in the presence of the high-salt growth media. Nanoparticles are known to agglomerate in high salt solutions and this may have limited their ability to cross the cell membrane of the microorganisms and cause fatal damage.

36 MATERIALS SCIENCE↗

Aerosol Manufacturing Technology to Produce Low-Cobalt Li-ion Battery Cathodes

Although considerable progress has been made with battery materials over the last 10 years, the cathode remains a major performance-limiting material in Li-ion battery (LIB) technology. New materials and battery chemistries will overcome some of the remaining challenges, but cathode materials must also be manufactured at a lower cost and with a smaller environmental footprint using new processes that can also enable improved control over stoichiometry, morphology, and compositional homogeneity. Cabot, Argonne National Laboratory and SAFT research teams are combining their extensive expertise in particle synthesis, battery materials and cell design to develop a low-cost, flexible aerosol manufacturing technology for production of high-performance cathode active materials (CAM). This project will develop low-Co CAMs via Reactive Spray Technology (RST) and Flame Spray Pyrolysis (FSP) to reach performance targets of < 50 mg Cobalt/Wh.

25 ENERGY STORAGE↗

Lidar stratospheric ozone measurements at the observatoire de Haute Provence (France)

Strastospheric ozone monitoring is of particular importance to confirm present day theories predicting a maximal ozone depletion, due to chlorofluorocarbon emission, in the 35 to 45 km altitude range. Measurements presently rely on both ground based and satellite-borne passive experiments. Such systems have been recently shown to have intrinsic limitations mainly due to atmospheric aerosol presence and calibration problems. During the last few years, active lidar profiling of the ozone vertical distribution by the Differential Absorption Laser technique (DIAL) in the UV wavelength range has been developed using two different laser sources: a Nd-YAG pumped dye laser which enables a large tuning range of the UV emitted wavelengths; and exciplex laser sources using xenon chloride as an active medium and emitting at 308 nm, the off wavelength being usually generated by Raman shifting techniques. Advantages and limitations of using both of these systems are briefly discussed.

Godin, S.↗

Measurements of cloud condensation nuclei spectra within maritime cumulus cloud droplets: Implications for mixing processes

In a cloud formed during adiabatic expansion, the droplet size distribution will be systematically related to the critical supersaturation of the cloud condensation nuclei (CNN), but this relationship can be complicated in entraining clouds. Useful information about cloud processes, such as mixing, can be obtained from direct measurements of the CNN involved in droplet nucleation. This was accomplished by interfacing two instruments for a series of flights in maritime cumulus clouds. One instrument, the counterflow virtual impactor, collected cloud droplets, and the nonvolatile residual nuclei of the droplets was then passed to a CCN spectrometer, which measured the critical supersaturation (S(sub c)) spectrum of the droplet nuclei. The measured S(sub c) spectra of the droplet nuclei were compared with the S(sub c) spectra of ambient aerosol particles in order to identify which CCN were actually incorporated into droplets and to determine when mixing processes were active at different cloud levels. The droplet nuclei nearly always exhibited lower median S(sub c)'s than the ambient aerosol, as expected since droplets nucleate perferentially on particles with lower critical supersaturations. Critical supersaturation spectra from nuclei of droplets near cloud base were similar to those predicted for cloud regions formed adiabatically, but spectra of droplet nuclei from middle cloud levels showed some evidence that mixing had occurred. Near cloud top, the greatest variation in the spectra of the droplet nuclei was observed, and nuclei with high S(sub c)'s were sometimes present even within relatively large droplets. This suggests that the extent of mixing increases with height in cumulus clouds and that inhomogeneous mixing may be important near cloud top. These promising initial results suggest improvements to the experimental technique that will permit more quantitative results in future experiments.

Twohy, Cynthia H.↗

Observed Spectral Invariant Behavior of Zenith Radiance in the Transition Zone Between Cloud-Free and Cloudy Regions

The Atmospheric Radiation Measurement Program's (ARM) new Shortwave Spectrometer (SWS) looks straight up and measures zenith radiance at 418 wavelengths between 350 and 2200 nm. Because of its 1-sec sampling resolution, the SWS provides a unique capability to study the transition zone between cloudy and clear sky areas. A surprising spectral invariant behavior is found between ratios of zenith radiance spectra during the transition from cloudy to cloud-free atmosphere. This behavior suggests that the spectral signature of the transition zone is a linear mixture between the two extremes (definitely cloudy and definitely clear). The weighting function of the linear mixture is found to be a wavelength-independent characteristic of the transition zone. It is shown that the transition zone spectrum is fully determined by this function and zenith radiance spectra of clear and cloudy regions. This new finding may help us to better understand and quantify such physical phenomena as humidification of aerosols in the relatively moist cloud environment and evaporation and activation of cloud droplets.

Marshak, A.↗

The role of local shipping emissions in aerosol-cloud interactions in the central Arctic

Arctic shipping is projected to increase as sea ice retreats, yet the impact of modern low-sulfur ship emissions on Arctic clouds and radiation remain poorly constrained. We use year-long in situ observations from the MOSAiC expedition to characterize ship-aerosol-cloud interactions for an icebreaker burning ultra-low sulfur fuel (0.1% mass per mass). Exhaust plumes were found to be strongly enriched in Aitken-mode particles, organic aerosol, and black carbon, but showed no detectable enhancement in particulate sulfate. Despite reduced hygroscopicity relative to ambient aerosols, ship emissions substantially increased local cloud condensation nuclei concentrations. A droplet activation parameterization was applied to quantify responses in cloud droplet number concentration ( N d ) to ship-induced perturbations in low-level Arctic clouds. In winter, abundant background accumulation-mode particles from Arctic haze supplied nearly all cloud droplets, while additional particles from ship emissions had little impact on N d . In contrast, during summer months, when unperturbed background aerosol concentrations are low, ship emissions nearly doubled N d compared to average background conditions and increased N d by a factor of five compared to very clean background conditions (25th percentile of background aerosol number concentrations). Longwave radiative transfer simulations for typical conditions of summer Arctic low-level clouds/fog suggest that these ship-induced increases in N d locally (i.e. <100 km downwind) lead to enhanced net surface longwave fluxes and consequent warming, primarily for optically thin clouds (liquid water path (LWP) ⩽ 30 g·m −2 ). For LWP = 10 g · m −2 , ship emissions lead to an increase of 1 W · m −2 in cloud longwave forcing at the surface compared to average unperturbed conditions (+7% relative increase), and up to 4 W · m −2 when compared to very clean background conditions (+22% relative increase). Even ultra-low sulfur fuel emissions can therefore locally and episodically modify Arctic cloud microphysics and radiative properties, especially during summer, implying that future increases in Arctic shipping could have non-negligible regional climate impacts.

Arctic↗

Desert Dust and Monsoon Rain

For centuries, inhabitants of the Indian subcontinent have know that heavy dust events brought on by strong winds occur frequently in the pre-monsoon season, before the onset of heavy rain. Yet scientists have never seriously considered the possibility that natural dust can affect monsoon rainfall. Up to now, most studies of the impacts of aerosols on Indian monsoon rainfall have focused on anthropogenic aerosols in the context of climate change. However, a few recent studies have show that aerosols from antropogenic and natural sources over the Indian subcontinent may affect the transition from break to active monsoon phases on short timescales of days to weeks. Writing in Nature Geoscience, Vinoj and colleagues describe how they have shown that desert dust aerosols over the Arabian Sea and West Asia can strenghten the summer monsoon over the Indial subcontinent in a matter of days.

monsoon↗

Why do Tornados and Hail Storms Rest on Weekends?

When anthropogenic aerosols over the eastern USA during summertime are at their weekly mid-week peak, tornado and hail storm activity there is also near its weekly maximum. The weekly cycle in storm activity is statistically significant and unlikely to be due to natural variability. The pattern of variability supports the hypothesis that air pollution aerosols invigorate deep convective clouds in a moist, unstable atmosphere, to the extent of inducing production of large hailstones and tornados. This is caused by the effect of aerosols on cloud-drop nucleation, making cloud drops smaller, delaying precipitation-forming processes and their evaporation, and hence affecting cloud dynamics.

Rosenfeld, Daniel↗

Sky-Scanning Sun-Tracking Airborne Radiometer (3STAR): Instrument Design, Flight Testing, and Tracking Performance

The Sky-Scanning, Sun-Tracking Airborne Radiometer (3STAR) adapts commercial radiometer technology developed for the ocean color research community to airborne measurement of spectrally resolved solar irradiance and sky radiance. These atmospheric observations are used to derive aerosol optical depth (AOD), supporting localized AOD inputs for atmospheric correction of satellite and airborne data over terrestrial and aquatic (including optically dark) targets. The ability to regionally “tune” atmospheric correction schemes with relevant spatial AOD supports constraining atmospheric correction of remote sensing reflectance. Very wide dynamic range has been achieved for multi-channel band-pass-filter-radiometers originally designed for deployment into the water column. By actively tracking and directly pointing to the Sun, the light attenuation by aerosol particles in the atmospheric column can be quantified. These measurements improve knowledge of atmospheric constituents and the atmospheric corrections required to improve remote sensing capabilities for interpreting reflectance measurements from the Earth surface. 3STAR incorporates a custom Sun-tracking/sky-scanning pointing head, a Sun-tracking camera, and a commercially available, cylindrical, 19-channel radiometer tube assembly. An accurate and responsive mount and tracking system has been developed and certified to NASA and Naval Air Systems Command (NAVAIR) airworthiness standards for deployment into the aircraft slipstream. Ground and flight testing indicate typical tracking errors of less than 0.1 degrees, well within the field of view of the radiometer as required to minimize measurement uncertainty from alignment error. Preliminary AOD measurements compare to within 0.013 with 15 measurements from an Aerosol Robotic Network (AERONET) Cimel instrument at 500 nm wavelength and low solar angle.

Atmosphere↗

Effective radiative forcing from emissions of reactive gases and aerosols - a multi-model comparison

This paper quantifies the pre-industrial (1850) to present-day (2014) effective radiative forcing (ERF) of anthropogenic emissions of NOX, volatile organic compounds (VOCs; including CO), SO2, NH3, black carbon, organic carbon, and concentrations of methane, N2O and ozone-depleting halocarbons, using CMIP6 models. Concentration and emission changes of reactive species can cause multiple changes in the composition of radiatively active species: tropospheric ozone, stratospheric ozone, stratospheric water vapour, secondary inorganic and organic aerosol, and methane. Where possible we break down the ERFs from each emitted species into the contributions from the composition changes. The ERFs are calculated for each of the models that participated in the AerChemMIP experiments as part of the CMIP6 project, where the relevant model output was available. The 1850 to 2014 multi-model mean ERFs (± standard deviations) are −1.03 ± 0.37 W/sq.m for SO2 emissions, −0.25 ± 0.09 W/sq.m for organic carbon (OC), 0.15 ± 0.17 W/sq.m for black carbon (BC) and −0.07 ± 0.01 W/sq.m for NH3. For the combined aerosols (in the piClim-aer experiment) it is −1.01 ± 0.25 W/sq.m. The multi-model means for the reactive well-mixed greenhouse gases (including any effects on ozone and aerosol chemistry) are 0.67 ± 0.17 W/sq.m for methane (CH4), 0.26 ± 0.07 W/sq.m for nitrous oxide (N2O) and 0.12 ± 0.2 W/sq.m for ozone-depleting halocarbons (HC). Emissions of the ozone precursors nitrogen oxides (NOx), volatile organic compounds and both together (O3) lead to ERFs of 0.14 ± 0.13, 0.09 ± 0.14 and 0.20 ± 0.07 W/sq.m respectively. The differences in ERFs calculated for the different models reflect differences in the complexity of their aerosol and chemistry schemes, especially in the case of methane where tropospheric chemistry captures increased forcing from ozone production.

radiative forcing↗

Aerosol in the Pacific troposphere

The use of near real-time optical techniques is emphasized for the measurement of mid-tropospheric aerosol over the Central Pacific. The primary focus is on measurement of the aerosol size distribution over the range of particle diameters from 0.15 to 5.0 microns that are essential for modeling CO2 backscatter values in support of the laser atmospheric wind sounder (LAWS) program. The measurement system employs a LAS-X (Laser Aerosol Spectrometer-PMS, Boulder, CO) with a custom 256 channel pulse height analyzer and software for detailed measurement and analysis of aerosol size distributions. A thermal preheater system (Thermo Optic Aerosol Descriminator (TOAD) conditions the aerosol in a manner that allows the discrimination of the size distribution of individual aerosol components such as sulfuric acid, sulfates and refractory species. This allows assessment of the relative contribution of each component to the BCO2 signal. This is necessary since the different components have different sources, exhibit independent variability and provide different BCO2 signals for a given mass and particle size. Field activities involve experiments designed to examine both temporal and spatial variability of these aerosol components from ground based and aircraft platforms.

Clarke, Antony D.↗

Aerosol responses to precipitation along North American air trajectories arriving at Bermuda

North American pollution outflow is ubiquitous over the western North Atlantic Ocean, especially in winter, making this location a suitable natural laboratory for investigating the impact of precipitation on aerosol particles along air mass trajectories. We take advantage of observational data collected at Bermuda to seasonally assess the sensitivity of aerosol mass concentrations and volume size distributions to accumulated precipitation along trajectories (APT). The mass concentration of particulate matter with aerodynamic diameter less than 2.5 µm normalized by the enhancement of carbon monoxide above background (PM 2.5 /ΔCO) at Bermuda was used to estimate the degree of aerosol loss during transport to Bermuda. Results for December–February (DJF) show that most trajectories come from North America and have the highest APTs, resulting in a significant reduction (by 53 %) in PM 2.5 /ΔCO under high-APT conditions (> 13.5 mm) relative to low-APT conditions (< 0.9 mm). Moreover, PM 2.5 /ΔCO was most sensitive to increases in APT up to 5 mm (–0.044 µg m –3 ppbv –1 mm –1 ) and less sensitive to increases in APT over 5 mm. While anthropogenic PM 2.5 constituents (e.g., black carbon, sulfate, organic carbon) decrease with high APT, sea salt, in contrast, was comparable between high- and low-APT conditions owing to enhanced local wind and sea salt emissions in high-APT conditions. The greater sensitivity of the fine-mode volume concentrations (versus coarse mode) to wet scavenging is evident from AErosol RObotic NETwork (AERONET) volume size distribution data. A combination of GEOS-Chem model simulations of the 210 Pb submicron aerosol tracer and its gaseous precursor 222 Rn reveals that (i) surface aerosol particles at Bermuda are most impacted by wet scavenging in winter and spring (due to large-scale precipitation) with a maximum in March, whereas convective scavenging plays a substantial role in summer; and (ii) North American 222 Rn tracer emissions contribute most to surface 210 Pb concentrations at Bermuda in winter (~75 %–80 %), indicating that air masses arriving at Bermuda experience large-scale precipitation scavenging while traveling from North America. A case study flight from the ACTIVATE field campaign on 22 February 2020 reveals a significant reduction in aerosol number and volume concentrations during air mass transport off the US East Coast associated with increased cloud fraction and precipitation. These results highlight the sensitivity of remote marine boundary layer aerosol characteristics to precipitation along trajectories, especially when the air mass source is continental outflow from polluted regions like the US East Coast.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Studying Aerosol, Clouds, and Air Quality in the Coastal Urban Environment of Southeastern Texas

A multi-agency succession of field campaigns was conducted in southeastern Texas during July 2021 through October 2022 to study the complex interactions of aerosols, clouds and air pollution in the coastal urban environment. As part of the Tracking Aerosol Convection interactions Experiment (TRACER), the TRACER- Air Quality (TAQ) campaign the Experiment of Sea Breeze Convection, Aerosols, Precipitation and Environment (ESCAPE) and the Convective Cloud Urban Boundary Layer Experiment (CUBE), a combination of ground-based supersites and mobile laboratories, shipborne measurements and aircraft-based instrumentation were deployed. These diverse platforms collected high-resolution data to characterize the aerosol microphysics and chemistry, cloud and precipitation micro- and macro-physical properties, environmental thermodynamics and air quality-relevant constituents that are being used in follow-on analysis and modeling activities. We present the overall deployment setups, a summary of the campaign conditions and a sampling of early research results related to: (a) aerosol precursors in the urban environment, (b) influences of local meteorology on air pollution, (c) detailed observations of the sea breeze circulation, (d) retrieved supersaturation in convective updrafts, (e) characterizing the convective updraft lifecycle, (f) variability in lightning characteristics of convective storms and (g) urban influences on surface energy fluxes. The work concludes with discussion of future research activities highlighted by the TRACER model-intercomparison project to explore the representation of aerosol-convective interactions in high-resolution simulations.

54 ENVIRONMENTAL SCIENCES↗