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TRACER-MAP Field Campaign Report

During July-August 2022, the U.S. Department of Energy (DOE) Atmospheric System Research (ASR)-funded Tracking Aerosol Convection Interactions Experiment (TRACER)-MAP campaign completed an Atmospheric Radiation Measurement (ARM) user facility field study to measure and map aerosol, volatile organic compounds (VOC), trace gas, and select meteorological observations across Houston, Texas. That ASR project and ARM field campaign, TRACER-MAP, was designed to complement measurements made at the first ARM Mobile Facility (AMF1) by the Aerosol Observing System (AOS) during the TRACER campaign. In this manner, TRACER-MAP effectively extended aerosol measurements from the TRACER AMF deployment, increasing the spatial coverage across the Houston metropolitan area, characterizing a greater diversity of source mixtures (e.g., industrial, traffic, residential, and biogenic) and capturing air masses with differential aging of urban source emissions (e.g., downtown versus downwind). That rich data set now offers many possibilities for in-depth analysis that align with the ASR mission to “research aerosol processes that affect Earth’s radiative balance and hydrological cycle.”

54 ENVIRONMENTAL SCIENCES↗

Optimizing radar scan strategies for tracking isolated deep convection using observing system simulation experiments

Abstract. Optimizing radar observation strategies is one of the most important considerations in pre-field campaign periods. This is especially true for isolated convective clouds that typically evolve faster than the observations captured by operational radar networks. This study investigates uncertainties in radar observations of the evolution of the microphysical and dynamical properties of isolated deep convective clouds developing in clean and polluted environments. It aims to optimize the radar observation strategy for deep convection through the use of high-spatiotemporal cloud-resolving model simulations, which resolve the evolution of individual convective cells every 1 min, coupled with a radar simulator and a cell tracking algorithm. The radar simulation settings are based on the Tracking Aerosol Convection Interactions ExpeRiment (TRACER) and Experiment of Sea Breeze Convection, Aerosols, Precipitation and Environment (ESCAPE) field campaigns held in the Houston, TX, area but are generalizable to other field campaigns focusing on isolated deep convection. Our analysis produces the following four outcomes. First, a 5–7 m s−1 median difference in maximum updrafts of tracked cells is shown between the clean and polluted simulations in the early stages of the cloud lifetimes. This demonstrates the importance of obtaining accurate estimates of vertical velocity from observations if aerosol impacts are to be properly resolved. Second, tracking of individual cells and using vertical cross section scanning every minute capture the evolution of precipitation particle number concentration and size represented by polarimetric observables better than the operational radar observations that update the volume scan every 5 min. This approach also improves multi-Doppler radar updraft retrievals above 5 km above ground level for regions with updraft velocities greater than 10 m s−1. Third, we propose an optimized strategy composed of cell tracking by quick (1–2 min) vertical cross section scans from more than one radar in addition to the operational volume scans. We also propose the use of a single-RHI (range height indicator) updraft retrieval technique for cells close to the radars, for which multi-Doppler radar retrievals are still challenging. Finally, increasing the number of deep convective cells sampled by such observations better represents the median maximum updraft evolution with sample sizes of more than 10 deep cells, which decreases the error associated with sampling the true population to less than 3 m s−1.

54 ENVIRONMENTAL SCIENCES↗

Effect of Spectrally Varying Albedo of Vegetation Surfaces on Shortwave Radiation Fluxes and Aerosol Direct Radiative Forcing

This study develops an algorithm for representing detailed spectral features of vegetation albedo based on Moderate Resolution Imaging Spectrometer (MODIS) observations at 7 discrete channels, referred to as the MODIS Enhanced Vegetation Albedo (MEVA) algorithm. The MEVA algorithm empirically fills spectral gaps around the vegetation red edge near 0.7 micrometers and vegetation water absorption features at 1.48 and 1.92 micrometers which cannot be adequately captured by the MODIS 7 channels. We then assess the effects of applying MEVA in comparison to four other traditional approaches to calculate solar fluxes and aerosol direct radiative forcing (DRF) at the top of atmosphere (TOA) based on the MODIS discrete reflectance bands. By comparing the DRF results obtained through the MEVA method with the results obtained through the other four traditional approaches, we show that filling the spectral gap of the MODIS measurements around 0.7 micrometers based on the general spectral behavior of healthy green vegetation leads to significant improvement in the instantaneous aerosol DRF at TOA (up to 3.02Wm(exp -2) difference or 48% fraction of the aerosol DRF, .6.28Wm(exp -2), calculated for high spectral resolution surface reflectance from 0.3 to 2.5 micrometers for deciduous vegetation surface). The corrections of the spectral gaps in the vegetation spectrum in the near infrared, again missed by the MODIS reflectances, also contributes to improving TOA DRF calculations but to a much lower extent (less than 0.27Wm(exp -2), or about 4% of the instantaneous DRF). Compared to traditional approaches, MEVA also improves the accuracy of the outgoing solar flux between 0.3 to 2.5 micrometers at TOA by over 60Wm(exp -2) (for aspen 3 surface) and aerosol DRF by over 10Wm(exp -2) (for dry grass). Specifically, for Amazon vegetation types, MEVA can improve the accuracy of daily averaged aerosol radiative forcing in the spectral range of 0.3 to 2.5 micrometers at equator at the equinox by 3.7Wm(exp -2). These improvements indicate that MEVA can contribute to regional climate studies over vegetated areas and can help to improve remote sensing-based studies of climate processes and climate change.

Zhu, L.↗

Accurate Airborne Particle Sampler

Air inducted isokinetically into centrifugal collector. Cloud drop collector accurately and efficiently samples droplets and rejects aerosol particles. Number of these collectors connected in series, each designed that largest size fraction of droplets captured in first one and successively smaller size fractions captured in others. By analyzing each size fraction, chemical composition of cloud droplets related to drop size.

Miller, I. M.↗

Reducing Aerosol Forcing Uncertainty by Combining Models With Satellite and Within-The-Atmosphere Observations: A Three-Way Street

Aerosol forcing uncertainty represents the largest climate forcing uncertainty overall. Its magnitude has remained virtually undiminished over the past 20 years despite considerable advances in understanding most of the key contributing elements. Recent work has produced modest increases only in the confidence of the uncertainty estimate itself. This review summarizes the contributions toward reducing the uncertainty in the aerosol forcing of climate made by satellite observations, measurements taken within the atmosphere, as well as modeling and data assimilation. We adopt a more measurement-oriented perspective than most reviews of the subject in assessing the strengths and limitations of each; gaps and possible ways to fill them are considered. Currently planned programs supporting advanced, global-scale satellite and surface-based aerosol, cloud, and precursor gas observations, climate modeling, and intensive field campaigns aimed at characterizing the underlying physical and chemical processes involved, are all essential. But in addition, new efforts are needed: (a) to obtain systematic aircraft in situ measurements capturing the multi-variate probability distribution functions of particle optical, microphysical, and chemical properties (and associated uncertainty estimates), as well as co-variability with meteorology, for the major aerosol airmass types; (b) to conceive, develop, and implement a suborbital (aircraft plus surface-based) program aimed at systematically quantifying the cloud-scale microphysics, cloud optical properties, and cloud-related vertical velocities associated with aerosol-cloud interactions; and (c) to focus much more research on integrating the unique contributions of satellite observations, suborbital measurements, and modeling, to reduce the persistent uncertainty in aerosol climate forcing.

aerosol climate forcing↗

Testing the Two-Layer Model for Correcting Clear Sky Reflectance near Clouds

A two-layer model (2LM) was developed in our earlier studies to estimate the clear sky reflectance enhancement due to cloud-molecular radiative interaction at MODIS at 0.47 micrometers. Recently, we extended the model to include cloud-surface and cloud-aerosol radiative interactions. We use the LES/SHDOM simulated 3D true radiation fields to test the 2LM for reflectance enhancement at 0.47 micrometers. We find: The simple model captures the viewing angle dependence of the reflectance enhancement near cloud, suggesting the physics of this model is correct; the cloud-molecular interaction alone accounts for 70 percent of the enhancement; the cloud-surface interaction accounts for 16 percent of the enhancement; the cloud-aerosol interaction accounts for an additional 13 percent of the enhancement. We conclude that the 2LM is simple to apply and unbiased.

MODIS↗

Bubble Mass Transport Measurement in the Large-Scale Test Loops at Oak Ridge National Laboratory

Molten salts are complex fluids that incorporate multi-phase behavior depending on the chemistry and the physical properties of the entrained components. These components include the carrier salt, the actinide fuel, and fission, activation, and corrosion products, the concentrations of which depends on the burnup history of the salt. Radionuclide transport from the salt into the cover gas / off-gas system depends on volatility as predicted by thermochemistry, but data from the Molten Salt Reactor Experiment (MSRE) conducted in the late 1960s suggest that bubble formation and transport are also important. Anomalously high fractions of noble metals were found in the off-gas system and were attributed to transportation with parent salt aerosols and their association with rising noble gas bubbles. The prediction of such phenomena requires coupled neutronic, thermal hydraulic, and chemical equilibrium calculations, the framework of which is being developed within the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program supported by the US Department of Energy (DOE) Office of Nuclear Energy (NE). However, separate effects tests and models of experiments using tools such as SAM and Thermochimica can guide model developers through important processes. Conversely, model development guides the choice of experiments and systems to provide data that are relevant for validation. This report describes several experiments that tracked gas transport in molten salts, ranging from small-scale systems to large-scale loops. Gas transportation in a molten salt, LiCl-KCl, has been studied using the shadowgraph technique. Sensors such as residual gas analysis, Raman spectroscopy, and laser-induced breakdown spectroscopy have been tested for off-gas measurements. These data were used to interpret how the gases move through the upstream salt / cover gas and the interface between them. Differential pressure measurements were able to detect individual gas bubbles as they popped at the liquid–gas interface. Salt aerosols were collected on a cascade impactor. Their formation was also observed directly via the shadowgraph method, and most of these aerosols were launched ballistically into the cover gas. Fine mists could also be observed. Convection currents through the salt were visualized and can be used to calculate the thermophysical properties of the salt itself. The apparatuses described in this report and in a previous work (McFarlane et al. 2023) have been commissioned and are available for use in making further measurements of salt/surrogate fission product behavior. Novel approaches using neutron imaging are planned for the study of fluoride salts, which cannot be contained in quartz, so shadowgraph visualization is not available. Bubble transport in convective flow and in a slow-moving salt column are planned. The mobile laser-induced breakdown spectroscopy (LIBS) system is available for several applications, including iodine capture in a molten hydroxide scrubber, H2 transport though molten salts to complement Raman analysis, and online tracking of salt aerosol generation, transport, and deposition. This report summarizes the findings from FY24 and the plans for FY25. The work completes milestone M2AT-24OR0702013 of the DOE-NE Advanced Reactor Technology, Molten Salt Reactor Campaign, DOE-NE-5.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Modeling aerosol bolus inhalations in the human lung with the multiple path particle deposition model: Comparison with experimental data

Existing one-dimensional (1D) models of aerosol dosimetry often ignore mixing mechanisms of inhaled aerosols during their transport in the lung. This mixing or aerosol dispersion results from different physical mechanisms in different regions of the lung. It is a higher order effect, which cannot be directly captured in 1D modeling approaches, and thus is sometimes modeled as a diffusive process. Here, in this study, we improved our recently developed alveolar mixing module incorporated in the multiple path particle dosimetry model (MPPD) to account for flow irreversibility and particle trapping in the alveolar spaces, as well as mixing occurring in the tracheobronchial region. This new version of MPPD was coupled with CFPD-based predictions of aerosol bolus dispersion in the oral airway. The model was used to predict the deposition, dispersion, and mode shift of aerosol bolus inhaled at different penetration depths within the lung for breathing patterns and particle size matching those used in a previous experimental study (Darquenne et al., 2016). Even though a quite simplified approach was used, the computations appear to describe subject-specific and test-specific experimental data reasonably well. The proposed combined dispersion-deposition model can be a useful tool for targeted drug delivery and also for exposure health risk assessment.

MPPD↗

Slipstream Testing of Amine-Based Solvents at a Low-Rank Coal-Fired Power Plant

Conference presentation for 38th Annual International Pittsburgh Coal Conference, Virtual, September 20–23, 2021. To better assess mitigation strategies for aerosol reduction to extend solvent life, the University of North Dakota Energy & Environmental Research Center (EERC) installed a pilot-scale CO 2 absorption system at a lignite-fired plant in central North Dakota. The pilot-scale system was operated using both commercial KS-1™ solvent and advanced KS-21™ solvent provided by Mitsubishi Heavy Industries (MHI). MHI’s proprietary amine emission reduction unit (AERU™) technology was installed downstream of the absorber columns to reduce solvent losses by recovering amines at the system outlet. Fine particulate loading was measured throughout the capture system with and without a WESP operating and using both solvents. Captured particulate was brought back to the EERC to be analyzed for chemical composition and to be examined by scanning electron microscopy for particulate structure. These variables were then correlated to performance of particulate control devices in reducing aerosol formation and solvent losses.

01 COAL, LIGNITE, AND PEAT↗

Modeled and observed properties related to the direct aerosol radiative effect of biomass burning aerosol over the southeastern Atlantic

Biomass burning smoke is advected over the southeastern Atlantic Ocean between July and October of each year. This smoke plume overlies and mixes into a region of persistent low marine clouds. Model calculations of climate forcing by this plume vary significantly in both magnitude and sign. NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) had deployments for field campaigns off the west coast of Africa in 3 consecutive years (September 2016, August 2017, and October 2018) with the goal of better characterizing this plume as a function of the monthly evolution by measuring the parameters necessary to calculate the direct aerosol radiative effect. Here, this dataset and satellite retrievals of cloud properties are used to test the representation of the smoke plume and the underlying cloud layer in two regional models (WRF-CAM5 and CNRM-ALADIN) and two global models (GEOS and UM-UKCA). The focus is on the comparisons of those aerosol and cloud properties that are the primary determinants of the direct aerosol radiative effect and on the vertical distribution of the plume and its properties. The representativeness of the observations to monthly averages are tested for each field campaign, with the sampled mean aerosol light extinction generally found to be within 20 % of the monthly mean at plume altitudes. When compared to the observations, in all models, the simulated plume is too vertically diffuse and has smaller vertical gradients, and in two of the models (GEOS and UM-UKCA), the plume core is displaced lower than in the observations. Plume carbon monoxide, black carbon, and organic aerosol masses indicate underestimates in modeled plume concentrations, leading, in general, to underestimates in mid-visible aerosol extinction and optical depth. Biases in mid-visible single scatter albedo are both positive and negative across the models. Observed vertical gradients in single scatter albedo are not captured by the models, but the models do capture the coarse temporal evolution, correctly simulating higher values in October (2018) than in August (2017) and September (2016). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (<4 %) uncertainty in integrated solar absorption by the aerosol and, therefore, in the aerosol direct radiative effect. Model biases in cloud fraction, and, therefore, the scene albedo below the plume, vary significantly across the four models. The optical thickness of clouds is, on average, well simulated in the WRF-CAM5 and ALADIN models in the stratocumulus region and is underestimated in the GEOS model; UM-UKCA simulates cloud optical thickness that is significantly too high. Overall, the study demonstrates the utility of repeated, semi-random sampling across multiple years that can give insights into model biases and how these biases affect modeled climate forcing. The combined impact of these aerosol and cloud biases on the direct aerosol radiative effect (DARE) is estimated using a first-order approximation for a subset of five comparison grid boxes. A significant finding is that the observed grid box average aerosol and cloud properties yield a positive (warming) aerosol direct radiative effect for all five grid boxes, whereas DARE using the grid-box-averaged modeled properties ranges from much larger positive values to small, negative values. It is shown quantitatively how model biases can offset each other, so that model improvements that reduce biases in only one property (e.g., single scatter albedo but not cloud fraction) would lead to even greater biases in DARE. Across the models, biases in aerosol extinction and in cloud fraction and optical depth contribute the largest biases in DARE, with aerosol single scatter albedo also making a significant contribution.

54 ENVIRONMENTAL SCIENCES↗

Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing

Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and pristine present-day (PD) atmospheres. Here we revisit the atmospheric oxidation chemistry of DMS, particularly under pristine conditions, and its impact on aerosol IRF. Based on previous laboratory studies, we expand the simplified DMS oxidation scheme used in the Community Atmospheric Model version 6 with chemistry (CAM6-chem) to capture the OH-addition pathway and the H-abstraction pathway and the associated isomerization branch. These additional oxidation channels of DMS produce several stable intermediate compounds, e.g., methanesulfonic acid (MSA) and hydroperoxymethyl thioformate (HPMTF), delay the formation of sulfate, and, hence, alter the spatial distribution of sulfate aerosol and radiative impacts. The expanded scheme improves the agreement between modeled and observed concentrations of DMS, MSA, HPMTF, and sulfate over most marine regions, based on the NASA Atmospheric Tomography (ATom), the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA), and the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) measurements. We find that the global HPMTF burden and the burden of sulfate produced from DMS oxidation are relatively insensitive to the assumed isomerization rate, but the burden of HPMTF is very sensitive to a potential additional cloud loss. We find that global sulfate burden under PI and PD emissions increase to 412 Gg S (+29 %) and 582 Gg S (+8.8 %), respectively, compared to the standard simplified DMS oxidation scheme. The resulting annual mean global PD direct radiative effect of DMS-derived sulfate alone is −0.11 W m−2. The enhanced PI sulfate produced via the gas-phase chemistry updates alone dampens the aerosol IRF as anticipated (−2.2 W m−2 in standard versus −1.7 W m−2, with updated gas-phase chemistry). However, high clouds in the tropics and low clouds in the Southern Ocean appear particularly sensitive to the additional aqueous-phase pathways, counteracting this change (−2.3 W m−2). This study confirms the sensitivity of aerosol IRF to the PI aerosol loading and the need to better understand the processes controlling aerosol formation in the PI atmosphere and the cloud response to these changes.

54 ENVIRONMENTAL SCIENCES↗

Evaluating Models' Response of Tropical Low Clouds to SST Forcings Using CALIPSO Observations

Recent studies have shown that, in response to a surface warming, the marine tropical low-cloud cover (LCC) as observed by passive-sensor satellites substantially decreases, therefore generating a smaller negative value of the top-of-the-atmosphere (TOA) cloud radiative effect (CRE). Here we study the LCC and CRE interannual changes in response to sea surface temperature (SST) forcings in the GISS model E2 climate model, a developmental version of the GISS model E3 climate model, and in 12 other climate models, as a function of their ability to represent the vertical structure of the cloud response to SST change against 10 years of CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) observations. The more realistic models (those that satisfy the observational constraint) capture the observed interannual LCC change quite well ([delta]LCC]/[delta]SST= -3.49±1.01%K [negative 1 superscript] vs. [delta]LCC/[delta]SST[subscript obs]= -3.59±0.28%K[negative 1 superscript]) while the others largely underestimate it ([delta]LCC/[delta]SST= -1.32±1.28%K[negative 1 superscript]). Consequently, the more realistic models simulate more positive shortwave (SW) feedback ([delta]CRE/[delta]SST=2.60±1.13Wm[negative 2 superscript] K[negative 1 superscript]) than the less realistic models (CRE/SST=0.87±2.63Wm2K1), in better agreement with the observations ([delta]CRE/[delta]SST[subscript obs]=3±0.26Wm[negative 2 superscript] K[negative 1 superscript] ), although slightly underestimated. The ability of the models to represent moist processes within the planetary boundary layer (PBL) and produce persistent stratocumulus (Sc) decks appears crucial to replicating the observed relationship between clouds, radiation and surface temperature. This relationship is different depending on the type of low clouds in the observations. Over stratocumulus regions, cloud-top height increases slightly with SST, accompanied by a large decrease in cloud fraction, whereas over trade cumulus (Cu) regions, cloud fraction decreases everywhere, to a smaller extent.

low clouds↗

Local to Global Air Quality Simulations using the NASA GEOS Composition Forecast Model, GEOS-CF

We give an overview of the NASA Global Earth Observing System Composition Forecast model (GEOS-CF), a high-resolution (roughly 25-km) global composition model developed by the NASA Global Modeling and Assimilation Office (GMAO). This system combines the GEOS weather and aerosol model with the GEOS-Chem chemistry module to provide a holistic view of atmospheric composition that captures a wide range of air pollutants such as ozone,nitrogen oxides, volatile organic compounds, and fine particulate matter.Given the global extent of the model, GEOS-CF captures large-scale processes such as long-range transport of air pollutants, across ocean basins and continents.

Knowland, Emma K.↗

The Thermal Structure and Composition of Jupiter's Great Red Spot From JWST/MIRI

Jupiter's Great Red Spot (GRS) was mapped by the James Webb Space Telescope (JWST)/Mid-Infrared Instrument (4.9–27.9 μm) in July and August 2022. These observations took place alongside a suite of visual and infrared observations from; Hubble, JWST/NIRCam, Very Large Telescope/VISIR and amateur observers which provided both spatial and temporal context across the jovian disc. The stratospheric temperature structure retrieved using the NEMESIS software revealed a series of hot-spots above the GRS. These could be the consequence of GRS-induced wave activity. In the troposphere, the temperature structure was used to derive the thermal wind structure of the GRS vortex. These winds were only consistent with the independently determined wind field by JWST/NIRCam at 240 mbar if the altitude of the Hubble-derived winds were located around 1,200 mbar, considerably deeper than previously assumed. No enhancement in ammonia was found within the GRS but a link between elevated aerosol and phosphine abundances was observed within this region. North-south asymmetries were observed in the retrieved temperature, ammonia, phosphine and aerosol structure, consistent with the GRS tilting in the north-south direction. Finally, a small storm was captured north-west of the GRS that displayed a considerable excess in retrieved phosphine abundance, suggestive of vigorous convection. Despite this, no ammonia ice was detected in this region. The novelty of JWST required us to develop custom-made software to resolve challenges in calibration of the data. This involved the derivation of the “FLT-5” wavelength calibration solution that has subsequently been integrated into the standard calibration pipeline.

Jake Harkett↗

Spaceborne Lidar Retrievals of PM2.5 for Air Quality Studies and Applications

Fine particulate matter (PM2.5) substantially contributes to air pollution and negatively affects human health. While many studies have investigated the use of passive column-integrated aerosol optical depth to infer surface PM2.5, the use of lidar observations for air quality characterization is not nearly as extensive. Lidar measurements are critical, however, due to the vertical aerosol information they provide, including near the surface. In this presentation, we first provide an overview of various lidar-based approaches for estimating PM2.5 concentrations and then discuss how lidar measurements can assist other air quality applications. For example, estimates of PM2.5 have been obtained in a physics-based approach through CALIOP near-surface aerosol extinction retrievals, assumptions on the mass extinction efficiency, and incorporating other parameters (an aerosol hygroscopic growth factor and PM2.5/PM10 ratio). Application of this algorithm over the contiguous United States (CONUS) from 2006 to 2018 yielded larger PM2.5 values over the eastern and western CONUS (~10-15 μg/m³) and lower PM2.5 levels in the central CONUS (~5 μg/m³). These spatial patterns were similar to those from gridded PM2.5 concentrations obtained through in situ measurements at ground stations operated by the US Environmental Protection Agency. In another approach, the Cloud Aerosol Transport System (CATS) lidar was used with the Goddard Earth Observing System (GEOS) model in a 1D ensemble-based variational technique to obtain PM2.5 over the US and Europe, and the spatial patterns of the CATS/GEOS based PM2.5 concentrations generally captured those from surface stations (with corresponding hourly EPA PM2.5 vs CATS PM2.5 statistics of R=0.4 and bias=1.5 μg/m³). In our recent work, as part of the Models, In situ, and Remote sensing of Aerosols (MIRA) Working Group, we have applied both the CALIOP and CATS/GEOS based approaches over the highly polluted country of India during the post-monsoon season (September-October 2016). We derived elevated levels of two-month mean PM2.5 (~100 μg/m³) in northern India, especially near New Delhi. These high PM2.5 concentrations in the Indo-Gangetic plain are driven in large part from the seasonal burning of crop residue and meteorological conditions typical at this time of the year, such as low wind speeds and a shallow boundary layer. While the satellite-derived PM2.5 moderately replicates (R = ~0.7-0.9) the spatial variability in the two-month mean of surface in situ PM2.5 from monitoring sites operated by the Central and State Pollution Control Boards, we show results from specific scenes for which there are large deviations between the satellite-derived PM2.5 and in situ measurements. Other current work on this topic focuses on developing PM2.5 estimates using airborne high spectral resolution lidar measurements through machine learning regression algorithms and involves several parameters (e.g., aerosol extinction, color ratio, lidar ratio). Application of this method over major metropolitan areas in the US and Asia have resulted in high correlations (R = 0.93) with surface measurements. This airborne lidar approach can be adapted to spaceborne lidar measurements, and all three of these approaches can be applied to ESA’s EarthCARE Atmospheric Lidar instrument, setting the stage for the future Cloud Aerosol Lidar for Global Scale Observations of the Ocean-Land Atmosphere System (CALIGOLA) mission. Ultimately, beyond estimates of PM2.5, the aerosol vertical distribution from lidars can benefit studies involving passive sensor approaches for PM2.5 proxies (including from geostationary satellites), wildfire smoke plume injection heights, volcanic emissions (e.g., ash height retrievals), and aerosol/air quality model assimilation, evaluation, and forecasts.

Travis D Toth↗

Improving Our Fundamental Understanding of the Role of Aerosol Cloud Interactions in the Climate System

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol−cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol−cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol−cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

general circulation models↗

Analysis of the Planetary Boundary Layer Height During DISCOVER-AQ Baltimore–Washington, D.C., with Lidar and High-Resolution WRF Modeling

The daytime planetary boundary layer (PBL) was examined for the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) Baltimore (Maryland)–Washington, D.C., campaign of July 2011 using PBL height (PBLH) retrievals from aerosol backscatter measurements from ground-based micropulse lidar (MPL), the NASA Langley Research Center airborne High Spectral Resolution Lidar-1 (HSRL-1), and the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) on the Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite. High-resolution Weather Research and Forecasting (WRF) Model simulations with horizontal grid spacing of 1 km and different combinations of PBL schemes, urban parameterization, and sea surface temperature inputs were evaluated against PBLHs derived from lidars, ozonesondes, and radiosondes. MPL and WRF PBLHs depicted a growing PBL in the morning that reached a peak height by midafternoon. WRF PBLHs calculated from gridded output profiles generally showed more rapid growth and higher peak heights than did the MPLs, and all WRF–lidar differences were dependent on model configuration, PBLH calculation method, and synoptic conditions. At inland locations, WRF simulated an earlier descent of the PBL top in the afternoon relative to the MPL retrievals and radiosonde PBLHs. At Edgewood, Maryland, the influence of the Chesapeake Bay breeze on the PBLH was captured by both the ozonesonde and WRF data but generally not by the MPL PBLH retrievals because of generally weaker gradients in the aerosol backscatter profile and limited normalized relative backscatter data near the top height of the marine layer.

Hegarty, Jennifer D.↗

Dynamics and composition of particles from an aeolian input event to the Sargasso Sea

The present paper is concerned with studies related to the capture of aeolian mineral particles in the Sargasso Sea region in late June 1980. Attention is given to measurement techniques, aerosol sampling, particle trap sampling, investigations utilizing scanning electron microscopy, and the obtained results. Conceivable sources for nonbiogenic particles measured in the water column are related to fallout from the Mount St. Helens eruption and soil materials transported by winds from the North American or African continents. It is found that present aerosol transport models are not adequaely addressing the transport of giant particles from the Sahara to the Sargasso Sea. Data regarding the variation of Sargasso Sea aerosol mass concentrations with time are presented in a table.

Carder, K. L.↗