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Predicting the Mineral Composition of Dust Aerosols: Representing Key Processes - Part 1

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wetsieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to measurements from North Africa shows that the model extensions result in better agreement, consistent with a more extensive comparison to global observations as well as measurements of elemental composition downwind of the Sahara, as described in companion articles.

aerosols↗

Exploring Climatology and Long-Term Variations of Aerosols from NASA Reanalysis MERRA-2 with Giovanni

Dust plays important roles in energy cycle and climate variations. The dust deposition is the major source of iron in the open ocean, which is an essential micronutrient for phytoplankton growth and therefore may influence the ocean uptake of atmospheric CO2. Mineral dust can also act as fertilizer for forests over long time periods. Over 35 years of simulated global aerosol products from NASA atmospheric reanalysis, second Modern-Era Retrospective analysis for Research and Applications (MERRA-2) are available from NASA Goddard Earth Science Data and Information Services Center (GES DISC). The MERRA-2 covers the period 1980-present, continuing as an ongoing climate analysis. Aerosol assimilation is included throughout the period, using MODIS, MISR, AERONET, and AVHRR (in the pre-EOS period). The aerosols are assimilated by using MERRA-2 aerosol model, which interact directly with the radiation parameterization, and radiatively coupled with atmospheric model dynamics in the Goddard Earth Observing System Model, Version 5 (GEOS-5). Dust deposition data along with other major aerosol compositions (e.g. black carbon, sea salt, and sulfate, etc.) are simulated as dry and wet deposition, respectively. The hourly and monthly data are available at spatial resolution of 0.5ox0.625o (latitude x longitude). Quick data exploration of climatology and interannual variations of MERRA-2 aerosol can be done through the online visualization and analysis tool, Giovanni. This presentation, using dust deposition as an example, demonstrates a number of MERRA-2 data services at GES DISC. Global distributions of dust depositions, and their seasonal and inter-annual variations are investigated from MERRA-2 monthly aerosol products.

data services↗

Aerosol Properties Derived from Airborne Sky Radiance and Direct Beam Measurements in Recent NASA and DoE Field Campaigns

The AERONET (AErosol RObotic NETwork) ground-based suite of sunphotometers provides measurements of spectral aerosol optical depth (AOD), precipitable water and spectral sky radiance, which can be inverted to retrieve aerosol microphysical properties that are critical to assessments of aerosol-climate interactions. Because of data quality criteria and sampling constraints, there are significant limitations to the temporal and spatial coverage of AERONET data and their representativeness for global aerosol conditions.The 4STAR (Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research) instrument, jointly developed by NASA Ames and PNNL (Pacific Northwest National Laboratory) with NASA Goddard collaboration, combines airborne sun tracking and AERONET-like sky scanning with spectroscopic detection. Being an airborne instrument, 4STAR has the potential to fill gaps in the AERONET data set. The 4STAR instrument operated successfully in the SEAC4RS (Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys) experiment in Aug./Sep. 2013 aboard the NASA DC-8 and in the DoE (Department of Energy)-sponsored TCAP (Two Column Aerosol Project, July 2012 & Feb. 2013) experiment aboard the DoE G-1 aircraft. 4STAR provided direct beam measurements of hyperspectral AOD, columnar trace gas retrievals (H2O, O3, NO2), and the first ever airborne hyperspectral sky radiance scans, which can be inverted to yield the same products as AERONET ground-based observations. In this presentation, we provide an overview of the new 4STAR capabilities, with an emphasis on 26 high-quality sky radiance measurements carried out by 4STAR in SEAC4RS. We compare collocated 4STAR and AERONET sky radiances, as well as their retrievals of aerosol microphysical properties for a subset of the available case studies. We summarize the particle property and air-mass characterization studies made possible by the combined 4STAR direct beam and sky radiance observations.

DoE↗

Retrieving the Height of Smoke and Dust Aerosols by Synergistic Use of Multiple Satellite Sensors

The Aerosol Single scattering albedo and Height Estimation (ASHE) algorithm was first introduced in Jeong and Hsu (2008) to provide aerosol layer height and single scattering albedo (SSA) for biomass burning smoke aerosols. By using multiple satellite sensors synergistically, ASHE can provide the height information over much broader areas than lidar observations alone. The complete ASHE algorithm uses aerosol data from MODIS or VIIRS, OMI or OMPS, and CALIOP. A simplified algorithm also exists that does not require CALIOP data as long as the SSA of the aerosol layer is provided by another source. Several updates have recently been made: inclusion of dust layers in the retrieval process, better determination of the input aerosol layer height from CALIOP, improvement in aerosol optical depth (AOD) for nonspherical dust, development of quality assurance (QA) procedure, etc.

satellite remote sensing↗

Implementing Marine Organic Aerosols Into the GEOS-Chem Model

Marine-sourced organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large under-prediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having > 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.

Aerosols↗

Aerosol Optical Depth as Observed by the Mars Science Laboratory REMS UV Photodiodes

Systematic observations taken by the REMS UV photodiodes on a daily basis throughout the landed Mars Science Laboratory mission provide a highly useful tool for characterizing aerosols above Gale Crater. Radiative transfer modeling is used to model the approximately two Mars Years of observations taken to date taking into account multiple scattering from aerosols and the extended field of view of the REMS UV photodiodes. The retrievals show in detail the annual cycle of aerosol optical depth, which is punctuated with numerous short timescale events of increased optical depth. Dust deposition onto the photodiodes is accounted for by comparison with aerosol optical depth derived from direct imaging of the Sun by Mastcam. The effect of dust on the photodiodes is noticeable, but does not dominate the signal. Cleaning of dust from the photodiodes was observed in the season around Ls=270deg, but not during other seasons. Systematic deviations in the residuals from the retrieval fit are indicative of changes in aerosol effective particle size, with larger particles present during periods of increased optical depth. This seasonal dependence of aerosol particle size is expected as dust activity injects larger particles into the air, while larger aerosols settle out of the atmosphere more quickly leading to a smaller average particle size over time. A full description of these observations, the retrieval algorithm, and the results can be found in Smith et al. (2016).

Aerosol↗

Coupled Aerosol-Cloud Systems over Northern Vietnam during 7-SEAS BASELInE: A Radar and Modeling Perspective

The 2013 7-SEASBASELInE campaign over northern Southeast Asia (SEA) provided, for the first time ever, comprehensive ground-based W-band radar measurements of the low-level stratocumulus (Sc) systems that often exist during the spring over northern Vietnam in the presence of biomass-burning aerosols. Although spatially limited, ground-based remote sensing observations are generally free of the surface contamination and signal attenuation effects that often hinder space-borne measurements of these low-level cloud systems. Such observations permit detailed measurements of structures and lifecycles of these clouds as part of a broader effort to study potential impacts of these coupled aerosol-cloud systems on local and regional weather and air quality. Introductory analyses of the W-band radar data show these Sc systems generally follow a diurnal cycle, with peak occurrences during the nighttime and early morning hours, often accompanied by light precipitation. Preliminary results from idealized simulations of Sc development over land based on the observations reveal the familiar response of increased numbers and smaller sizes of cloud droplets, along with suppressed drizzle formation, as aerosol concentrations increase. Slight reductions in simulated W-band reflectivity values also are seen with increasing aerosol concentrations and result primarily from decreased droplet sizes. As precipitation can play a large role in removing aerosol from the atmosphere, and thereby improving air quality locally, quantifying feedbacks between aerosols and cloud systems over this region are essential, particularly given the negative impacts of biomass burning on human health in SEA. Such an endeavor should involve improved modeling capabilities along with comprehensive measurements of time-dependent aerosol and cloud profiles.

aerosol cloud interactions↗

In-Situ and Remotely-Sensed Observations of Biomass Burning Aerosols at Doi Ang Khang, Thailand During 7-SEAS BASELInE 2015

The spring 2015 deployment of a suite of instrumentation at Doi Ang Khang (DAK) in northwestern Thailand enabled the characterization of air masses containing smoke aerosols from burning predominantly in Myanmar. Aerosol Robotic Network (AERONET) Sun photometer data were used to validate Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 6 "Deep Blue" aerosol optical depth (AOD) retrievals; MODIS Terra and Aqua provided results of similar quality, with correlation coefficients of 0.93-0.94 and similar agreement within expected uncertainties to global-average performance. Scattering and absorption measurements were used to compare surface and total column aerosol single scatter albedo (SSA); while the two were well-correlated, and showed consistent positive relationships with moisture (increasing SSA through the season as surface relative humidity and total columnar water vapor increased), in situ surface-level SSA was nevertheless significantly lower by 0.12-0.17. This could be related to vertical heterogeneity and/or instrumental issues. DAK is at approximately 1,500 meters above sea level in heterogeneous terrain, and the resulting strong diurnal variability in planetary boundary layer depth above the site leads to high temporal variability in both surface and column measurements, and acts as a controlling factor to the ratio between surface particulate matter (PM) levels and column AOD. In contrast, while some hygroscopic effects were observed relating to aerosol particle size and Angstrom exponent, relative humidity variations appear to be less important for this ratio here. As part of the Seven South-East Asian Studies (7-SEAS) project, the Biomass-burning Aerosols & Stratocumulus Environment: Lifecycles and Interactions Experiment (BASELInE) was intended to probe physicochemical processes, interactions, and feedbacks related to biomass burning aerosols and clouds during the spring burning season (February-April) in southeast Asia (SEA).

biomass burning↗

Comparisons of Spectral Aerosol Single Scattering Albedo in Seoul, South Korea

Quantifying aerosol absorption at ultraviolet (UV) wavelengths is important for monitoring air pollution and aerosol amounts using current (e.g., Aura/OMI (Ozone Monitoring Instrument)) and future (e.g., TROPOMI (TROPOspheric Monitoring Instrument), TEMPO (Tropospheric Emissions: Monitoring of POllution), GEMS (Geostationary Environment Monitoring Spectrometer) and Sentinel-4) satellite measurements. Measurements of column average atmospheric aerosol single scattering albedo (SSA) are performed on the ground by the NASA AERONET (AEROsol robotic NETwork) in the visible (VIS) and near-infrared (NIR) wavelengths and in the UV-VIS-NIR by the SKYNET (SKY radiometer NETwork) networks. Previous comparison studies have focused on VIS and NIR wavelengths due to the lack of co-incident measurements of aerosol and gaseous absorption properties in the UV. This study compares the SKYNET-retrieved SSA in the UV with the SSA derived from a combination of AERONET, MFRSR (MultiFilter Rotating Shadowband Radiometer), and Pandora (AMP) retrievals in Seoul, South Korea, in spring and summer 2016. The results show that the spectrally invariant surface albedo assumed in the SKYNET SSA retrievals leads to underestimated SSA compared to AMP values at near UV wavelengths. Re-processed SKYNET inversions using spectrally varying surface albedo, consistent with the AERONET retrieval improve agreement with AMP SSA. The combined AMP inversions allow for separating aerosol and gaseous (NO2 and O3) absorption and provide aerosol retrievals from the shortest UVB (305 nanometers) through VIS to NIR wavelengths (870 nanometers).

aerosol and gaseous absorption properties↗

Satellite-Based View of the Aerosol Spatial and Temporal Variability in the Cordoba Region (Argentina) Using over Ten Years of High-Resolution Data

Space-based observations offer a unique opportunity to investigate the atmosphere and its changes over decadal time scales, particularly in regions lacking in situ and/or ground based observations. In this study, we investigate temporal and spatial variability of atmospheric particulate matter (aerosol) over the urban area of Córdoba (central Argentina) using over ten years (2003–2015) of high-resolution (1 km) satellite-based retrievals of aerosol optical depth (AOD). This fine resolution is achieved exploiting the capabilities of a recently developed inversion algorithm (Multiangle implementation of atmospheric correction, MAIAC) applied to the MODIS sensor datasets of the NASA-Terra and -Aqua platforms. Results of this investigation show a clear seasonality of AOD over the investigated area. This is found to be shaped by an intricate superposition of aerosol sources, acting over different spatial scales and affecting the region with different yearly cycles. During late winter and spring (August-October), local as well as near- and long-range transported biomass burning (BB) aerosols enhance the Córdoba aerosol load, and AOD levels reach their maximum values (>0.35 at 0.47 µm). The fine AOD spatial resolution allowed to disclose that, in this period, AOD maxima are found in the rural/agricultural area around the city, reaching up to the city boundaries pinpointing that fires of local and near-range origin play a major role in the AOD enhancement. A reverse spatial AOD gradient is found from December to March, the urban area showing AODs 40–80% higher than in the city surroundings. In fact, during summer, the columnar aerosol load over the Córdoba region is dominated by local (urban and industrial) sources, likely coupled to secondary processes driven by enhanced radiation and mixing effects within a deeper planetary boundary layer (PBL). With the support of modelled AOD data from the Modern-Era Retrospective Analysis for Research and Application (MERRA), we further investigated into the chemical nature of AOD. The results suggest that mineral dust is also an important aerosol component in Córdoba, with maximum impact from November to February. The use of a long-term dataset finally allowed a preliminary assessment of AOD trends over the Córdoba region. For those months in which local sources and secondary processes were found to dominate the AOD (December to March), we found a positive AOD trend in the Córdoba outskirts, mainly in the areas with maximum urbanization/population growth over the investigated decade. Conversely, a negative AOD trend (up to −0.1 per decade) is observed all over the rural area of Córdoba during the BB season, this being attributed to a decrease of fires both at the local and the continental scale.

aerosols↗

Retrieval of Daily Maps of PM2.5 Aerosol in the Problematic California Valleys: Bright, Speckled Reflectances, Thin AOT, but High Pollution

The San Joaquin Valley suffers from severe episodes of respirable aerosol (PM2.5) in wintertime.We provide maps of aerosol episodes using daily snapshots of PM2.5 and its changing features despite numerous difficulties inherent to sampling the region. Linear relationships relating aerosol optical thickness (AOT) to PM2.5 give an explained variance of approximately 3.The GEO-CAPE mission has as a goal the provision of relevant measures of respirable aerosol to the community,but has not formulated a science goal beyond the limited goal of retrieval of AOT, bringing the usefulness of GEO-CAPE into doubt.Our special focus was on the DISCOVER-AQ period, Jan-Feb 2013, which had many supporting measurements.Both high pollution and retrieval difficulties tend to occur in many Mediterranean agricultural regions like the San Joauin. One difficulty is the relatively bright surfaces with considerable exposed soil. NASAs MAIAC and MODIS Deep Blue retrieval techniques are shown to have considerable skill even at low aerosol optical thickness (AOT) values, as evaluated by concurrent AERONET sunphotometer measurements.More significantly, these AOT values can correspond to high daytime PM2.5 since aerosol mixed layer depth is thin and variable, 200m 600 m. The thin layers derive from typical subsidence of dry air between more stormy periods. This situation provides an advantage: water vapor column is also almost completely limited to a similar mixed layer depth, and can thus serve as a measure of aerosol dilution.Using the MAIAC Water Vapor Column:In order to make the maps below, we used the MAIAC data but subtracted partial water-vapor columns estimated from MERRA Reanalysis Data availabe from the GSFC GMAO using kriging. We did not use the mixed-layer estimates from MERRA, since such analyses were found problematic during our forecasting exercises for DISCOVER-AQ. Observations from the aircraft soundings suggested that this overlying moisture was mostly due to larger scale flows, not ML venting.However, the specific humidity at the surface and a nearly well-mixed ML was analyzed by kriging from the surface network (MesoWest, University of Utah). These were thought to be truer, uninfluenced by physical process modeling that combines with data observations. (TBD: How different are they?) Procedure: Subtract overlying partial water columns from MAIAC column water and divide this by a surface value of water vapor. (MAIAC column is expressed in cm of water, i.e., water vapor at surface conditions.This method appears to bring out useful details in the distribution of submicron particles in the very problematic Wintertime San Joaquin Valley, and allow analysis of pollution episodes throughout the valley, rather than long-term averages.

san joaquin valley↗

Apparent dust size discrepancy in aerosol reanalysis in north African dust after long-range transport

North African dust reaches the southeastern United States every summer. Size-resolved dust mass measurements taken in Miami, Florida, indicate that more than one-half of the surface dust mass concentrations reside in particles with geometric diameters less than 2.1 µm, while vertical profiles of micropulse lidar depolarization ratios show dust reaching above 4 km during pronounced events. These observations are compared to the representation of dust in the Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) aerosol reanalysis and closely related Goddard Earth Observing System model version 5 (GEOS-5) Forward Processing (FP) aerosol product, both of which assimilate satellite-derived aerosol optical depths using a similar protocol and inputs. These capture the day-to-day variability in aerosol optical depth well, in a comparison to an independent sun-photometer-derived aerosol optical depth dataset. Most of the modeled dust mass resides in diameters between 2 and 6 µm, in contrast to the measurements. Model-specified mass extinction efficiencies equate light extinction with approximately 3 times as much aerosol mass, in this size range, compared to the measured dust sizes. GEOS-5 FP surface-layer sea salt mass concentrations greatly exceed observed values, despite realistic winds and relative humidities. In combination, these observations help explain why, despite realistic total aerosol optical depths, (1) free-tropospheric model volume extinction coefficients are lower than those retrieved from the micro-pulse lidar, suggesting too-low model dust loadings in the free troposphere, and (2) model dust mass concentrations near the surface can be higher than those measured. The modeled vertical distribution of dust, when captured, is reasonable. Large, aspherical particles exceeding the modeled dust sizes are also occasionally present, but dust particles with diameters exceeding 10 µm contribute little to the measured total dust mass concentrations after such long-range transport. Remaining uncertainties warrant a further integrated assessment to confirm this study's interpretations.

MEERA-2 aerosols reanalysis↗

Detecting Layer Height of Smoke Aerosols over Vegetated Land and Water Surfaces via Oxygen Absorption Bands: Hourly Results from EPIC/DSCOVR in Deep Space

We present an algorithm for retrieving aerosol layer height (ALH) and aerosol optical depth (AOD) for smoke over vegetated land and water surfaces from measurements of the Earth Polychromatic Imaging Camera (EPIC) onboard the Deep Space Climate Observatory (DSCOVR). The algorithm uses Earth-reflected radiances in six EPIC bands in the visible and near-infrared and incorporates flexible spectral fitting that accounts for specifics of land and water surface reflectivity. The fitting procedure first determines AOD using EPIC atmospheric window bands (443 nm, 551 nm, 680nm, and 780 nm), then uses oxygen (O2) A and B bands (688 nm and 764 nm) to derive ALH, which represents an optical centroid altitude. ALH retrieval over vegetated surface primarily takes advantage of measurements in the O2B band. We applied the algorithm to EPIC observations of several biomass burning events over the United States and Canada in August 2017. We found that the algorithm can be used to obtain AOD and ALH multiple times daily over water and vegetated land surface. Validation is performed against aerosol extinction profiles detected by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and against AOD observed at nine Aerosol Robotic Network (AERONET) sites, showing, on average, an error of 0.58 km and a bias of -0.13 km in retrieved ALH and an error of 0.05 and a bias of 0.03 in retrieved AOD. Additionally, we show that the aerosol height information retrieved by the present algorithm can potentially benefit the retrieval of aerosol properties from EPIC’s ultraviolet (UV) bands.

Cloud–Aerosol Lidar with Orthogonal Polarization (↗

Observation of absorbing aerosols above clouds over the South-East Atlantic Ocean from the geostationary satellite SEVIRI - Part 2: Comparison with MODIS and aircraft measurements from the CLARIFY-2017 field campaign

To evaluate the SEVIRI retrieval for aerosols above clouds presented in Part 1 of the companion paper, the algorithm is applied over the south-east Atlantic Ocean during the CLARIFY-2017 field campaign period. The first step of our analysis compares the retrieved aerosol and cloud properties against equivalent products from the MODIS MOD06ACAERO retrieval (Meyer et al., 2015). While the correlation between the two satellite retrievals of the above-cloud aerosol optical thickness (AOT) is good (R = 0.78), the AOT retrieved by SEVIRI is 20.3 % smaller than that obtained from the MODIS retrieval. This difference in AOT is attributed mainly to the more absorbing aerosol model assumed for the SEVIRI retrieval compared to MODIS. The underlying cloud optical thickness (COT) derived from the two satellites is in good agreement (R = 0.90). The cloud droplet effective radius (CER) retrieved by SEVIRI is consistently smaller than MODIS by 2.2 µm, which is mainly caused by the use of different spectral bands of the satellite instruments. In the second part of our analysis, we compare the forecast water vapour profiles used for the SEVIRI atmospheric correction as well as the aforementioned aerosol and cloud products with in situ measurements made from the Facility for Airborne Atmospheric Measurements (FAAM) aircraft platform during the CLARIFY-2017 campaign. Around Ascension Island, the column water vapour used to correct the SEVIRI signal is overestimated by 3.1 mm in the forecast compared to that measured by dropsondes. However, the evidence suggests that the accuracy of the atmospheric correction improves closer to the African coast. Consistency is observed between the SEVIRI above-cloud AOT and in situ measurements (from cavity ring-down spectroscopy instruments) when the measured single-scattering albedo is close to that assumed in the retrieval algorithm. On the other hand, the satellite retrieval overestimates the AOT when the assumed aerosol model is not absorbing enough. Consistency is also found between the cloud properties retrieved by SEVIRI and the CER measured by a cloud droplet probe and the liquid water path derived from a microwave radiometer. Despite the instrumental limitations of the geostationary satellite, the consistency obtained between SEVIRI, MODIS and the aircraft measurements demonstrates the ability of the retrieval in providing additional information on the temporal evolution of the aerosol properties above clouds.

absorbing aerosols↗

Analysis of Near-Cloud Changes in Atmospheric Aerosols Using Satellite Observations and Global Model Simulations

This paper examines cloud-related variations of atmospheric aerosols that occur in partly cloudy regions containing low-altitude clouds. The goal is to better understand aerosol behaviors and to help better represent the radiative effects of aerosols on climate. For this, the paper presents a statistical analysis of a multi-month global dataset that combines data from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instruments with data from the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) global reanalysis. Among other findings, the results reveal that near-cloud enhancements in lidar backscatter (closely related to aerosol optical depth) are larger (1) over land than ocean by 35%, (2) near optically thicker clouds by substantial amounts, (3) for sea salt than for other aerosol types, with the difference from dust reaching 50%. Finally, the study found that mean lidar backscatter is higher near clouds not because of large-scale variations in meteorological conditions, but because of local processes associated with individual clouds. The results help improve our understanding of aerosol-cloud-radiation interactions and our ability to represent them in climate models and other atmospheric models

aerosol↗

Above-Aircraft Cirrus Cloud and Aerosol Optical Depth From Hyperspectral Irradiances Measured By a Total-Diffuse Radiometer

This study develops the use of spectral total and diffuse irradiance measurements, made from a prototype hyperspectral total-diffuse sunshine pyranometer (SPN-S), to retrieve layer fine-mode aerosol (τ aer ) and total optical depths from airborne platforms. Additionally, we use spectral analysis in an attempt to partition the total optical depth into its τ aer and cirrus cloud optical depth (τ cld ) components in the absence of coarse-mode aerosols. Two retrieval methods are developed: one leveraging information in the diffuse irradiance and the other using spectral characteristics of the transmitted direct beam, with each approach best suited for specific cloud and aerosol conditions. The SPN-S has advantages over traditional sun photometer systems, including no moving parts and a low cost. However, a significant drawback of the instrument is that it is unable to measure the direct-beam irradiance as accurately as sun photometers. To compensate for the greater measurement uncertainty in the radiometric irradiances, these retrieval techniques employ ratioed inputs or spectral information to reduce output uncertainty. This analysis uses irradiance measurements from the SPN-S and the solar spectral flux radiometer (SSFR) aboard the National Aeronautics and Space Administration’s (NASA) P-3 aircraft during the 2018 deployment of the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) campaign and the 2019 Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP 2 Ex) mission to quantify above-aircraft cirrus τ cld and derive vertical profiles of layer τ aer . Validation of the τ aer retrieval is accomplished by comparison with co-located measurements of direct solar irradiance made by the Sky-Scanning Sun-Tracking Atmospheric Research (4STAR) and in situ measurements of aerosol optical depth. For the aggregated 2018 ORACLES results, regression between the SPN-S-based method and sun photometer τ aer values yields a slope of 0.96 with an R 2 of 0.96, while the root mean square error (RMSE) is 3.0 x 10 -2 . When comparing the retrieved τ aer to profiles of integrated in situ measurements of optical extinction, the slope, R 2 , and RMSE values for ORACLES are 0.90, 0.96, and 3.4 x 10 -2 , and for CAMP 2 Ex they are 0.94, 0.97, and 3.4 x 10 -2 , respectively. This paper is a demonstration of methods for deriving cloud and aerosol optical properties in environments where both atmospheric constituents may be present. With improvements to the low-cost SPN-S radiometer instrument, it may be possible to extend these methods to a broader set of sampling applications, such as ground-based settings.

spectral instrument (SPN-S)↗

Secondary Inorganic Aerosol Chemistry and Its Impact on Atmospheric Visibility Over an Ammonia-Rich Urban Area in Central Taiwan

This study investigated the hourly inorganic aerosol chemistry and its impact on atmospheric visibility over an urban area in Central Taiwan, by relying on measurements of aerosol light extinction, inorganic gases, and PM 2.5 water-soluble ions (WSIs), and simulations from a thermodynamic equilibrium model. On average, the sulfate (SO 4 2− ), nitrate (NO 3 − ), and ammonium (NH 4 + ) components (SNA) contributed ∼90% of WSI concentrations, which in turn made up about 50% of the PM 2.5 mass. During the entire observation period, PM 2.5 and SNA concentrations, aerosol pH, aerosol liquid water content (ALWC), and sulfur and nitrogen conversion ratios all increased with decreasing visibility. In particular, the NO 3 − contribution to PM 2.5 increased, whereas the SO 4 2− contribution decreased, with decreasing visibility. The diurnal variations of the above parameters indicate that the interaction and likely mutual promotion between NO 3 − and ALWC enhanced the hygroscopicity and aqueous-phase reactions conducive for NO 3 − formation, thus led to severely impaired visibility. The high relative humidity (RH) at the study area (average 70.7%) was a necessary but not sole factor leading to enhanced NO 3 − formation, which was more directly associated with elevated ALWC and aerosol pH. Simulations from the thermodynamic model depict that the inorganic aerosol system in the study area was characterized by fully neutralized SO 4 2− (i.e. a saturated factor in visibility reduction) and excess NH 4 + amidst a NH 3 -rich environment. As a result, PM 2.5 composition was most sensitive to gas-phase HNO 3 , and hence NOx, and relatively insensitive to NH 3 . Consequently, a reduction of NOx would result in instantaneous cuts of NO 3 − , PM 2.5 , and ALWC, and hence improved visibility. On the other hand, a substantial amount of NH 3 reduction (>70%) would be required to lower the aerosol pH, driving more than 50% of the particulate phase NO 3 − to the gas phase, thereby making NH 3 a limiting factor in shifting PM 2.5 composition.

aerosol chemistry↗

The Complex Refractive Indices of Mineral Aerosols and Why They Matter

Aerosol refractive indices are fundamental parameters that are generally measured by spec-troscopists with specialized knowledge. We in the Earth science community frequently utilizethese refractive indices because they are essential for computing aerosol radiative effects andretrieving aerosol composition. Unfortunately, there are a wide variety of refractive indiceswith significant differences for some aerosol species (e.g., hematite) and a lack of refractiveindex choices for other aerosols (e.g., clay minerals, goethite), and this hinders our ability toaccurately compute the radiative effect of mineral dust. Additionally, the mineral refractiveindices used in atmospheric science are not necessarily linked to the mineral reflectancesused to identify surface mineralogy; this creates a disconnect between the atmosphere andthe surface that frustrates closure analyses.In this talk, we will present an overview of some refractive indices of radiative importancein aeolian dust (illite, kaolinite, montmorillonite, hematite, goethite). We will discuss howmineral refractive indices are used in aerosol retrievals, and how we can use remote sensingretrievals to narrow the range of viable choices. We will also discuss how we can use pub-lished spectroscopic measurements to extrapolate the refractive indices that are inferred ata handful of visible and near-infrared wavelengths to the longwave regime. Finally, we willdiscuss how working groups like MIRA (Models, In situ, and Remote sensing of Aerosols;https://science.larc.nasa.gov/mira-wg/) and community repositories like TAO (Tables ofAerosol Optics) can improve radiative closure by enhancing interactions between the threedisciplines.1

aerosols↗