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NASA NTRS2016

Multi-Sensor Cloud and Aerosol Retrieval Simulator and Remote Sensing from Model Parameters : Aerosols - Part 2

The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a simulated radiance product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers. This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled. In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model sub grid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to operational remote-sensing algorithms. Specifically, the MCARS-computed radiances are input into the processing chain used to produce the MODIS Data Collection 6 aerosol product (MOYD04). TheMOYD04 product is of course normally produced from MOYD021KM MODIS Level-1B radiance product directly acquired by the MODIS instrument. MCARS matches the format and metadata of a MOYD021KM product. The resulting MCARS output can be directly provided to MODAPS (MODIS Adaptive Processing System) as input to various operational atmospheric retrieval algorithms. Thus the operational algorithms can be tested directly without needing to make any software changes to accommodate an alternative input source. We show direct application of this synthetic product in analysis of the performance of the MOD04 operational algorithm. We use biomass-burning case studies over Amazonia employed in a recent Working Group on Numerical Experimentation (WGNE)-sponsored study of aerosol impacts on numerical weather prediction (Freitas et al., 2015). We demonstrate that a known low bias in retrieved MODIS aerosol optical depth appears to be due to a disconnect between actual column relative humidity and the value assumed by the MODIS aerosol product.

aerosol retrieval↗

DOE OSTI2023

Measurements of aerosol microphysical and chemical properties in the central Arctic atmosphere during MOSAiC

The Arctic environment is transforming rapidly due to climate change. Aerosols’ abundance and physicochemical characteristics play a crucial, yet uncertain, role in these changes due to their influence on the surface energy budget through direct interaction with solar radiation and indirectly via cloud formation. Importantly, Arctic aerosol properties are also changing in response to climate change. Despite their importance, year-round measurements of their characteristics are sparse in the Arctic and often confined to lower latitudes at Arctic land-based stations and/or short high-latitude summertime campaigns. Here, we present unique aerosol microphysics and chemical composition datasets collected during the year-long Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition, in the central Arctic. These datasets, which include aerosol particle number concentrations, size distributions, cloud condensation nuclei concentrations, fluorescent aerosol concentrations and properties, and aerosol bulk chemical composition (black carbon, sulfate, nitrate, ammonium, chloride, and organics) will serve to improve our understanding of high-Arctic aerosol processes, with relevance towards improved modelling of the future Arctic (and global) climate.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2018

PACE Technical Report Series, Volume 4: Cloud Retrievals in the PACE Mission: PACE Science Team Consensus Document

Earth is a complex dynamical system exhibiting continuous change in its atmosphere, ocean,and surface elements. Nearly all (99.97%) of the energy driving these systems is linked to the Sun. Measurements of reflected sunlight contain a unique signature of wavelength-specific scattering and absorption interactions occurring between incoming solar energy and atmospheric (molecules, aerosols,clouds) and surface features Clouds can affect significantly both shortwave and long wave radiation, depending on altitude/vertical structure, thermodynamic phase, and optical properties. Low, warm, and optically thick clouds predominantly have a cooling effect, while high, cold, optically thin clouds can cause warming by absorbing warmer radiation emitted from the surface and lower atmosphere.When the net difference between outgoing and incoming solar radiation is matched by the net infrared radiation emitted to space, the Earth's climate is in radiative balance. While radiative forcing components (GHGs, aerosols - direct and indirect) contribute to a net radiative imbalance, climate sensitivity is ultimately determined by the contribution of various system feed backs. The role of cloud feedback in a warming climate is currently the largest inter-model uncertainty in climate sensitivity and therefore in climate prediction [Bony and Dufresne 2005]. A comprehensive understanding of current cloud propertiesand dynamic/microphysical processes requires a global perspective from satellites.

Plankton, Aerosol, Cloud, ocean Ecosystem (PACE)↗

NASA NTRSDate not supplied

TPSAS-NF1676L-10947-DND

There are large uncertainties in quantifying dust effects on the climate because of the limitations on the measurements and observations of dust-cloud-precipitation-dynamics interactions. As a major terrestrial source of atmospheric aerosols, dusts may serve as a significant climate forcing for the changing climate due to its effect on solar and thermal radiation as well as on clouds and precipitation processes. Latest satellites measurements enable us to determine dust loadings and cloud distributions and can potentially be used to reduce the uncertainties in the estimations of aerosol effects on climate. This study uses sensors on various satellites to investigate the impact of mineral dust on cloud microphysical and precipitation processes in convective systems. A trans-Atlantic dust outbreak of Saharan origin occurring in early March 2004 is considered. For the observed convective systems under a given convective strength, small hydrometeors were found more prevalent in the dusty stratiform regions than in those regions that were dust free. Evidence of abundant cloud ice particles in the dust regions, particularly at altitudes where heterogeneous nucleation of mineral dust prevails, further supports the observed changes of clouds and precipitation. These microphysical effects of the dusts on clouds are to shift the size spectrum of precipitation-sized hydrometeors from heavy precipitation to light precipitation and ultimately to suppress precipitation and increase the lifecycle of cloud systems, especially for stratiform clouds.

B Lin↗

DOE OSTI2017

Condensed-phase biogenic-anthropogenic interactions with implications for cold cloud formation

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil-fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without presence of sulfate or soot particles. Corresponding particle glass transition (T g ) and full deliquescence relative humidity (FDRH) were estimated by a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibit a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation in agreement with respective T g and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid inducing ice nucleation. Naphthalene SOA coated soot particles acted as IN above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate further renders this even less likely. Furthermore, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during preindustrial times or in pristine areas.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

Data from both laboratory studies and atmospheric measurements are used to develop an empirical parameterization for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RH w ) are taken as a measure of the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterization developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A calibration factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RH w of 105% vs. maximum fractions active at higher RH w . Instrumental factors that affect activation behavior vs. RH w in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this calibration factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization, including calibration correction, to predictions of the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first-order approximation in numerical modeling investigations.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2018

Characterizing Differences in the Aerosol Plume and Cloud Structure over Ascension Island During the 2016 and 2017 Biomass Burning Seasons

Marine boundary layer clouds, including the transition from stratocumulus to cumulus, are poorly represented in numerical weather prediction and general circulation models. In many cases, the complex physical relationships between marine boundary cloud morphology and the environmental conditions in which the clouds exist are not well understood. Such uncertainties arise in the presence of biomass burning carbonaceous aerosol, as is the case over the southeast Atlantic Ocean. It is likely that the absorbing and heating properties of these aerosols influence the microphysical composition and macrophysical arrangement of marine stratocumulus and trade cumulus in this region; however, this has yet to be quantified. The deployment of the Atmospheric Radiation Measurement Mobile Facility #1 (AMF1) in support of LASIC (Layered Atlantic Smoke Interactions with Clouds) provided a unique opportunity to collect observations of cloud and aerosol properties during two consecutive biomass burning seasons during July through October of 2016 and 2017 over Ascension Island (7.96 S, 14.35 W). Through the use of AMF1 observations, the Modern Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2), and back trajectories from the Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT), it will be demonstrated that differences in the atmospheric circulation during the two years result in varying aerosol conditions over Ascension Island. When the aerosol plume is overhead, the aerosol loading is higher during the 2016 season as a result of a weaker subtropical high-pressure system. Furthermore, the aerosol plume originates from central Africa in 2016, but further south in 2017. Contrasts in the season-to-season and day-to-day aerosol loading are used to categorize boundary layer cloud and sub-cloud turbulence measurements above Ascension Island using the AMF1 Doppler lidar and cloud radar.

Collow, Allison B. Marquardt↗

NASA NTRS2019

Aerosol Radiative Effects over Ascension Island Using LASIC Observations and MERRA-2

Marine boundary layer clouds, including the transition from stratocumulus to cumulus, are poorly represented in numerical weather prediction and general circulation models. In many cases, the complex physical relationships between marine boundary cloud morphology and the environmental conditions in which the clouds exist are not well understood. Such uncertainties arise in the presence of biomass burning carbonaceous aerosol, as is the case over the southeast Atlantic Ocean. It is likely that the absorbing and heating properties of these aerosols influence the microphysical composition and macrophysical arrangement of marine stratocumulus and trade cumulus in this region; however, this has yet to be quantified. The deployment of the Atmospheric Radiation Measurement Mobile Facility #1 (AMF1) in support of LASIC (Layered Atlantic Smoke Interactions with Clouds) provided a unique opportunity to collect observations of cloud and aerosol properties during two consecutive biomass burning seasons during July through October of 2016 and 2017 over Ascension Island (7.96 S, 14.35 W). Thermodynamic profiles will be analyzed through the unique combination of sounding data from radiosonde launches and microwave profiling radiometers, giving observations of additional quantities important for cloud development such as CAPE and CIN at a fine temporal resolution. The thermodynamic profiles will be presented in conjunction with detailed observations of the cloud structure over the site from a K-band cloud radar, micropulse lidar, and laser ceilometer. Finally, the observed thermodynamic and cloud profiles will be used as input forcing, alongside aerosols from the Modern Era Retrospective analysis for Research and Applications, version 2 (MERRA-2), for the Rapid Radiative Transfer Model (RRTM) to gain information regarding the radiative heating profiles. Idealized experiments using RRTM with and without aerosols will be used to quantify the impact of biomass burning carbonaceous aerosol plumes as they pass over the site.

Collow, Allie↗

NASA NTRS2019

Thermodynamic, Cloud, and Radiative Heating Profiles over Ascension Island During the 2016 and 2017 Biomass Burning Seasons

Marine boundary layer clouds, including the transition from stratocumulus to cumulus, are poorly represented in numerical weather prediction and general circulation models. In many cases, the complex physical relationships between marine boundary cloud morphology and the environmental conditions in which the clouds exist are not well understood. Such uncertainties arise in the presence of biomass burning carbonaceous aerosol, as is the case over the southeast Atlantic Ocean. It is likely that the absorbing and heating properties of these aerosols influence the microphysical composition and macrophysical arrangement of marine stratocumulus and trade cumulus in this region; however, this has yet to be quantified. The deployment of the Atmospheric Radiation Measurement Mobile Facility #1 (AMF1) in support of LASIC (Layered Atlantic Smoke Interactions with Clouds) provided a unique opportunity to collect observations of cloud and aerosol properties during two consecutive biomass burning seasons during July through October of 2016 and 2017 over Ascension Island (7.96 S, 14.35 W). Thermodynamic profiles will be analyzed through the unique combination of sounding data from radiosonde launches and microwave profiling radiometers, giving observations of additional quantities important for cloud development such as CAPE and CIN at a fine temporal resolution. The thermodynamic profiles will be presented in conjunction with detailed observations of the cloud structure over the site from a K-band cloud radar, micropulse lidar, and laser ceilometer. Finally, the observed thermodynamic and cloud profiles will be used as input forcing, alongside aerosols from the Modern Era Retrospective analysis for Research and Applications, version 2 (MERRA-2), for the Rapid Radiative Transfer Model (RRTM) to gain information regarding the radiative heating profiles. Idealized experiments using RRTM with and without aerosols will be used to quantify the impact of biomass burning carbonaceous aerosol plumes as they pass over the site.

Collow, Allison B.↗

NASA NTRS2020

Radiative Heating from Biomass Burning Aerosol and its Impact on Cloud Structure in the Southeast Atlantic

Marine boundary layer clouds, including the transition from stratocumulus to cumulus, are poorly represented in numerical weather prediction and general circulation models. In many cases, the complex physical relationships between marine boundary cloud morphology and the environmental conditions in which the clouds exist are not well understood. Such uncertainties arise in the presence of biomass burning carbonaceous aerosol, as is the case over the southeast Atlantic Ocean. It is likely that the absorbing and heating properties of these aerosols influence the microphysical composition and macrophysical arrangement of marine stratocumulus and trade cumulus in this region; however, this has yet to be quantified. The deployment of the Atmospheric Radiation Measurement Mobile Facility #1 (AMF1) in support of LASIC (Layered Atlantic Smoke Interactions with Clouds) provided a unique opportunity to collect observations of cloud and aerosol properties during two consecutive biomass burning seasons during July through October of 2016 and 2017 over Ascension Island (7.96 S, 14.35 W). Thermodynamic profiles will be analyzed through the unique combination of sounding data from radiosonde launches and microwave profiling radiometers, giving observations of additional quantities important for cloud development such as CAPE and CIN at a fine temporal resolution. The thermodynamic profiles will be presented in conjunction with detailed observations of the cloud structure over the site from a K-band cloud radar, micropulse lidar, and laser ceilometer. The observed thermodynamic and cloud profiles will be used as input forcing, alongside aerosols from the Modern Era Retrospective analysis for Research and Applications, version 2 (MERRA-2), for the Rapid Radiative Transfer Model (RRTM) to gain information regarding the radiative heating profiles. Idealized experiments using RRTM with and without aerosols will be used to quantify the impact of biomass burning carbonaceous aerosol plumes as they pass over the site. Due to documented discrepancies in the single scatter albedo (SSA) between models and observations, further sensitivity experiments will demonstrate the importance of the optical properties of biomass burning aerosol in accurately representing heating within the column. Finally, the heating rates will be put into context of the cloud structure over the site from the perspective of the mass flux closure from the University of Washington shallow convective scheme.

Collow, Allison↗

DOE OSTI2026

Kent Island Boundary Layer Field Campaign Report

Understanding the mechanisms governing the urban atmospheric environment is critical for informing urban populations about the impacts of climate change and associated mitigation and adaptation measures. The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) User Facility’s Coast-Urban-Rural Atmospheric Gradient Experiment (CoURAGE) was conducted to study the interactions among the earth’s surface, the atmospheric boundary layer (ABL), aerosols, atmospheric composition, clouds, radiation, and precipitation at each experimental site, and to examine how the spatial gradients across the region interact to create the climate conditions in Baltimore. In this activity we performed weekly soundings, alternating between day and night from Kent Island, to get low-frequency, long-term observations of ABL/lower tropospheric thermodynamic structure. However, during the CoURAGE intensive operational period (IOP), we performed high-frequency sampling (2x/day), at times coinciding with CoURAGE IOP soundings at the main site. The short-term, high-frequency sounding information that was launched at 12Z and 18Z was to complement the longer-term data set.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Long-Term Land-Atmosphere Studies in Northern Alabama

A new multiyear research effort in northern Alabama will gather data on how clouds, vegetation, and tiny aerosol particles in the atmosphere interact to affect local weather and Earth’s climate.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2016

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↗

DOE OSTI2014

A Physically Based Framework for Modelling the Organic Fractionation of Sea Spray Aerosol from Bubble Film Langmuir Equilibria

The presence of a large fraction of organic matter in primary sea spray aerosol (SSA) can strongly affect its cloud condensation nuclei activity and interactions with marine clouds. Global climate models require new parameterizations of the SSA composition in order to improve the representation of these processes. Existing proposals for such a parameterization use remotely-sensed chlorophyll-a concentrations as a proxy for the biogenic contribution to the aerosol. However, both observations and theoretical considerations suggest that existing relationships with chlorophyll-a, derived from observations at only a few locations, may not be representative for all ocean regions. We introduce a novel framework for parameterizing the fractionation of marine organic matter into SSA based on a competitive Langmuir adsorption equilibrium at bubble surfaces. Marine organic matter is partitioned into classes with differing molecular weights, surface excesses, and Langmuir adsorption parameters. The classes include a lipid-like mixture associated with labile dissolved organic carbon (DOC), a polysaccharide-like mixture associated primarily with semi-labile DOC, a protein-like mixture with concentrations intermediate between lipids and polysaccharides, a processed mixture associated with recalcitrant surface DOC, and a deep abyssal humic-like mixture. Box model calculations have been performed for several cases of organic adsorption to illustrate the underlying concepts. We then apply the framework to output from a global marine biogeochemistry model, by partitioning total dissolved organic carbon into several classes of macromolecule. Each class is represented by model compounds with physical and chemical properties based on existing laboratory data. This allows us to globally map the predicted organic mass fraction of the nascent submicron sea spray aerosol. Predicted relationships between chlorophyll-\textit{a} and organic fraction are similar to existing empirical parameterizations, but can vary between biologically productive and non-productive regions, and seasonally within a given region. Major uncertainties include the bubble film thickness at bursting and the variability of organic surfactant activity in the ocean, which is poorly constrained. In addition, marine colloids and cooperative adsorption of polysaccharides may make important contributions to the aerosol, but are not included here. This organic fractionation framework is an initial step towards a closer linking of ocean biogeochemistry and aerosol chemical composition in Earth system models. Future work should focus on improving constraints on model parameters through new laboratory experiments or through empirical fitting to observed relationships in the real ocean and atmosphere, as well as on atmospheric implications of the variable composition of organic matter in sea spray.

bubble film↗

DOE OSTI2013

Study of Mechanisms of Aerosol Indirect Effects on Glaciated Clouds: Progress during the Project (Final Technical Report)

This 3-year project has studied how aerosol pollution influences glaciated clouds. The tool applied has been an 'aerosol-cloud model'. It is a type of Cloud-System Resolving Model (CSRM) modified to include 2-moment bulk microphysics and 7 aerosol species, as described by Phillips et al. (2009, 2013). The study has been done by, first, improving the model and then performing sensitivity studies with validated simulations of a couple of observed cases from ARM. These are namely the Tropical Warm Pool International Cloud Experiment (TWP-ICE) over the tropical west Pacific and the Cloud and Land Surface Interaction Campaign (CLASIC) over Oklahoma. During the project, sensitivity tests with the model showed that in continental clouds, extra liquid aerosols (soluble aerosol material) from pollution inhibited warm rain processes for precipitation production. This promoted homogeneous freezing of cloud droplets and aerosols. Mass and number concentrations of cloud-ice particles were boosted. The mean sizes of cloud-ice particles were reduced by the pollution. Hence, the lifetime of glaciated clouds, especially ice-only clouds, was augmented due to inhibition of sedimentation and ice-ice aggregation. Latent heat released from extra homogeneous freezing invigorated convective updrafts, and raised their maximum cloud-tops, when aerosol pollution was included. In the particular cases simulated in the project, the aerosol indirect effect of glaciated clouds was twice than of (warm) water clouds. This was because glaciated clouds are higher in the troposphere than water clouds and have the first interaction with incoming solar radiation. Ice-only clouds caused solar cooling by becoming more extensive as a result of aerosol pollution. This 'lifetime indirect effect' of ice-only clouds was due to higher numbers of homogeneously nucleated ice crystals causing a reduction in their mean size, slowing the ice-crystal process of snow production and slowing sedimentation. In addition to the known indirect effects (glaciation, riming and thermodynamic), new indirect effects were discovered and quantified due to responses of sedimentation, aggregation and coalescence in glaciated clouds to changing aerosol conditions. In summary, the change in horizontal extent of the glaciated clouds ('lifetime indirect effects'), especially of ice-only clouds, was seen to be of higher importance in regulating aerosol indirect effects than changes in cloud properties ('cloud albedo indirect effects').

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2013

Study of Mechanisms of Aerosol Indirect Effects on Glaciated Clouds: Progress during the Project (Final Technical Report)

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Chemical Imaging of Atmospheric Organic Particles in the Southern Great Plains Field Campaign Report

The main goal of this field project was to characterize the chemical and physical properties of atmospheric particles representative of the Southern Great Plains (SGP) environment to establish a relationship between the composition of aerosol particles and their atmospheric impacts. The specific research efforts were focused on in-depth microscopy studies of chemical and physical properties of atmospheric organic particles collected at the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) SGP observatory. An array of novel molecular-level characterization and chemical imaging approaches were used to characterize chemical composition of particles and elucidate fundamental processes governing their atmospheric aging, evolution of chemical composition, optical properties, cloud formation ability, and implications for particle-cloud interactions – the most challenging problems relevant to predictive understanding of aerosol effects on climate.(1, 2) Atmospheric particles consist of a complex mixture of organic compounds with a wide range of molecular structures, morphologies, physical properties, and chemical reactivity. The chemical composition, morphology, and phase state of atmospheric particles are of crucial importance for understanding the formation and reaction mechanisms of particles, their atmospheric evolution, and their impact on climate. It is of great interest to understand how the chemical and morphological particle microstructure affects their physicochemical properties such as chemical reactivity, thermodynamics of gas-particle partitioning, phase separations inside individual particles, hygroscopicity, optical properties, and ability to form liquid droplets (cloud condensation nuclei) and ice crystals (ice nuclei) in clouds. The phase state of organic particles, which yet remains poorly understood, plays a key role in their physicochemical properties and has important implications in various atmospheric processes. Fundamental understanding of these physicochemical properties and their possible evolution in time requires advanced analytical approaches for chemical imaging of particles with a resolution on the scale of 10-100 nm.(3) Comprehensive characterization of the size-dependent chemical composition of individual particles collected at the site was carried out using advanced molecular-level characterization and imaging approaches to identify their possible sources and to correlate to their climatic properties.

Southern Great Plains, aerosols, HI-SCALE field ca↗

NASA NTRSDate not supplied

Excessive Subsidence of the Southeast Atlantic Biomass Burning Aerosol Plume in the NASA Goddard Earth Observing System (GEOS) Model

Global models struggle to accurately represent the meteorological environment over the Southeast Atlantic Ocean, as evidenced by the poor representation of persistent marine stratocumulus decks off the west coast of southern Africa. This complex regime also experiences significant seasonal biomass burning aerosol plumes that are transported from southern Africa over the Atlantic Ocean, which gradually descend via large scale subsidence and interact radiatively and microphysically with the cloudy environment of the region. In comparisons to space borne lidar and aircraft observations we find that the NASA Goddard Earth Observing System (GEOS) model’s MERRA-2 aerosol and meteorology reanalysis shows that the aerosol plume descends too rapidly due to exaggerated large-scale downward vertical motion. This complicates the evaluation of aerosol properties utilizing aircraft observations collected throughout the ORACLES campaign as well as the model’s representation of the heating rate profiles due to the aerosol itself and its radiative interaction with the semi-permanent cloud deck typically located lower in altitude than the smoke. Two types of modeling experiments using GEOS will be presented to diagnose deficiencies in the model related to the excessive subsidence. Ensembles of free-running model simulations with and without radiatively active biomass burning aerosol will be used to quantify the impact of smoke on the atmospheric circulation. It will be demonstrated that heating within the aerosol layer results in self lofting through a reduction of the subsidence but did not alter the vertical placement or speed of the African Easterly jet. The amount of aerosol absorption required to eliminate the bias in the height of the aerosol plume through self-lofting will then be quantified. Finally, a second type of modeling experiment will be discussed in which the meteorology is constrained to observations. This will allow for biases in the height of the aerosol plume due to the general circulation model to be distinguished from biases that may be induced through the data assimilation process.

Allison Collow↗