Analysis of aerosol cloud interactions with a consistent signal of meteorology and other influencing parameters
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54 ENVIRONMENTAL SCIENCES↗
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Assessing effective radiative forcing from aerosol–cloud interactions over the global ocean
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54 ENVIRONMENTAL SCIENCES↗
Local Limits of Detection for Anthropogenic Aerosol-Cloud Interactions.
Abstract not provided.
Shand, Lyndsay↗
ARM Aerial Facility (AAF) Merged Value-Added Product Report for Historical G-1 Field Campaigns
For 30 years, the U.S. Department of Energy (DOE) Office of Science supported an instrumented Grumman Gulfstream-1 (G-1) aircraft for atmospheric field campaigns. Data from the final decade of G-1 operations were archived by the Atmospheric Radiation Measurement (ARM) user facility Data Center (ADC) and made publicly available at no cost to all registered users. To ensure a consistent data format and to improve the accessibility of the ARM airborne data, an integrated data set was recently developed covering the final six years of G-1 operations (2013 to 2018). The integrated data set includes data collected from 236 flights (766.4 hours). Four of the seven field campaigns were based in the U.S. One campaign collected data from the wildfires in the U.S. Pacific Northwest and agricultural burns in the lower Mississippi River valley as part of the Biomass Burning Observation Project (BBOP) in 2013. In 2015, the ARM Cloud Aerosol Precipitation Experiment provided data on atmospheric rivers and associated aerosol-cloud interactions that produce heavy precipitation on the U.S. west coast during the early spring. Research data from Airborne Carbon Measurements-V (ACME-V), collected during the summer of 2015, gave scientists insight into trends and variability of trace gases in the atmosphere over the North Slope of Alaska to improve arctic climate models. In the early summer and autumn of 2016, the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign provided an extensive data set geared toward coupled processes that affect the life cycle of shallow clouds through the interaction among aerosol, cloud, land surface, and ecosystems. In 2014 (March and October), the airborne sampling moved outside of the U.S. to the city of Manaus in central Amazonia, Brazil, where residential and industrial emissions were extensively characterized by flights of the G-1. The GoAmazon2014/15 aircraft campaign data are being integrated with aquatic and terrestrial ecosystem measurements to quantify anthropogenic perturbations to a usually pristine tropical environment. Another international airborne mission was carried out in the Eastern North Atlantic region. The Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign saw the G-1 aircraft fly from Terceira Island in the Azores during the summer of 2017 and the winter of 2018. The campaign studied both seasons to measure key aerosol and cloud processes under various meteorological and cloud conditions with different aerosol sources. Then the G-1 deployed to the Sierras de Córdoba range in central Argentina from October to November 2018 for the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) campaign to study orographic convective cloud interactions with their surrounding environment. These comprehensive datastreams provide much-needed insight into spatiotemporal variability of thermodynamic quantities, aerosol and cloud states, and properties for addressing essential science questions in Earth system process studies.
54 ENVIRONMENTAL SCIENCES↗
ARM Aerial Facility (AAF) Merged Value-Added Product Report for Historical G-1 Field Campaigns
For 30 years, the U.S. Department of Energy (DOE) Office of Science supported an instrumented Grumman Gulfstream-1 (G-1) aircraft for atmospheric field campaigns. Data from the final decade of G-1 operations were archived by the Atmospheric Radiation Measurement (ARM) user facility Data Center (ADC) and made publicly available at no cost to all registered users. To ensure a consistent data format and to improve the accessibility of the ARM airborne data, an integrated data set was recently developed covering the final six years of G-1 operations (2013 to 2018). The integrated data set includes data collected from 236 flights (766.4 hours). Four of the seven field campaigns were based in the U.S. One campaign collected data from the wildfires in the U.S. Pacific Northwest and agricultural burns in the lower Mississippi River valley as part of the Biomass Burning Observation Project (BBOP) in 2013. In 2015, the ARM Cloud Aerosol Precipitation Experiment provided data on atmospheric rivers and associated aerosol-cloud interactions that produce heavy precipitation on the U.S. west coast during the early spring. Research data from Airborne Carbon Measurements-V (ACME-V), collected during the summer of 2015, gave scientists insight into trends and variability of trace gases in the atmosphere over the North Slope of Alaska to improve arctic climate models. In the early summer and autumn of 2016, the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign provided an extensive data set geared toward coupled processes that affect the life cycle of shallow clouds through the interaction among aerosol, cloud, land surface, and ecosystems. In 2014 (March and October), the airborne sampling moved outside of the U.S. to the city of Manaus in central Amazonia, Brazil, where residential and industrial emissions were extensively characterized by flights of the G-1. The GoAmazon2014/15 aircraft campaign data are being integrated with aquatic and terrestrial ecosystem measurements to quantify anthropogenic perturbations to a usually pristine tropical environment. Another international airborne mission was carried out in the Eastern North Atlantic region. The Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign saw the G-1 aircraft fly from Terceira Island in the Azores during the summer of 2017 and the winter of 2018. The campaign studied both seasons to measure key aerosol and cloud processes under various meteorological and cloud conditions with different aerosol sources. Then the G-1 deployed to the Sierras de Córdoba range in central Argentina from October to November 2018 for the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) campaign to study orographic convective cloud interactions with their surrounding environment. These comprehensive datastreams provide much-needed insight into spatiotemporal variability of thermodynamic quantities, aerosol and cloud states, and properties for addressing essential science questions in Earth system process studies.
54 ENVIRONMENTAL SCIENCES↗
Aerosol characteristics at the Southern Great Plains site during the HI-SCALE campaign
Abstract. Large uncertainties exist in global climate model predictions of radiative forcing due to insufficient understanding and simplified numerical representation of cloud formation and cloud–aerosol interactions. The Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) campaign was conducted near the DOE's Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site in north-central Oklahoma to provide a better understanding of land–atmosphere interactions, aerosol and cloud properties, and the influence of aerosol and land–atmosphere interactions on cloud formation. The HI-SCALE campaign consisted of two intensive observational periods (IOPs) (April–May and August–September, 2016), during which coincident measurements were conducted both on the G-1 aircraft platform and at the SGP ground site. In this study we focus on the observations at the SGP ground site. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and an Ionicon proton-transfer-reaction mass spectrometer (PTR-MS) were deployed, characterizing chemistry of non-refractory aerosol and trace gases, respectively. Contributions from various aerosol sources, including biogenic and biomass burning emissions, were retrieved using factor analysis of the AMS data. In general, the organic aerosols at the SGP site was highly oxidized, with oxygenated organic aerosol (OOA) identified as the dominant factor for both the spring and summer IOP though more aged in spring. Cases of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX SOA) and biomass burning events were further investigated to understand additional sources of organic aerosol. Unlike other regions largely impacted by IEPOX chemistry, the IEPOX SOA at SGP was more highly oxygenated, likely due to the relatively weak local emissions of isoprene. Biogenic emissions appear to largely control the formation of organic aerosol (OA) during the HI-SCALE campaign. Potential HOM (highly oxygenated molecule) chemistry likely contributes to the highly oxygenated feature of aerosols at the SGP site, with impacts on new particle formation and global climate.
54 ENVIRONMENTAL SCIENCES↗
Aerosol-Radiation-Cloud Interactions in the South-East Atlantic: First Results from the ORACLES-2016 Deployment and Plans for Future Activities
Southern Africa produces almost a third of the Earths biomass burning (BB) aerosol particles. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical stratocumulus (Sc) cloud decks in the world. The SE Atlantic stratocumulus deck interacts with the dense layers of BB aerosols that initially overlay the cloud deck, but later subside and may mix into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects, and their global representation in climate models remains one of the largest uncertainties in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for regional and global climate change predictions.Our understanding of aerosol-cloud interactions in the SE Atlantic is severely limited. Most notably, we are missing knowledge on the absorptive and cloud nucleating properties of aerosols, including their vertical distribution relative to clouds, on the locations and degree of aerosol mixing into clouds, on the processes that govern cloud property adjustments, and on the importance of aerosol effects on clouds relative to co-varying synoptic scale meteorology.We describe first results from various synergistic, international research activities aimed at studying aerosol-cloud interactions in the region:NASAs airborne ORACLES (ObseRvations of Aerosols Above Clouds and Their IntEractionS) deployment in AugustSeptember of 2016,the DoEs LASIC (Layered Atlantic Smoke Interactions with Clouds) deployment of the ARM Mobile Facility to Ascension Island (June 2016 October 2017), the ground-based components of CNRS AEROCLO-sA (Aerosols Clouds and Fog over the west coast of southern Africa), and ongoing regional-scale integrative, process-oriented science efforts as part of SEALS-sA (Sea Earth Atmosphere Linkages Study in southern Africa).We expect to describe experimental setups as well as showcase initial aerosol and cloud property distributions. Furthermore, we discuss the implementation of future activities in these programs in coordination with the UK Met Offices CLARIFY (CLoud-Aerosol-Radiation Interactions and Forcing) experiment in 2017.
aerosol↗
Evaluating Clouds, Aerosols, and their Interactions in Three Global Climate Models using COSP and Satellite Observations
Accurately representing aerosol-cloud interactions in global climate models is challenging. As parameterizations evolve, it is important to evaluate their performance with appropriate use of observations. In this work we compare aerosols, clouds, and their interactions in three climate models (AM3, CAM5, ModelE) to MODIS satellite observations. Modeled cloud properties were diagnosed using the CFMIP Observations Simulator Package (COSP). Cloud droplet number concentrations (N) were derived using the same algorithm for both satellite-simulated model values and observations. We find that aerosol optical depth tau simulated by models is similar to observations. For N, AM3 and CAM5 capture the observed spatial pattern of higher values in near-coast versus remote ocean regions, though modeled values in general are higher than observed. In contrast, ModelE simulates lower N in most near-coast versus remote regions. Aerosol- cloud interactions were computed as the sensitivity of N to tau for marine liquid clouds off the coasts of South Africa and Eastern Asia where aerosol pollution varies in time. AM3 and CAM5 are in most cases more sensitive than observations, while the sensitivity for ModelE is statistically insignificant. This widely used sensitivity could be subject to misinterpretation due to the confounding influence of meteorology on both aerosols and clouds. A simple framework for assessing the N – tau sensitivity at constant meteorology illustrates that observed sensitivity can change from positive to statistically insignificant when including the confounding influence of relative humidity. Satellite simulated values of N were compared to standard model output and found to be higher with a bias of 83 cm-3.
aerosols↗
Advancements in the Representation of Cloud-Aerosol Microphysics in the GEOS-5 AGCM
Despite numerous challenges, the physical parameterization of cloud-aerosol interactions in atmospheric GCMs has become a top priority for advancement because of our need to simulate and understand past, current, and future indirect effects of aerosols on clouds. The challenges stem from the involvement of wide range of cloud-scale dynamics and aerosol activation physical processes. Cloud dynamics modulate cloud areal extent and condensate, while aerosol activation depends on aerosol mass load, size distribution, internal mixing state, and nucleating properties, and ultimately determines cloud optical properties via particle sizes. Both macro- and micro-scale processes are obviously important for cloud-radiation interactions. We will present the main features of cloud microphysical properties in the GEOS- 5 Atmospheric GCM (AGCM) as simulated by the McRAS-AC (Microphysics of Clouds with Relaxed Arakawa-Schubert and Aerosol-Cloud interaction) scheme. McRAS-AC uses Fountoukis and Nenes (2005) aerosol activation for liquid clouds, and has an option for either Liu and Penner (2005) or Barahona and Nenes (2008, 2009) aerosol activation for ice clouds. Aerosol loading (on-line or climatological) comes from GOCART, with an assumed log-normal size distribution. Other features of McRAS-AC are level-by-level cloud-scale thermodynamics, and Seifert-Beheng (2001)-type precipitation microphysics, particularly from moist convection. Results from Single-Column Model simulations will be shown to demonstrate how cloud radiative properties, lifetimes, and precipitation are influenced by different parameterization assumptions. Corresponding fields from year-long simulations of the full AGCM will also be presented with geographical distributions of cloud effective particle sizes compared to satellite retrievals. While the primary emphasis will be on current climate, simulation results with perturbed aerosol loadings will also be shown to expose the radiative sensitivity of the microphysical parameterization.
Lee, D.↗
Developing and testing capabilities for simulating cases with heterogeneous land/water surfaces in a novel atmospheric large eddy simulation code
Large eddy simulations (LES) are the primary computational tool used to simulate high Reynolds number three-dimensional turbulent flows. In the context of earth system sciences, particularly atmospheric science, LES are uniquely able to resolve the scales of atmospheric motion that are key for building process-level understanding of boundary layer turbulence, atmosphere-surface interaction, clouds, and cloud-aerosol-chemistry interaction, and are a core limited-area modeling capability. Increasing demands are being placed on LES code bases as growing high performance computing resources allow LES to address a wider range of scientific problems. In addition, LES are emerging as a source of high-quality machine learning training data. These demands necessitate an agile and extensible code base that allows the model to quickly adapt to emergent needs. However, LES have largely relied on legacy Fortran code bases that lack flexibility. A new, Python-based LES capability called Predicting INteractions of Aerosol and Clouds in Large Eddy Simulation (PINACLES) has been developed as part of the Department of Energy’s Earth System Model Development (ESMD) program area’s Enabling Aerosol-cloud interactions at Global convection-permitting scalES (EAGLES) project. PINACLES was developed from the ground up with a philosophy of maximizing scientific throughput, by attempting to optimize for both model throughput and software extensibility. The initial development of PINACLES delivered a state-of-the-art idealized LES capability solving the non-hydrostatic anelastic equations of motion with doubly periodic boundary conditions and idealized homogenous surface boundary conditions. Here we provide a final report on the outcomes of a fiscal year 2021 Seed Laboratory Directed Research Project that extended PINACLES in two key ways. First, PINACLES was coupled to a state-of-the-art land surface model enabling it to simulate spatially inhomogeneous land-atmosphere interactions that are known to control key atmospheric processes. Second, the dynamical core of PINACLES was modified to permit non-periodic boundary conditions. This model enhancement enables simulation of realistic cases with boundary conditions prescribed from atmospheric reanalysis and enables nested simulations conducted on a hierarchy of computational domains with increasing resolution. Together, these extensions to PINACLES make it a formidable modeling capability and expand its potential application to diverse components of DOE’s atmospheric science portfolio.
42 ENGINEERING↗
Cloud Processing of Aerosol during SAIL Field Campaign Report
Globally, on average, the release rate of aerosols from clouds is estimated to be about 6,000 Tg/yr and an aerosol particle is estimated to experience about three cloud cycles. Cloud processing of aerosol produces aerosols that have dramatically different physicochemical properties compared to their original form. Cloud processing may transform particles to efficient cloud condensation nuclei (CCN) or ice nucleating particles (INP) that can further participate in cloud formation. We investigated cloud processing of aerosol during the U.S. Department of Energy (DOE)’s Atmospheric Radiation Measurement (ARM) Surface Atmosphere Integrated Field Laboratory (SAIL) field campaign using multi-modal offline analysis techniques available at DOE’s Environmental Molecular Sciences Laboratory (EMSL). The main scientific aim of this project was to understand the processes that transform aerosols (chemically, and physically), and influence aerosol-cloud interactions. Aerosol particles undergo significant modifications due to warm (cloud droplets) and cold cloud (ice crystals) processing. Cloud processing of aerosol has important effects on the atmospheric aerosol number and mass concentration, size distribution, phase separation, and chemical composition.
54 ENVIRONMENTAL SCIENCES↗
Droplet Number Concentration Value Added Product
Cloud droplet number concentration is an important factor in understanding aerosol-cloud interactions. As aerosol concentration increases, it is expected that droplet number concentration (Nd) will increase and droplet size will decrease, for a given liquid water path. This will greatly affect cloud albedo as smaller droplets reflect more shortwave radiation; however, the magnitude and variability of these processes under different environmental conditions is still uncertain.McComiskey et al. (2009) have implemented a method, based onBoers and Mitchell (1994), for calculating Nd from ground-based remote sensing measurements of optical depth and liquid water path. They show that the magnitude of the aerosol-cloud interactions (ACI) varies with a range of factors, including the relative value of the cloud liquid water path (LWP), the aerosol size distribution, and the cloud updraft velocity. Estimates of Nd under a range of cloud types and conditions and at a variety of sites are needed to further quantify the impacts of aerosol cloud interactions. In order to provide data sets for studying aerosol-cloud interactions, the McComiskey et al. (2009) method was implemented as the Droplet Number Concentration (NDROP) value-added product (VAP).
Sivaraman, Chitra↗
Droplet Number Concentration Value Added Product
Cloud droplet number concentration is an important factor in understanding aerosol-cloud interactions. As aerosol concentration increases, it is expected that droplet number concentration (Nd) will increase and droplet size will decrease, for a given liquid water path. This will greatly affect cloud albedo as smaller droplets reflect more shortwave radiation; however, the magnitude and variability of these processes under different environmental conditions is still uncertain.McComiskey et al. (2009) have implemented a method, based onBoers and Mitchell (1994), for calculating Nd from ground-based remote sensing measurements of optical depth and liquid water path. They show that the magnitude of the aerosol-cloud interactions (ACI) varies with a range of factors, including the relative value of the cloud liquid water path (LWP), the aerosol size distribution, and the cloud updraft velocity. Estimates of Nd under a range of cloud types and conditions and at a variety of sites are needed to further quantify the impacts of aerosol cloud interactions. In order to provide data sets for studying aerosol-cloud interactions, the McComiskey et al. (2009) method was implemented as the Droplet Number Concentration (NDROP) value-added product (VAP).
Chitra Sivaraman, PNNL↗
Biomass-burning smoke's properties and its interactions with marine stratocumulus clouds in WRF-CAM5 and southeastern Atlantic field campaigns
Abstract. A large part of the uncertainty in climate projections comes from uncertain aerosol properties and aerosol–cloud interactions as well as the difficulty in remotely sensing them. The southeastern Atlantic functions as a natural laboratory to study biomass-burning smoke and to constrain this uncertainty. We address these gaps by comparing the Weather Research and Forecasting with Chemistry Community Atmosphere Model (WRF-CAM5) to the multi-campaign observations ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS), CLARIFY (CLoud–Aerosol–Radiation Interaction and Forcing), and LASIC (Layered Atlantic Smoke Interactions with Clouds) in the southeastern Atlantic in August 2017 to evaluate a large range of the model's aerosol chemical properties, size distributions, processes, and transport, as well as aerosol–cloud interactions. Overall, while WRF-CAM5 is able to represent smoke properties and transport, some key discrepancies highlight the need for further analysis. Observations of smoke composition show an overall decrease in aerosol mean diameter as smoke ages over 4–12 d, while the model lacks this trend. A decrease in the mass ratio of organic aerosol (OA) to black carbon (BC), OA:BC, and the OA mass to carbon monoxide (CO) mixing ratio, OA:CO, suggests that the model is missing processes that selectively remove OA from the particle phase, such as photolysis and heterogeneous aerosol chemistry. A large (factor of ∼2.5) enhancement in sulfate from the free troposphere (FT) to the boundary layer (BL) in observations is not present in the model, pointing to the importance of properly representing secondary sulfate aerosol formation from marine dimethyl sulfide and gaseous SO2 smoke emissions. The model shows a persistent overprediction of aerosols in the marine boundary layer (MBL), especially for clean conditions, which multiple pieces of evidence link to weaker aerosol removal in the modeled MBL than reality. This evidence includes several model features, such as not representing observed shifts towards smaller aerosol diameters, inaccurate concentration ratios of carbon monoxide and black carbon, underprediction of heavy rain events, and little evidence of persistent biases in modeled entrainment. The average below-cloud aerosol activation fraction (NCLD/NAER) remains relatively constant in WRF-CAM5 between field campaigns (∼0.65), while it decreases substantially in observations from ORACLES (∼0.78) to CLARIFY (∼0.5), which could be due to the model misrepresentation of clean aerosol conditions. WRF-CAM5 also overshoots an observed upper limit on liquid cloud droplet concentration around NCLD= 400–500 cm−3 and overpredicts the spread in NCLD. This could be related to the model often drastically overestimating the strength of boundary layer vertical turbulence by up to a factor of 10. We expect these results to motivate similar evaluations of other modeling systems and promote model development to reduce critical uncertainties in climate simulations.
54 ENVIRONMENTAL SCIENCES↗
Effect of Cloud Fraction on Near-Cloud Aerosol Behavior in the MODIS Atmospheric Correction Ocean Color Product
Characterizing the way satellite-based aerosol statistics change near clouds is important for better understanding both aerosol-cloud interactions and aerosol direct radiative forcing. This study focuses on the question of whether the observed near-cloud increases in aerosol optical thickness and particle size may be explained by a combination of two factors: (i) Near-cloud data coming from areas with higher cloud fractions than far-from-cloud data and (ii) Cloud fraction being correlated with aerosol optical thickness and particle size. This question is addressed through a statistical analysis of aerosol parameters included in the MODIS (MODerate resolution Imaging Spectroradiometer) ocean color product. Results from ten Septembers (2002-2011) over part of the northeast Atlantic Ocean confirm that the combination of these two factors working together explains a significant but not dominant part (in our case, 15%-30%) of mean optical thickness changes near clouds. Overall, the findings show that cloud fraction plays a large role in shaping the way aerosol statistics change with distance to clouds. This implies that both cloud fraction and distance to clouds are important to consider when aerosol-cloud interactions or aerosol direct radiative effects are examined in satellite or modeling studies.
Remote sensing↗
A Concept of a Convection–Cloud Chamber to Study Aerosol–Cloud–Drizzle Interactions
Understanding and quantifying the full chain of processes from aerosol activation to drizzle formation, and the associated feedbacks to the aerosol chemical and physical properties, all within a turbulent cloud are some of the toughest challenges in atmospheric chemistry and physics and are keys to the cloud–precipitation puzzle. This paper describes a concept for a new type of research facility consisting of a cloud chamber plus associated instrumentation and computational models, to explore aerosol–cloud interactions and processing, cloud optical properties, entrainment–cloud interactions, and quantitative assessment of drizzle onset. The envisioned design is for a 3 m × 3 m × 9 m chamber, such that the height is sufficient to achieve long lifetimes for aerosol processing and for significant drizzle growth by collision and coalescence. A suite of computational tools for simulating microphysical properties in the chamber provides a digital twin for designing the chamber and a range of example experiments. Theory and test results from novel remote sensing systems for exploring chemical and physical interactions and evolution of aerosols, cloud droplets, and drizzle within turbulent clouds are described. Testing of technology needed for the operation of a large-volume chamber, including aerosol generation methods and novel materials for water vapor boundary conditions, is described. Simulations suggest that spatially uniform turbulence and microphysical properties can be sustained in a steady state, with reasonable aerosol and water vapor fluxes, and that substantial drizzle can be produced through collision and coalescence of cloud droplets. Remaining challenges for more detailed engineering design and a discussion of possible first-light experiments are described.
54 ENVIRONMENTAL SCIENCES↗
Source attribution of Arctic black carbon and sulfate aerosols and associated Arctic surface warming during 1980–2018
Observations show that the concentrations of Arctic sulfate and black carbon (BC) aerosols have declined since the early 1980s. Previous studies have reported that reducing sulfate aerosols potentially contributed to the recent rapid Arctic warming. In this study, a global aerosol–climate model (Community Atmosphere Model, version 5) equipped with Explicit Aerosol Source Tagging (CAM5-EAST) is applied to quantify the source apportionment of aerosols in the Arctic from 16 source regions and the role of aerosol variations in affecting changes in the Arctic surface temperature from 1980 to 2018. The CAM5-EAST simulated surface concentrations of sulfate and BC in the Arctic had a decrease of 43% and 23%, respectively, in 2014–2018 relative to 1980–1984 mainly due to the reduction of emissions from Europe, Russia and local Arctic sources. Increases in emissions from South and East Asia led to positive trends in Arctic sulfate and BC in the upper troposphere. All aerosol radiative impacts are considered including aerosol–radiation and aerosol–cloud interactions, as well as black carbon deposition on snow- and ice-covered surfaces. Within the Arctic, sulfate reductions caused a top-of-atmosphere (TOA) warming of 0.11 and 0.25 W m -2 through aerosol–radiation and aerosol–cloud interactions, respectively. While the changes in Arctic atmospheric BC has little impact on local radiative forcing, the decrease in BC in snow and ice led to a net cooling of 0.05 W m -2 . By applying climate sensitivity factors for different latitudinal bands, global changes in sulfate and BC during 2014–2018 (with respect to 1980–1984) exerted a +0.088 and 0.057 K Arctic surface warming, respectively, through aerosol–radiation interactions. Through aerosol–cloud interactions, the sulfate reduction caused an Arctic warming of +0.193 K between the two time periods. The weakened BC effect on snow–ice albedo led to an Arctic surface cooling of -0.041 K. The changes in atmospheric sulfate and BC outside the Arctic produced a total Arctic warming of +0.25 K, the majority of which is due to the midlatitude changes in radiative forcing. Our results suggest that changes in aerosols over the midlatitudes of the Northern Hemisphere have a larger impact on Arctic temperature than other regions through enhanced poleward heat transport. The combined total effects of sulfate and BC produced an Arctic surface warming of +0.297 K, explaining approximately 20% of the observed Arctic warming since the early 1980s.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Reconciling Contrasting Relationships Between Relative Dispersion and Volume-Mean Radius of Cloud Droplet Size Distributions
Cloud droplet spectral relative dispersion is critical to parameterizations of cloud radiative properties, warm-rain initiation, and aerosol-cloud interactions in models; however, there is no consistent relationship between relative dispersion and volume-mean radius in literature, which hinders improving relative dispersion parameterization and calls for physical explanation. Here we show, by analyzing aircraft observations of cumulus clouds during Routine AAF [Atmospheric Radiation Measurement (ARM) Aerial Facility] Clouds with Low Optical Water Depths (CLOWD) Optical Radiative Observations, that the correlation between relative dispersion and volume-mean radius changes from positive to negative as volume-mean radius increases. With the new observation, we postulate that the sign of the correlation is determined by whether or not condensation (evaporation) occurs simultaneously with significant new activation (deactivation). The hypothesis is validated by simulations of both an adiabatic cloud parcel model and a parcel model accounting for entrainment-mixing. A new quantity, first bin strength, is introduced to quantify this new observation. Theoretical analysis of truncated gamma and modified gamma size distributions further supports the hypothesis and reconciles the contrasting relationships between relative dispersion and volume-mean radius, including the results in polluted fog observations. The results could shed new light on the so-called “twilight zone” between cloudy and cloud-free air, which in turn affects evaluation of aerosol-cloud interactions and retrieval of aerosol optical depth.
Lu, Chunsong↗