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At least 109 records · Page 6

Bridging New Observational Capabilities and Process-Level Simulation: Insights into Aerosol Roles in the Earth System

The spatial distribution of ambient aerosol particles significantly impacts aerosol–radiation–cloud interactions, which contribute to the largest uncertainty in global anthropogenic radiative forcing estimations. However, the atmospheric boundary layer and lower free troposphere have not been adequately sampled in terms of spatiotemporal resolution, hindering a comprehensive characterization of various atmospheric processes and impeding our understanding of the Earth system. To address this research data gap, we have leveraged the development of uncrewed aerial systems (UAS) and advanced measurement techniques to obtain mesoscale spatial data on aerosol microphysical and optical properties around the U.S. Southern Great Plains (SGP) atmospheric observatory. Our study also benefits from state-of-the-art laboratory facilities that include three-dimensional molecular imaging techniques enabled by secondary ion mass spectrometry and nanogram-level chemical composition analysis via micronebulization aerosol mass spectrometry. Through our study, we have developed a framework for observation–modeling integration, enabling an examination of how various assumptions about the organic–inorganic components mixing state, inferred from chemical analysis, affect clouds and radiation in observation-constrained model simulations. By integrating observational constraints (derived from offline chemical analysis of the aerosol surface using collected samples) with in situ UAS observations, we have identified a prominent role of organic-enriched nanometer layers located at the surface of aerosol particles in determining profiles of aerosol optical and hygroscopic properties over the SGP observatory. Furthermore, we have improved the agreement between predicted clouds and ground-based cloud lidar measurements. This UAS–model–laboratory integration exemplifies how these new advanced capabilities can significantly enhance our understanding of aerosol–radiation–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

Improving BC Mixing State and CCN Activity Representation With Machine Learning in the Community Atmosphere Model Version 6 (CAM6)

Abstract Representing mixing state of black carbon (BC) is challenging for global climate models (GCMs). The Community Atmosphere Model version 6 (CAM6) with the four‐mode version of the Modal Aerosol Module (MAM4) represents aerosols as fully internal mixtures with uniform composition within each aerosol mode, resulting in high degree of internal mixing of BC with non‐BC species and large mass ratio of coating to BC ( R BC , the mass ratio of non‐BC species to BC in BC‐containing particles). To improve BC mixing state representation, we coupled a machine learning (ML) model of BC mixing state index trained on particle‐resolved simulations to the CAM6 with MAM4 (MAM4‐ML). In MAM4‐ML, we use R BC to partition accumulation mode particles into two new modes, BC‐free particles and BC‐containing particles. We adjust R BC to make the modeled BC mixing state index ( χ mode ) match the one predicted by the ML model ( χ ML ). On a global average, the mass fraction of BC‐containing particles in accumulation mode decreases from 100% (MAM4‐default) to 48% (MAM4‐ML). The globally averaged χ mode decreases from 78% (MAM4‐default) to 63% (MAM4‐ML, 19% reduction) and agrees well with χ ML (66%). The R BC decreases by 52% for accumulation mode and better agrees with observations. The hygroscopicity drops by 9% for BC‐containing particles in accumulation mode, leading to a 20% reduction in the BC activation fraction. The surface BC concentration increases most (6.9%) in the Arctic, and the BC burden increases by 4%, globally. Our study highlights the application of the ML model for improving key aerosol processes in GCMs.

Meteorology & Atmospheric Sciences↗

Microphysics of liquid water in sub-10 nm ultrafine aerosol particles

Abstract. Ultrafine aerosol particles with sizes smaller than 50 nm have been shown in recent studies to serve as a large source of cloud condensation nuclei that can promote additional cloud droplet formation under supersaturation conditions. Knowledge of the microphysics of liquid water in these droplets remains limited, particularly in the sub-10 nm particle size range, due to experimental and theoretical challenges associated with the complexity of aerosol components and the small length scales of interest (e.g., difficulty of precisely sampling the liquid–air interface, questionable validity of mean-field theoretical representations). Here, we carried out molecular dynamics (MD) simulations of aerosol particles with diameters between 1 and 10 nm and characterized atomistic-level structure and water dynamics in well-mixed and phase-separated systems with different particle sizes, NaCl salinities, and pimelic acid (PML) organic surface loadings as a function of distance from the time-averaged Gibbs dividing interface or instantaneous water–air interface. We define a sphericity factor (ϕ) that can shed light on the phase-mixing state of nanodroplets, and we reveal an unexpected dependence of mixing state on droplet size. Our results also evidence an ion concentration enhancement in ultrafine aerosols, which should modulate salt nucleation kinetics in sub-10 nm droplets, and provide detailed characterization of the influence of droplet size on surface tension and on water self-diffusivity near the interface. Analysis of water evaporation free energy and water activity demonstrates the validity of the Kelvin equation and Köhler theory at droplet sizes larger than 4 nm under moderate salinities and organic loadings and the need for further extension to account for ion concentration enhancement in sub-10 nm aerosols, droplet-size-dependent phase separation effects, and a sharp decrease in the cohesiveness of liquid water in sub-4 nm droplets. Finally, we show that an idealized fractional surface coating factor (fs) can be used to categorize and reconcile water accommodation coefficients (α*) observed in MD simulations and experimental results in the presence of organic coatings, and we resolve the droplet size dependence of α*.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Cloud condensation nuclei characteristics at the Southern Great Plains site: role of particle size distribution and aerosol hygroscopicity

The activation ability of aerosols as cloud condensation nuclei (CCN) is crucial in climate and hydrological cycle studies, but their properties are not well known. We investigated the long-term measurements of atmospheric aerosol properties, CCN concentrations (N CCN ) at supersaturation (SS = 0.1%–1.0%), and hygroscopicity at the Department of Energy's Southern Great Plains (SGP) site to illustrate the dependence of N CCN on aerosol properties and transport pathways. Cluster analysis was applied to the back trajectories of air masses to investigate their respective source regions. The results showed that aged biomass burning aerosols from Central America were characterized by higher accumulation mode particles (N accu ; median value 805 cm -3 ) and relatively high aerosol hygroscopicity (κ; median value ~0.25) values that result in the higher CCN activation and relatively high N CCN (median value 258–1578 cm -3 at a SS of 0.1%–1.0%). Aerosols from the Gulf of Mexico were characterized by higher N accu (~35%), and N CCN (230–1721 cm -3 at a SS of 0.1%–1.0%) with the lowest κ (~0.17). In contrast, relatively high nucleation mode particles (N nucl ; ~20%) and low N CCN (128–1553 cm -3 at a SS of 0.1%–1.0%) with higher κ (~0.30) values were observed on the aerosols associated with a westerly wind. The results indicate particle size as the most critical factor influencing the ability of aerosols to activate, whereas the effect of chemical composition was secondary. Our CCN closure analysis suggests that chemical composition and mixing state information are more crucial at lower SS, whereas at higher SS, most particles become activated regardless of their chemical composition and size. This study affirms that soluble organic fraction information is required at higher SS for better N CCN prediction, but both the soluble organics fraction and mixing state are vital to reduce the N CCN prediction uncertainty at lower SS.

54 ENVIRONMENTAL SCIENCES↗

Predicting secondary organic aerosol phase state and viscosity and its effect on multiphase chemistry in a regional-scale air quality model

Atmospheric aerosols are a significant public health hazard and have substantial impacts on the climate. Secondary organic aerosols (SOAs) have been shown to phase separate into a highly viscous organic outer layer surrounding an aqueous core. This phase separation can decrease the partitioning of semi-volatile and low-volatile species to the organic phase and alter the extent of acid-catalyzed reactions in the aqueous core. A new algorithm that can determine SOA phase separation based on their glass transition temperature (T g ), oxygen to carbon (O:C) ratio and organic mass to sulfate ratio, and meteorological conditions was implemented into the Community Multiscale Air Quality Modeling (CMAQ) system version 5.2.1 and was used to simulate the conditions in the continental United States for the summer of 2013. SOA formed at the ground/surface level was predicted to be phase separated with core–shell morphology, i.e., aqueous inorganic core surrounded by organic coating 65.4 % of the time during the 2013 Southern Oxidant and Aerosol Study (SOAS) on average in the isoprene-rich southeastern United States. Our estimate is in proximity to the previously reported ~70 % in literature. The phase states of organic coatings switched between semi-solid and liquid states, depending on the environmental conditions. The semi-solid shell occurring with lower aerosol liquid water content (western United States and at higher altitudes) has a viscosity that was predicted to be 10 2 –10 12 Pa s, which resulted in organic mass being decreased due to diffusion limitation. Organic aerosol was primarily liquid where aerosol liquid water was dominant (eastern United States and at the surface), with a viscosity <10 2 Pa s. Phase separation while in a liquid phase state, i.e., liquid–liquid phase separation (LLPS), also reduces reactive uptake rates relative to homogeneous internally mixed liquid morphology but was lower than aerosols with a thick viscous organic shell. The sensitivity cases performed with different phase-separation parameterization and dissolution rate of isoprene epoxydiol (IEPOX) into the particle phase in CMAQ can have varying impact on fine particulate matter (PM 2.5 ) organic mass, in terms of bias and error compared to field data collected during the 2013 SOAS. This highlights the need to better constrain the parameters that govern phase state and morphology of SOA, as well as expand mechanistic representation of multiphase chemistry for non-IEPOX SOA formation in models aided by novel experimental insights.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Haze processing of atmospheric particles during wintertime in the Indo-Gangetic Plains

The impacts of haze on visibility, air quality, and climate are not well quantified due to a lack of understanding of the evolution of the mixing state and phase state of atmospheric particles during haze processing. The variability of the mixing state of atmospheric particles contributes significantly to uncertainties associated with the estimated aerosol radiative forcing. We collected particle samples in January 2018 from the highly polluted Indo-Gangetic plain during hazy conditions to study haze-processed particles. Single particle analysis using multi-modal micro-spectroscopy techniques revealed an abundance (40–70% by number) of potassium-rich sulfate particles from biomass-burning influenced smoke. Tilted view imaging showed that most of the organic particles that had inorganic potassium and sulfate inclusions were liquid-like while those without inclusions were more semi-solid. High-resolution mass spectrometry analysis revealed a significant presence of organosulfates and nitroxy-organosulfates in the morning samples (24%) compared to the afternoon samples (9%), despite higher relative humidity in the afternoon. Overall, our results highlight the significant contribution of both organic and inorganic sulfate to the total particulate sulfur budget during haze processing in winter, when anthropogenic emissions such as household burning, agricultural burning, and vehicular emissions are major contributors to particle mass.

Mathai, Susan [Pacific Northwest National Laborato↗

Aerosol-induced closure of marine cloud cells: enhanced effects in the presence of precipitation

Abstract. The Weather Research Forecasting (WRF) version 4.3 model is configured within a Lagrangian framework to quantify the impact of aerosols on evolving cloud fields. Kilometer-scale simulations utilizing meteorological boundary conditions are based on 10 case study days offering diverse meteorology during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA). Measurements from aircraft, the ground-based Atmosphere Radiation Measurement (ARM) site at Graciosa Island in the Azores, and A-Train and geostationary satellites are utilized for validation, demonstrating good agreement with the WRF-simulated cloud and aerosol properties. Higher aerosol concentration leads to suppressed drizzle and increased cloud water content in all case study days. These changes lead to larger radiative cooling rates at cloud top, enhanced vertical velocity variance, and increased vertical and horizontal wind speed near the base of the lower-tropospheric inversion. As a result, marine cloud cell area expands, narrowing the gap between shallow clouds and increasing cloud optical thickness, liquid water content, and the top-of-atmosphere outgoing shortwave flux. While similar aerosol effects are observed in lightly to non-raining clouds, they tend to be smaller by comparison. These simulations show a relationship between cloud cell area expansion and the radiative adjustments caused by liquid water path and cloud fraction changes. The adjustments are positive and scale as 74 % and 51 %, respectively, relative to the Twomey effect. While higher-resolution large-eddy simulations may provide improved representation of cloud-top mixing processes, these results emphasize the importance of addressing mesoscale cloud-state transitions in the quantification of aerosol radiative forcing that cannot be attained from traditional climate models.

54 ENVIRONMENTAL SCIENCES↗

North Slope of Alaska Black Carbon Loadings and Mixing State for MOSAiC Field Campaign Report

The Arctic represents a unique region to study global climate change in that it exhibits pronounced sensitivity towards aerosol radiative forcing, referred to as arctic amplification. Of the aerosol species that are expected to contribute to this aerosol forcing, black carbon (BC) is arguably at the top of the list. Black carbon has this distinction because it exerts two radiative forcing influences that can be characterized as atmospheric and non-atmospheric. As an atmospheric forcer, BC behaves much as it does in the mid-latitudes – through the direct effect and semi-direct effects – collectively causing surface dimming with subsequent surface cooling and mid-altitude warming affecting cloud cover. As a terrestrial forcer, which is unique to the cryosphere, the deposition of BC on the surface can readily decrease polar surface albedo that, in turn, can activate a positive feedback wherein the increased surface absorption leads to further snow melt causing still further reduction in surface albedo.

54 ENVIRONMENTAL SCIENCES↗

Linking Remotely Sensed Aerosol Types to Their Chemical Composition

Aerosol types measured during the Ship-Aircraft Bio-Optical Research (SABOR) experiment are related to GEOS-Chem model chemical composition. The application for this procedure to link model chemical components to aerosol type is desirable for understanding aerosol evolution over time. The Mahalanobis distance (DM) statistic is used to cluster model groupings of five chemical components (organic carbon, black carbon, sea salt, dust and sulfate) in a way analogous to the methods used by Burton et al. [2012] and Russell et al. [2014]. First, model-to-measurement evaluation is performed by collocating vertically resolved aerosol extinction from SABOR High Spectral Resolution LiDAR (HSRL) to the GEOS-Chem nested high-resolution data. Comparisons of modeled-to-measured aerosol extinction are shown to be within 35% +/- 14%. Second, the model chemical components are calculation into five variables to calculate the DM and cluster means and covariances for each HSRL-retrieved aerosol type. The layer variables from the model are aerosol optical depth (AOD) ratios of (i) sea salt and (ii) dust to total AOD, mass ratios of (iii) total carbon (i.e. sum of organic and black carbon) to the sum of total carbon and sulfate (iv) organic carbon to black carbon, and (v) the natural log of the aerosol-to-molecular extinction ratio. Third, the layer variables and at most five out of twenty SABOR flights are used to form the pre-specified clusters for calculating DM and to assign an aerosol type. After determining the pre-specified clusters, model aerosol types are produced for the entire vertically resolved GEOS-Chem nested domain over the United States and the model chemical component distributions relating to each type are recorded. Resulting aerosol types are Dust/Dusty Mix, Maritime, Smoke, Urban and Fresh Smoke (separated into 'dark' and 'light' by a threshold of the organic to black carbon ratio). Model-calculated DM not belonging to a specific type (i.e. not meeting a threshold probability) is termed an outlier and those DM values that can belong to multiple types (i.e. showing weak probability of belonging to a specific cluster) are termed as Overlap. MODIS active fires are overlaid on the model domain to qualitatively evaluate the model-predicted Smoke aerosol types.

Aerosol Types↗

Coupling of Dust Mineralogy to Radiation in NASA GISS ModelE: Impact Upon Dust Optical Properties and Direct Radiative Effect

Estimates of dust direct radiative effect (DRE) are still largely uncertain mainly due to the poor constraining of regional variations of dust absorption, whose known connection with mineral composition is still largely neglected by most Earth System Models. The inaccurate knowledge of soil mineralogy and insufficient measurements of dust physical and optical properties still present the main challenges for a proper representation of the dust-radiation interaction in climate models. We recently upgraded the coupling of dust minerals to shortwave radiation in the NASA GISS ModelE. In particular, we extended the interaction to online-calculated minerals and implemented two different mixing configurations: i) external mixing of three main mineral components and ii) internal mixing of all minerals, allowing a dynamic fraction of iron oxides. We used a semi-empirical approach for the optical calculations, mostly based on aerosol chamber measurements from natural soils, aiming to reduce the influence of uncertain assumptions on the optical properties and mixing state of individual minerals. In this contribution, we present the results of our first calculations of dust optical properties and DREs based on different mixing configurations of interactive minerals. We show the changes to dust optical depth and single scattering albedo, with respect to the control case using homogeneous dust composition, and the consequent global and regional variations in dust DREs at the top of atmosphere and at surface. We also compare the model optical properties with AERONET data, filtered to identify dust scenes. We find that accounting for the diverse properties of dust minerals modifies the pattern of regional dust absorption and therefore its impact upon climate. We also show that the mineralogy effect is sensitive to the assumed mixing state of minerals.

dust direct radiative effect↗

Ground-Based High Spectral Resolution Lidar Observation of Aerosol Vertical Distribution in the Summertime Southeast United States

As part of the Southeast United States-based Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS), and collinear with part of the Southeast Atmosphere Study, the University of Wisconsin High Spectral Resolution Lidar system was deployed to the University of Alabama from 19 June to 4 November 2013. With a collocated Aerosol Robotic Network (AERONET) sun photometer, a nearby Chemical Speciation Network (PM2.5) measurement station, and near daily ozonesonde releases for the August-September SEAC4RS campaign, the site allowed the regions first comprehensive diurnal monitoring of aerosol particle vertical structure. A 532nm lidar ratio of 55 sr provided good closure between aerosol backscatter and AERONET (aerosol optical thickness, AOT). A principle component analysis was performed to identify key modes of variability in aerosol backscatter. ''Fair weather'' days exhibited classic planetary boundary layer structure of a mixed layer accounting for approx. 50% of AOT and an entrainment zone providing another 25%. An additional 5-15% of variance is gained from the lower free troposphere from either convective detrainment or frequent intrusions of western United States biomass burning smoke. Generally, aerosol particles were contained below the 0 C level, a common level of stability in convective regimes. However, occasional strong injections of smoke to the upper troposphere were also observed, accounting for the remaining 10-15% variability in AOT. Examples of these common modes of variability in frontal and convective regimes are presented, demonstrating why AOT often has only a weak relationship to surface PM2.5 concentration.

HSRL↗

RACORO Continental Boundary Layer Cloud Investigations: 1. Case Study Development and Ensemble Large-Scale Forcings

Observation-based modeling case studies of continental boundary layer clouds have been developed to study cloudy boundary layers, aerosol influences upon them, and their representation in cloud- and global-scale models. Three 60 h case study periods span the temporal evolution of cumulus, stratiform, and drizzling boundary layer cloud systems, representing mixed and transitional states rather than idealized or canonical cases. Based on in situ measurements from the Routine AAF (Atmospheric Radiation Measurement (ARM) Aerial Facility) CLOWD (Clouds with Low Optical Water Depth) Optical Radiative Observations (RACORO) field campaign and remote sensing observations, the cases are designed with a modular configuration to simplify use in large-eddy simulations (LES) and single-column models. Aircraft measurements of aerosol number size distribution are fit to lognormal functions for concise representation in models. Values of the aerosol hygroscopicity parameter, kappa, are derived from observations to be approximately 0.10, which are lower than the 0.3 typical over continents and suggestive of a large aerosol organic fraction. Ensemble large-scale forcing data sets are derived from the ARM variational analysis, European Centre for Medium-Range Weather Forecasts, and a multiscale data assimilation system. The forcings are assessed through comparison of measured bulk atmospheric and cloud properties to those computed in "trial" large-eddy simulations, where more efficient run times are enabled through modest reductions in grid resolution and domain size compared to the full-sized LES grid. Simulations capture many of the general features observed, but the state-of-the-art forcings were limited at representing details of cloud onset, and tight gradients and high-resolution transients of importance. Methods for improving the initial conditions and forcings are discussed. The cases developed are available to the general modeling community for studying continental boundary clouds.

Boundary layers↗

Cloud microphysical response to entrainment and mixing is locally inhomogeneous and globally homogeneous: Evidence from the lab

Entrainment of dry air into clouds strongly influences cloud optical and precipitation properties and the response of clouds to aerosol perturbations. The response of cloud droplet size distributions to entrainment–mixing is examined in the Pi convection-cloud chamber that creates a turbulent, steady-state cloud. The experiments are conducted by injecting dry air with temperature (T e ) and flow rate (Q e ) through a flange in the top boundary, into the otherwise well-mixed cloud, to mimic the entrainment–mixing process. Due to the large-scale circulation, the downwind region is directly affected by entrained dry air, whereas the upwind region is representative of the background conditions. Droplet concentration (Cn) and liquid water content (L) decrease in the downwind region, but the difference in the mean diameter of droplets (D m ) is small. The shape of cloud droplet size distributions relative to the injection point is unchanged, to within statistical uncertainty, resulting in a signature of inhomogeneous mixing, as expected for droplet evaporation times small compared to mixing time scales. As T e and Q e of entrained air increase, however, Cn, L, and D m of the whole cloud system decrease, resulting in a signature of homogeneous mixing. The apparent contradiction is understood as the cloud microphysical responses to entrainment and mixing differing on local and global scales: locally inhomogeneous and globally homogeneous. This implies that global versus local sampling of clouds can lead to seemingly contradictory results for mixing, which informs the long-standing debate about the microphysical response to entrainment and the parameterization of this process for coarse-resolution models.

54 ENVIRONMENTAL SCIENCES↗

Impact of Nonabsorbing Anthropogenic Aerosols on Clear-Sky Atmospheric Absorption

Absorption of solar radiation by atmospheric aerosol has become recognized as important in regional and global climate. Nonabsorbing, hydrophilic aerosols, such as sulfate, potentially affect atmospheric absorption in opposing ways: first, decreasing absorption through aging initially hydrophobic black carbon (BC) to a hydrophilic state, enhancing its removal by wet scavenging, and consequently decreasing BC lifetime and abundance, and second, increasing absorption through enhancement of the BC absorption efficiency by internal mixing as well as through increasing the amount of diffuse solar radiation in the atmosphere. On the basis of General Circulation Model studies with an embedded microphysical aerosol module we systematically demonstrate the significance of these mechanisms both on the global and regional scales. In remote transport regions, the first mechanism prevails, reducing atmospheric absorption, whereas in the vicinity of source regions, despite enhanced wet scavenging, absorption is enhanced owing to the prevalence of the second mechanisms. Our findings imply that the sulfur to BC emission ratio plays a key role in aerosol absorption.

Stier, Philip↗

Studies on propagation of microbes in the airborne state

An investigation was conducted to demonstrate whether airborne microbes could propagate. The procedure consisted of: (1) looking for dilution of a labelled base in DNA; (2) looking for labelling of DNA by mixing aerosols of the label and the cells; (3) examining changes in cell size; (4) testing the possibility of spore germination; and (5) seeking evidence of an increase in cell number. Results indicate that growth and propagation can occur under special conditions, principally at temperatures of approximately 30 C (87 F) and water activity equivalents of 0.95 to 0.98.

Dimmick, R. L.↗

Application of aerosol-ice nucleating particle closure to establish the leading parameters governing ice crystal number concentration under commonly observed mixed-phase cloud conditions

This is the final technical report for DOE DE-SC0021034 award entitled “Application of aerosol-ice nucleating particle closure to establish the leading parameters governing ice crystal number concentration under commonly observed mixed-phase cloud conditions”. The overarching objective of this project was to gain a predictive understanding of the processes that lead from aerosols to ice-nucleating particles (INPs) to ice crystal number concentrations (ICNCs) in stratiform mixed-phase clouds where supercooled water droplets and ice crystals coexist, and to inform climate model parameterizations. During this four-year project we addressed the three main research goals of this objective: 1) Study the aerosol-INP link; 2) Develop an aerosol-cloud column model (AC-1D); and 3) Study the INP-ICNC link. Those activities significantly advanced our predictive understanding of how to represent INPs in could models and its implications on ice crystal number concentrations. The results have been published in five peer-reviewed publications with three more in review and preparation. It allowed for collaboration resulting in additional fourteen peer-reviewed publications that are concerned with the objective of this research project. This research has been communicated to the scientific community at national and international meetings and conferences by numerous talks, seminars, and posters including fifteen invited presentations. This project allowed training of four graduate students and one postdoctoral research associate resulting in one M.S. thesis and advancement to Ph.D. candidacy.

54 ENVIRONMENTAL SCIENCES↗

The Dual Nature of Entrainment-Mixing Signatures Revealed through Large-Eddy Simulations of a Convection-Cloud Chamber

Abstract Entrainment of subsaturated air into a cloud can influence its optical and microphysical properties in various ways, depending on the droplet evaporation and turbulent mixing time scales. Previous experiments in the Pi convection-cloud chamber have revealed that, given a fixed entrained air property, the mixing of entrained subsaturated air results in complete evaporation of some cloud droplets, with the rest remaining unchanged. This is a signature of inhomogeneous mixing. While comparing the results of entrainment with varying air properties, the mixing signature appears as if the subsaturated air is well mixed with the cloud to evenly reduce the droplets’ size. In other words, taken together, the experiments appear to have the signature of homogeneous mixing. To explore these results in a greater depth, we conduct large-eddy simulations combined with a bin microphysics scheme. Our results reproduce the similar signatures of inhomogeneous and homogeneous mixing, implying that LES can resolve the inhomogeneous mixing when the grid spacing is smaller than the entrained air parcel. Additionally, we observe that increasing the aerosol injection rate enhances the signature of inhomogeneous mixing, while coarser grid spacing diminishes it. Finally, the change in wall fluxes in response to various entrained air properties confirms that the homogeneous signature seen in the analysis of an ensemble of simulations is the result of various equilibrium states. This further strengthens the suggestion that the homogeneous mixing signature found in aircraft observations near the cloud top may result from combining entrainment events of different intensities, possibly caused by various-sized eddies. Significance Statement Large-eddy simulation and size-resolved microphysics can resolve time scales for turbulent mixing and evaporation and, therefore, are well suited for reproducing, extending, and interpreting the entrainment experiment in the Pi convection-cloud chamber. Our simulation results confirm (i) the inhomogeneous mixing signature for an individual entrainment event and (ii) the appearance of homogeneous mixing in an ensemble of entrainment episodes. Furthermore, we demonstrate that the inhomogeneous mixing signature is more pronounced in a polluted cloud, but coarser grid spacing in simulations may compromise the accuracy of this signature. Last, the homogeneous mixing signature results from various equilibrium states established for different entrainment intensities and adjusted wall fluxes, which are challenging to measure experimentally but can be easily analyzed in the simulations.

54 ENVIRONMENTAL SCIENCES↗

Tethered Balloon Systems

Among ARM’s aerial platforms are tethered balloon systems (TBS), which consist of a helium-filled balloon, tether, winch, and sensors. TBS provide a safe way to collect data inside clouds, including mixed-phase clouds, where icing is a concern for airborne platforms. These systems are also flown above and below clouds to gather data related to wind, turbulence, thermodynamic state, aerosols, and the cloud-top environment.

54 ENVIRONMENTAL SCIENCES↗