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At least 1,027 records · Page 57

The Impact of Nonzenith Elevation Angles on Ground-Based Infrared Thermodynamic Retrievals

Observing thermodynamic profiles within the planetary boundary layer is essential to understanding and predicting atmospheric phenomena because of the significant exchange of sensible and latent heat between the land and atmosphere within that layer. The Atmospheric Emitted Radiance Interferometer (AERI) is a ground-based infrared spectrometer used to obtain the vertical profiles of temperature and water vapor mixing ratio. Most AERIs are only capable of zenith views, although the Marine AERI (M-AERI) has a design that allows it to view various elevation angles. In this study, we quantify the improvement in the information content and accuracy of the retrieved profiles when nonzenith angles are included, as is common with microwave radiometer profilers. The impacts of the additional scan angles are quantified through both a synthetic study and with M-AERI observations from the ARM Cloud Aerosol Precipitation Experiment (ACAPEX) campaign. Furthermore, the simulation study shows that low elevation angles contain more information content for temperature whereas high elevation angles have more information content for water vapor. Outside of very humid environments, the addition of low elevation angles also results in lower root-mean-square errors when compared with high angles for both temperature and water vapor mixing ratio, although this is primarily a result of averaging multiple observations together to reduce instrument noise. Real-world results from the ACAPEX dataset indicate similar results as were found for the simulation study, although not all predicted benefits are realized because of the small sample size and observational uncertainties.

54 ENVIRONMENTAL SCIENCES↗

Heavy and wet: The consequences of violating assumptions of measuring soil microbial growth efficiency using the 18O water method

Soils store more carbon than the biosphere and atmosphere combined, and the efficiency to which soil microorganisms allocate carbon to growth rather than respiration is increasingly considered a proxy for the soil capacity to store carbon. This carbon use efficiency (CUE) is measured via different methods, and more recently, the 18O-H2O method has been embraced as a significant improvement for measuring CUE of soil microbial communities. Based on extrapolating 18O incorporation into DNA to new biomass, this measurement makes various implicit assumptions about the microbial community at hand. Here we conducted a literature review to evaluate how viable these assumptions are and then developed a mathematical model to test how violating them affects estimates of the growth component of CUE in soil. We applied this model to previously collected data from two kinds of soil microbial communities. By changing one parameter at a time, we confirmed our previous observation that CUE was reduced by fungal removal. Our results also show that depending on the microbial community composition, there can be substantial discrepancies between estimated and true microbial growth. Of the numerous implicit assumptions that might be violated, not accounting for the contribution of sources of oxygen other than extracellular water to DNA leads to a consistent underestimation of CUE. We present a framework that allows researchers to evaluate how their experimental conditions may influence their 18O-H2O-based CUE measurements and suggest the parameters that need further constraining to more accurately quantify growth and CUE.

Environmental Sciences & Ecology↗

Microbial community response to a decade of simulated global changes depends on the plant community

Global changes such as increased drought and atmospheric nitrogen deposition perturb both the microbial and plant communities that mediate terrestrial ecosystem functioning. However, few studies consider how microbial responses to global changes may be influenced by interactions with plant communities. To begin to address the role of microbial–plant interactions, we tested the hypothesis that the response of microbial communities to global change depends on the plant community. We characterized bacterial and fungal communities from 395 plant litter samples taken from the Loma Ridge Global Change Experiment, a decade-long global change experiment in Southern California that manipulates rainfall and nitrogen levels across two adjacent ecosystems, a grassland and a coastal sage scrubland. The differences in bacterial and fungal composition between ecosystems paralleled distinctions in plant community composition. In addition to the direct main effects, the global change treatments altered microbial composition in an ecosystem-dependent manner, in support of our hypothesis. The interaction between the drought treatment and ecosystem explained nearly 5% of the variation in bacterial community composition, similar to the variation explained by the ecosystem-independent effects of drought. Unexpectedly, we found that the main effect of drought was approximately four times as strong on bacterial composition as that of nitrogen addition, which did not alter fungal or plant composition. Overall, the findings underscore the importance of considering plant–microbe interactions when considering the transferability of the results of global change experiments across ecosystems.

54 ENVIRONMENTAL SCIENCES↗

Investigating permafrost carbon dynamics in Alaska with artificial intelligence

Abstract Positive feedbacks between permafrost degradation and the release of soil carbon into the atmosphere impact land–atmosphere interactions, disrupt the global carbon cycle, and accelerate climate change. The widespread distribution of thawing permafrost is causing a cascade of geophysical and biochemical disturbances with global impacts. Currently, few earth system models account for permafrost carbon feedback (PCF) mechanisms. This research study integrates artificial intelligence (AI) tools and information derived from field-scale surveys across the tundra and boreal landscapes in Alaska. We identify and interpret the permafrost carbon cycling links and feedback sensitivities with GeoCryoAI, a hybridized multimodal deep learning (DL) architecture of stacked convolutionally layered, memory-encoded recurrent neural networks (NN). This framework integratesin-situmeasurements and flux tower observations for teacher forcing and model training. Preliminary experiments to quantify, validate, and forecast permafrost degradation and carbon efflux across Alaska demonstrate the fidelity of this data-driven architecture. More specifically, GeoCryoAI logs the ecological memory and effectively learns covariate dynamics while demonstrating an aptitude to simulate and forecast PCF dynamics—active layer thickness (ALT), carbon dioxide flux (CO 2 ), and methane flux (CH 4 )—with high precision and minimal loss (i.e. ALT RMSE : 1.327 cm [1969–2022]; CO 2 RMSE : 0.697µmolCO 2 m −2 s −1 [2003–2021]; CH 4 RMSE : 0.715 nmolCH 4 m −2 s −1 [2011–2022]). ALT variability is a sensitive harbinger of change, a unique signal characterizing the PCF, and our model is the first characterization of these dynamics across space and time.

Environmental Sciences & Ecology↗

Mitigation of ventilation air methane (VAM) using novel methanotrophic coating materials: a technical analysis

Abstract Ventilation air methane (VAM) is a potent greenhouse gas source originating from geological wells, current and extinct mineshafts and other terrestrial conduits venting methane to the atmosphere, contributing to global methane emissions and disproportionate warming potential. Herein, we introduce the concept of the methanotrophic material as an engineering solution. Such materials should be capable of converting methane at ambient temperatures and pressures to a binder product, capturing and permanently sequestering the methane while simultaneously restricting its further emission. While such materials are currently under research development, this goal is supported and facilities by the mathematical framework, introduced and used herein, to evaluate the ability to convert methane, using currently published activity data. We include a case study of the conversion of a characteristic stream of VAM (0.6% methane in air, 1.7 × 10 8 l hr −1 equivalent to 100 000 standard cubic feet per minute). We show that when appropriately designed, such systems require a surface coverage of less than 1000 m of mine tunnel length (equivalent to 20 000 m 2 areal coverage) in order to reduce the methane emission from this stream by over 99%. Finally, we highlight formaldehyde as a reactive intermediate of methane oxidation which may itself be incorporated into these coating materials. As a component of binders and polymers already used ubiquitously in commercial products, this intermediate ultimately allows these systems to sequester the carbon from methane in a stable and solid form. The results presented here are easily extended to the treatment of other methane streams—either more concentrated or dilute—and the results herein will guide the design and development of a new class of carbon-negative materials.

Environmental Sciences & Ecology↗

Source apportionment of VOCs, IVOCs and SVOCs by positive matrix factorization in suburban Livermore, California

Abstract. Gas- and particle-phase molecular markers provide highly specific information about the sources and atmospheric processes that contribute to air pollution. In urban areas, major sources of pollution are changing as regulation selectively mitigates some pollution sources and climate change impacts the surrounding environment. In this study, a comprehensive thermal desorption aerosol gas chromatograph (cTAG) was used to measure volatile, intermediate-volatility and semivolatile molecular markers every other hour over a 10 d period from 11 to 21 April 2018 in suburban Livermore, California. Source apportionment via positive matrix factorization (PMF) was performed to identify major sources of pollution. The PMF analysis identified 13 components, including emissions from gasoline, consumer products, biomass burning, secondary oxidation, aged regional transport and several factors associated with single compounds or specific events with unique compositions. The gasoline factor had a distinct morning peak in concentration but lacked a corresponding evening peak, suggesting commute-related traffic emissions are dominated by cold starts in residential areas. More monoterpene and monoterpenoid mass was assigned to consumer product emissions than biogenic sources, underscoring the increasing importance of volatile chemical products to urban emissions. Daytime isoprene concentrations were controlled by biogenic sunlight- and temperature-dependent processes, mediated by strong midday mixing, but gasoline was found to be the dominant and likely only source of isoprene at night. Biomass burning markers indicated residential wood burning activity remained an important pollution source even in the springtime. This study demonstrates that specific high-time-resolution molecular marker measurements across a wide range of volatility enable more comprehensive pollution source profiles than a narrower volatility range would allow.

54 ENVIRONMENTAL SCIENCES↗

Improving the particle dry deposition scheme in the CMAQ photochemical modeling system

Dry deposition of atmospheric aerosols in large-scale models is a critical, but highly uncertain, sink process with a strong dependence on particle size, meteorological conditions, and land surface properties. This study investigates the particle dry deposition scheme implemented in the standard Community Multiscale Air Quality (CMAQ) model v5.2.1, characterizes its underlying parameterized components with comparison to a similar scheme in a contemporary regional-scale model, and proposes two updated schemes that are then evaluated with available ambient particle deposition velocity (V d ) measurements. Both updated schemes reduce the surprisingly strong dependence of deposition velocity on the aerosol mode width, with one scheme further introducing a dependence on vegetation coverage that is broadly consistent with variability in observations between vegetated and non-vegetated surfaces. Compared to the base scheme, the updated scheme with vegetation dependence increases V d for submicron particles and decreases it for larger particles by an average of 37% and –66%, respectively. This scheme performs statistically better than the base scheme, reducing fractional biases by 56%–97% for vegetated land-use types and has roughly equivalent performance over water. The base and updated schemes are tested with three annual CMAQ (v5.2.1) simulations for the year 2011; predicted ambient aerosol concentrations are evaluated with routine monitoring network observations and predicted dry deposition fluxes are evaluated with data from the Clean Air Status and Trends Network (CASTNET). The updated scheme with vegetation dependence reduces negative fractional biases for PM 10 by 41% and positive fractional biases for PM 2.5 organic carbon by 15%. This scheme has been incorporated into the most recent publicly accessible versions of CMAQ (v5.3 and beyond) to replace the scheme used in previous versions of CMAQ (v4.5 through v5.2.1).

54 ENVIRONMENTAL SCIENCES↗

A new process-based and scale-aware desert dust emission scheme for global climate models – Part I: Description and evaluation against inverse modeling emissions

Desert dust accounts for most of the atmosphere's aerosol burden by mass and produces numerous important impacts on the Earth system. However, current global climate models (GCMs) and land-surface models (LSMs) struggle to accurately represent key dust emission processes, in part because of inadequate representations of soil particle sizes that affect the dust emission threshold, surface roughness elements that absorb wind momentum, and boundary-layer characteristics that control wind fluctuations. Furthermore, because dust emission is driven by small-scale (~ 1 km or smaller) processes, simulating the global cycle of desert dust in GCMs with coarse horizontal resolutions (~ 100 km) presents a fundamental challenge. This representation problem is exacerbated by dust emission fluxes scaling nonlinearly with wind speed above a threshold wind speed that is sensitive to land-surface characteristics. Here, we address these fundamental problems underlying the simulation of dust emissions in GCMs and LSMs by developing improved descriptions of (1) the effect of soil texture on the dust emission threshold, (2) the effects of nonerodible roughness elements (both rocks and green vegetation) on the surface wind stress, and (3) the effects of boundary-layer turbulence on driving intermittent dust emissions. We then use the resulting revised dust emission parameterization to simulate global dust emissions in a standalone model forced by reanalysis meteorology and land-surface fields. We further propose (4) a simple methodology to rescale lower-resolution dust emission simulations to match the spatial variability of higher-resolution emission simulations in GCMs. The resulting dust emission simulation shows substantially improved agreement against regional dust emissions observationally constrained by inverse modeling. We thus find that our revised dust emission parameterization can substantially improve dust emission simulations in GCMs and LSMs.

54 ENVIRONMENTAL SCIENCES↗

Modeling dust mineralogical composition: sensitivity to soil mineralogy atlases and their expected climate impacts

Soil dust aerosols are a key component of the climate system, as they interact with short- and long-wave radiation, alter cloud formation processes, affect atmospheric chemistry and play a role in biogeochemical cycles by providing nutrient inputs such as iron and phosphorus. The influence of dust on these processes depends on its physicochemical properties, which, far from being homogeneous, are shaped by its regionally varying mineral composition. The relative amount of minerals in dust depends on the source region and shows a large geographical variability. However, many state-of-the-art Earth system models (ESMs), upon which climate analyses and projections rely, still consider dust mineralogy to be invariant. The explicit representation of minerals in ESMs is more hindered by our limited knowledge of the global soil composition along with the resulting size-resolved airborne mineralogy than by computational constraints. In this work we introduce an explicit mineralogy representation within the state-of-the-art Multiscale Online Nonhydrostatic AtmospheRe CHemistry (MONARCH) model. We review and compare two existing soil mineralogy datasets, which remain a source of uncertainty for dust mineralogy modeling and provide an evaluation of multiannual simulations against available mineralogy observations. Soil mineralogy datasets are based on measurements performed after wet sieving, which breaks the aggregates found in the parent soil. Our model predicts the emitted particle size distribution (PSD) in terms of its constituent minerals based on brittle fragmentation theory (BFT), which reconstructs the emitted mineral aggregates destroyed by wet sieving. Our simulations broadly reproduce the most abundant mineral fractions independently of the soil composition data used. Feldspars and calcite are highly sensitive to the soil mineralogy map, mainly due to the different assumptions made in each soil dataset to extrapolate a handful of soil measurements to arid and semi-arid regions worldwide. For the least abundant or more difficult-to-determine minerals, such as iron oxides, uncertainties in soil mineralogy yield differences in annual mean aerosol mass fractions of up to ~ 100 %. Although BFT restores coarse aggregates including phyllosilicates that usually break during soil analysis, we still identify an overestimation of coarse quartz mass fractions (above 2 µm in diameter). In a dedicated experiment, we estimate the fraction of dust with undetermined composition as given by a soil map, which makes up ~ 10 % of the emitted dust mass at the global scale and can be regionally larger. Changes in the underlying soil mineralogy impact our estimates of climate-relevant variables, particularly affecting the regional variability of the single-scattering albedo at solar wavelengths or the total iron deposited over oceans. All in all, this assessment represents a baseline for future model experiments including new mineralogical maps constrained by high-quality spaceborne hyperspectral measurements, such as those arising from the NASA Earth Surface Mineral Dust Source Investigation (EMIT) mission.

54 ENVIRONMENTAL SCIENCES↗

Molecular understanding of new-particle formation from α-pinene between -50 and +25 °C

Abstract. Highly oxygenated organic molecules (HOMs) contribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human health and Earth's climate. HOMs are formed by rapid, gas-phase autoxidation of volatile organic compounds (VOCs) such as α-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role in new-particle formation (NPF) and the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds such as sulfuric acid. Both the autoxidation reaction forming HOMs and their NPF rates are expected to be strongly dependent on temperature. However, experimental data on both effects are limited. Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN to address this question. In this study, we show that a decrease in temperature (from +25 to -50°C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (J1.7 nm) increase substantially. Measurements with two different chemical ionization mass spectrometers (using nitrate and protonated water as reagent ion, respectively) provide the molecular composition of the gaseous oxidation products, and a two-dimensional volatility basis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2 % at 25°C to 0.7 % at -50°C. However, there is a strong reduction of the saturation vapor pressure of each oxidation state as the temperature is reduced. Overall, the reduction in volatility with temperature leads to an increase in the nucleation rates by up to 3 orders of magnitude at -50°C compared with 25°C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature, since the neutral molecular clusters have increased stability against evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic NPF at the molecular level. Our measurements, therefore, improve our understanding of pure biogenic NPF for a wide range of tropospheric temperatures and precursor concentrations.

54 ENVIRONMENTAL SCIENCES↗

Department of Energy’s Atmospheric System Research (ASR) Program’s Workshop on the Future of Atmospheric Large Eddy Simulation (LES): Workshop Report

Large-eddy simulation (LES) is used as a tool to understand physical processes such as turbulence, aerosols, clouds, precipitation, radiation, the interactions among all these, and their interactions with the underlying surface. Over the next 10 years, LES will drive fundamental progress in open scientific questions in these areas as LES is increasingly used to gain understanding of complex interacting physical processes involving atmospheric turbulence. This growth will be driven both by scientific demand and the expansion of computational resources needed to conduct LES, and the form that the growth takes will largely be determined by how computational resources are leveraged for scientific gain. In particular, we suggest that computational resources are likely to be leveraged in two separate but not necessarily distinct ways. On one hand, growth in computational resources will allow LES to be made more routine, that is, performed more frequently, while on the other hand, the computational expense (measured in total floating point operations) afforded to individual LES will expand dramatically, allowing simulations to increase in both domain size and resolution as well as physical detail. Current U.S. Department of Energy (DOE) projects such as LES ARM Symbiotic Simulation and Observation Activity (LASSO) are leading the way in conducting routine LES, building large, public databases that are accessible for data science, sensitivity studies, and training for machine learning. LES will also become more routine as it becomes more accessible for individual researchers to address their scientific questions of interest. Scientific questions addressed by LES over the next 10 years are likely to include cloud organization and aggregation; aerosol cloud interactions and atmospheric chemistry (including geo-engineering); urban-scale LES; atmospheric extreme events, ranging from small-scale severe weather to wildfires; and ocean-wave-atmosphere interactions. Further LES-related research will likely grow significantly in areas related to societal impact studies of air quality and extreme weather events, applications to renewable energy forecasting and resource assessment, and aid in decision-making processes. The growth in the use of LES in atmospheric science research will drive the need for better physical process representations (e.g., cloud aerosol microphysics, radiation, and atmospheric chemistry) at the scales resolved by LES. To date, many of the process representations used by LES have been taken directly from coarser-resolution models. Promising methods for LES process representations include superdroplet and quadrature methods for microphysics, 3D approaches for radiation, and better representation of chemistry and aerosol processes. At LES resolution, land-atmosphere interactions for complex terrains, land cover/types, biogeochemistry, and plant canopy models are needed as an improvement beyond traditional and widely used Monin-Obuhkov similarity theory.

54 ENVIRONMENTAL SCIENCES↗

Advancing Marine Arctic Science through Facilitating International Collaborations

The Consortium for the Advancement of Marine Arctic Science (CAMAS) held its inaugural Workshop and Early Career School in Santa Fe, New Mexico, from 13 to 16 February 2024. The event brought together 80 Arctic marine scientists from around the world to discuss current research and to develop ideas for collaborative research projects that can be executed in the next few years to advance our understanding of the marine Arctic system.

54 ENVIRONMENTAL SCIENCES↗

Are Atmospheric Models Too Cold in the Mountains? The State of Science and Insights from the SAIL Field Campaign

Mountains play an outsized role in water resource availability, and the amount and timing of water they provide depend strongly on temperature. To that end, we ask the question: How well are atmospheric models capturing mountain temperatures? We synthesize results showing that high-resolution, regionally relevant climate models produce 2-m air temperature (T2m) measurements colder than what is observed (a “cold bias”), particularly in snow-covered midlatitude mountain ranges during winter. We find common cold biases in 44 studies across global mountain ranges, including single-model and multimodel ensembles. We explore the factors driving these biases and examine the physical mechanisms, data limitations, and observational uncertainties behind T2m. Our analysis suggests that the biases are genuine and not due to observation sparsity or resolution mismatches. Cold biases occur primarily on mountain peaks and ridges, whereas valleys are often warm biased. Our literature review suggests that increasing model resolution does not clearly mitigate the bias. By analyzing data from the Surface Atmosphere Integrated Field Laboratory (SAIL) field campaign in the Colorado Rocky Mountains, we test various hypotheses related to cold biases and find that local wind circulations, longwave (LW) radiation, and surface-layer parameterizations contribute to the T2m biases in this particular location. We conclude by emphasizing the value of coordinated model evaluation and development efforts in heavily instrumented mountain locations for addressing the root cause(s) of T2m biases and improving predictive understanding of mountain climates.

54 ENVIRONMENTAL SCIENCES↗

Are Atmospheric Models Too Cold in the Mountains? The State of Science and Insights from the SAIL Field Campaign

Mountains play an outsized role in water resource availability, and the amount and timing of water they provide depend strongly on temperature. To that end, we ask the question: How well are atmospheric models capturing mountain temperatures? We synthesize results showing that high-resolution, regionally relevant climate models produce 2-m air temperature (T2m) measurements colder than what is observed (a “cold bias”), particularly in snow-covered midlatitude mountain ranges during winter. We find common cold biases in 44 studies across global mountain ranges, including single-model and multimodel ensembles. We explore the factors driving these biases and examine the physical mechanisms, data limitations, and observational uncertainties behind T2m. Our analysis suggests that the biases are genuine and not due to observation sparsity or resolution mismatches. Cold biases occur primarily on mountain peaks and ridges, whereas valleys are often warm biased. Our literature review suggests that increasing model resolution does not clearly mitigate the bias. By analyzing data from the Surface Atmosphere Integrated Field Laboratory (SAIL) field campaign in the Colorado Rocky Mountains, we test various hypotheses related to cold biases and find that local wind circulations, longwave (LW) radiation, and surface-layer parameterizations contribute to the T2m biases in this particular location. We conclude by emphasizing the value of coordinated model evaluation and development efforts in heavily instrumented mountain locations for addressing the root cause(s) of T2m biases and improving predictive understanding of mountain climates.

54 ENVIRONMENTAL SCIENCES↗

Acclimation of Phytoplankton Fe:C Ratios Dampens the Biogeochemical Response to Varying Atmospheric Deposition of Soluble Iron

Abstract Dissolved iron (dFe) plays an important role in regulating marine productivity. In high nutrient, low chlorophyll regions (>33% of the global ocean), iron is the primary growth limiting nutrient, and elsewhere iron can regulate nitrogen fixation by diazotrophs. The link between iron availability and carbon export is strongly dependent on the phytoplankton iron quotas or cellular Fe:C ratios. This ratio varies by more than an order of magnitude in the open ocean and is positively correlated with ambient dFe concentrations in field observations. Representing Fe:C ratios within models is necessary to investigate how ocean carbon cycling will interact with perturbations to iron cycling in a changing climate. The Community Earth System Model ocean component was modified to simulate dynamic, group‐specific, phytoplankton Fe:C that varies as a function of ambient iron concentration. The simulated Fe:C ratios improve the representation of the spatial trends in the observed Fe:C ratios. The acclimation of phytoplankton Fe:C ratios dampens the biogeochemical response to varying atmospheric deposition of soluble iron, compared to a fixed Fe:C ratio. However, varying atmospheric soluble iron supply has first order impacts on global carbon and nitrogen fluxes and on nutrient limitation spatial patterns. Our results suggest that pyrogenic Fe is a significant dFe source that rivals mineral dust inputs in some regions. Changes in dust flux and iron combustion sources (anthropogenic and wildfires) will modify atmospheric Fe inputs in the future. Accounting for dynamic phytoplankton iron quotas is critical for understanding ocean biogeochemistry and projecting its response to variations in atmospheric deposition.

Environmental Sciences & Ecology↗

2025 Atmospheric Radiation Measurement (ARM) Annual Report

ARM is a multi-laboratory, U.S. Department of Energy (DOE) Office of Science user facility and a key contributor to atmospheric research efforts. For more than 30 years, ARM has supported the DOE and Office of Science missions by providing atmospheric observations to enable scientific discovery, transform our understanding of the atmosphere, and evaluate and improve the accuracy of atmospheric models. ARM’s cutting-edge capabilities for scientists include continuously operating ground-based observatories, aerial observation platforms, and high performance computing.

54 ENVIRONMENTAL SCIENCES↗

Evaluating Entrainment–Mixing Characteristics through Direct Comparisons of Drop Size Distributions Using In Situ Observations from ACE-ENA

Abstract Constraining the impacts of entrainment and associated mixing (i.e., entrainment–mixing) on cloud properties continues to be difficult, partly due to observational uncertainties as well as a lacking consensus of which methodologies for diagnosing entrainment–mixing are most appropriate. This study introduces a novel method to evaluate the presence and degree of inhomogeneous and homogeneous mixing using ∼100 h of in situ observations from a research aircraft over the northeastern Atlantic. Specifically, drop size distributions are compared between regions containing negligible and significant entrainment for select flight legs, making a direct characterization of the degree of homogeneous and inhomogeneous mixing possible. A measure of drop concentration variance is used as a proxy variable to diagnose entrainment–mixing. Results correspond well with entrainment–mixing metrics, showing lower Damköhler numbers where drop size distributions shift toward smaller drop sizes (i.e., inhomogeneous mixing) and greater transition length scales where drop size distributions do not (i.e., homogeneous mixing). Inhomogeneous mixing occurs in most samples from Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA) (regardless of homogeneous mixing frequencies increasing with increasing spatial resolution from ∼100 to ∼10 m) and is associated with decreased drop size relative dispersion and both greater aerosol and drop concentrations compared with homogeneous mixing. Precipitating clouds have a greater frequency of homogeneous mixing compared with nonprecipitating clouds. The proposed methodology is similarly applied to in situ observations of southeast Pacific stratocumulus, shallow convective clouds over central Oklahoma and low-level clouds over the Southern Ocean. All four locations are primarily dominated by inhomogeneous mixing with minimal variability among each region.

Clouds↗