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Hygroscopicity of organic compounds as a function of carbon chain length, carboxyl, hydroperoxy, and carbonyl functional groups

The albedo and microphysical properties of clouds are controlled in part by the hygroscopicity of particles serving as cloud condensation nuclei (CCN). Hygroscopicity of complex organic mixtures in the atmosphere varies widely and remains challenging to predict. Here we present new measurements characterizing the CCN activity of pure compounds in which carbon chain length and the number of hydroperoxy, carboxyl, and carbonyl functional groups were systematically varied to establish the contributions of these groups to organic aerosol apparent hygroscopicity. Apparent hygroscopicity decreased with carbon chain length and increased with polar functional groups in the order carboxyl > hydroperoxy > carbonyl. Activation diameters at different supersaturations deviated from the -3/2 slope in log-log space predicted by Köhler theory, suggesting that water solubility limits CCN activity of particles composed of weakly functionalized organic compounds. Results are compared to a functional group contribution model that predicts CCN activity of organic compounds. The model performed well for most compounds but under-predicted the CCN activity of hydroperoxy groups. New best-fit hydroperoxy group/water interaction parameters were derived from the available CCN data. Lastly, these results may help improve estimates of the CCN activity of ambient organic aerosols from composition data.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exobiology experiments for Earth-orbital platforms

Low-gravity (microgravity) studies relevant to prebiotic evolution and the history of the biogenic elements (C, H, N, O, P, S) are particularly suited to orbital platforms. Relevant to these topics are phenomena such as gas-particle interactions (e.g., formation of organic aerosols via photolytic reactions) including nucleation, condensation, evaporation, adsorption, and catalytic reactions on surfaces; and, small-particle or grain interactions (e.g., growth of interstellar dust particles and planetesimals) including processes such as aggregation (or coagulation), scavenging, and collisions. Both gas-particle and grain (i.e., dust, crystals, organic aerosols, etc.) interactions studies can benefit from microgravity and are pertinent to studies in the areas of chemical evolution in the solar nebula, the interstellar medium, and planetary atmospheres; growth of planetesimals; and prebiotic evolution. In general, the microgravity environment allows for long duration and controlled simulations of processes occurring in exobiologically significant systems such as Titan's atmosphere, interstellar dust clouds, and the solar nebula in which gas-particle or particle-particle interactions play a significant role.

Huntington, J. L.↗

Impact of Assimilated and Interactive Aerosol on Tropical Cyclogenesis

This article investigates the impact 3 of Saharan dust on the development of tropical cyclones in the Atlantic. A global data assimilation and forecast system, the NASA GEOS-5, is used to assimilate all satellite and conventional data sets used operationally for numerical weather prediction. In addition, this new GEOS-5 version includes assimilation of aerosol optical depth from the Moderate Resolution Imaging Spectroradiometer (MODIS). The analysis so obtained comprises atmospheric quantities and a realistic 3-d aerosol and cloud distribution, consistent with the meteorology and validated against Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) and CloudSat data. These improved analyses are used to initialize GEOS-5 forecasts, explicitly accounting for aerosol direct radiative effects and their impact on the atmospheric dynamics. Parallel simulations with/without aerosol radiative effects show that effects of dust on static stability increase with time, becoming highly significant after day 5 and producing an environment less favorable to tropical cyclogenesis.

dust↗

"Electrostructural Phase Changes" In Charged Particulate Clouds: Planetary and Astrophysical Implications

There is empirical evidence that freely-suspended triboelectrostatically charged particulate clouds of dielectric materials undergo rapid conversion from (nominally) monodispersed "aerosols" to a system of well-defined grain aggregates after grain motion or fluid turbulence ceases within the cloud. In United States Microgravity Laboratory Space Shuttle experiments USML-1 and USML-2, it was found that ballistically-energized grain dispersions would rapidly convert into populations of filamentary aggregates after natural fluid (air) damping of grain motion. Unless continuously disrupted mechanically, it was impossible to maintain a non-aggregated state for the grain clouds of sand-size materials. Similarly, ground- based experiments with very fine dust-size material produced the same results: rapid, impulsive "collapse" of the dispersed grains into well-defined filamentary structures. In both ground-based and microgravity experiments, the chains or filaments were created by long-range dipole electrostatic forces and dipole-induced dielectric interactions, not by monopole interactions. Maintenance of the structures was assisted by short-range static boundary adhesion forces and van der Waals interactions. When the aggregate containers in the USML experiments were disturbed after aggregate formation, the quiescently disposed filaments would rearrange themselves into fractal bundles and tighter clusters as a result of enforced encounters with one another. The long-range dipole interactions that bring the grains together into aggregates are a product of randomly-distributed monopole charges on the grain surfaces. In computer simulations, it has been shown that when the force vectors of all the random charges (of both sign) on a grain are resolved mathematically by assuming Coulombic interaction between them, the net result is a dipole moment on individual grains, even though the grains are electrically neutral insofar as there is no predominance, on their surface, of one charge sign over another. The random charges of both sign derive from natural grain-to-grain interactions that produce triboelectrification via charge exchange every time grain surfaces make contact with one another. The conversion from a random distribution of grains (upon which there are randomly distributed charges) into an organization of electrostatically-ordered aggregates, can be regarded (within the framework of granular-material science) as an "electrical or Coulombic phase change" of the particulate cloud. It is not totally dissimilar from the more normal phase-change concept in which, for example, a gas with long free-path-molecules suddenly becomes a solid as a result of structural ordering of the molecules (notably, also the result of electronic forces, albeit at a different scale). In both the gas-to-solid case, and the aerosol-to-aggregate case, the same materials and charges are present before and after the phase change, but their arrangement now has a higher degree of order and a lower-energy configuration. An input of energy into the system is required to reverse the situation. The aggregates in the USML experiments were observed to undergo at least two phase changes as noted above. The point about phase changes, and by implication, the "electrostructural" reorganizations in particulate clouds, is the following: (a) they can occur very rapidly, almost spontaneously, above a critical cloud density, (b) in going from a higher energy state to a lower energy state, they convert to a denser system, (c) energy must be required to reverse the situation, implying that energy is released during the high-to-low energy phase change. In applying this information to natural particulate clouds, some inferences can be made (it is stressed that reference is still to dielectric materials attracted by dipole forces). There are several natural settings to which the USML observations apply, and to which the phase-change implications likewise apply. Dense clouds of triboelectrically-charged, kinetically-energized grains are to be found in volcanic eruptions (particularly on earth), aeolian dust storms (particularly on Mars), meteorite impact ejecta curtains (on all planets), in "immature" debris rings around planets (e.g., that from which our own Moon may have condensed), and in gravitationally collapsing protoplanetary dust/planetesimal debris disks where dielectric granules are being increasingly brought into collisional relationships with one another (increasing both charge exchange and physical proximity). It is noted that in many of these cases, the degree of electrical charging on the grains is likely to be much higher than that in the USML experiments where charging was not enhanced above the "normal", naturally encountered level for the particular materials (quartz, glass, and various silicate minerals). Application of the phase-change concept suggests that volcanic, aeolian, and impact debris clouds may, under certain circumstances, undergo rapid, impulsive, or even catastrophic collapse into a denser state that will lead to rapid precipitation or fall-out of suspended particulates. Although this idea has been suggested previously by the author , the phase change concept possibly permits some new insights into cloud-system behavior. For example, in a protoplanetary debris disk, the work of gravity may suddenly be enhanced by electrostatically driven collapse of the system when materials reach a critical intergranular spacing or grain number density. This might reduce the rate of planet formation by orders of magnitude (considering the ratio of g-forces to electrostatic ones for very small grains in close proximity), and indeed, it might drive the collapse into a system configuration that would perhaps not be created by gravity alone. Additional information is contained in the original.

Marshall, J. R.↗

Assessing Alternatives in the Systems Engineering Process: Case Study of an Earth Observing Satellite Concept

Defining design alternatives constitutes one of the critical initial steps of the systems engineering process. Once these design alternatives have been identified, assessing which alternatives best satisfy the project’s objectives can prove to be challenging when dealing with complex decision frameworks. Complex systems often involve the participation of different interest groups, who have different value systems and are focused on distinct aspects of the project. For example, design alternatives might be assessed predominantly for their technical merit by one group of stakeholders, while a different group might be more inclined to assess the design alternatives primarily based on programmatic values. MESCAL (Monitoring the Evolving State of Clouds and Aerosol Layers) is an ongoing NASA / CNES (Centre National d’Etudes Spatiales) joint study for an active remote sensing Earth observing satellite. Several design alternatives have been identified and the assessment of these alternatives requires consideration of a variety of factors. This paper presents the approach that was used to support a global assessment of the MESCAL design alternatives. A mapping of the interactions between mission, instrument, and science requirements was modeled to support the assessment of the trade space. In addition, a set of metrics was developed to structure the assessment that was conducted. Finally, this paper also discusses the general applicability of these metrics to other science mission concepts in the formulation phase.

Ivanco, Marie L.↗

A Sensitivity Study of Radiative Fluxes at the Top of Atmosphere to Cloud-Microphysics and Aerosol Parameters in the Community Atmosphere Model CAM5

In this study, we investigated the sensitivity of net radiative fluxes (FNET) at the top of atmosphere (TOA) to 16 selected uncertain parameters mainly related to the cloud microphysics and aerosol schemes in the Community Atmosphere Model version 5 (CAM5). We adopted a quasi-Monte Carlo (QMC) sampling approach to effectively explore the high dimensional parameter space. The output response variables (e.g., FNET) were simulated using CAM5 for each parameter set, and then evaluated using generalized linear model analysis. In response to the perturbations of these 16 parameters, the CAM5-simulated global annual mean FNET ranges from -9.8 to 3.5 W m-2 compared to the CAM5-simulated FNET of 1.9 W m-2 with the default parameter values. Variance-based sensitivity analysis was conducted to show the relative contributions of individual parameter perturbation to the global FNET variance. The results indicate that the changes in the global mean FNET are dominated by those of cloud forcing (CF) within the parameter ranges being investigated. The size threshold parameter related to auto-conversion of cloud ice to snow is confirmed as one of the most influential parameters for FNET in the CAM5 simulation. The strong heterogeneous geographic distribution of FNET variation shows parameters have a clear localized effect over regions where they are acting. However, some parameters also have non-local impacts on FNET variance. Although external factors, such as perturbations of anthropogenic and natural emissions, largely affect FNET variations at the regional scale, their impact is weaker than that of model internal parameters in terms of simulating global mean FNET in this study. The interactions among the 16 selected parameters contribute a relatively small portion of the total FNET variations over most regions of the globe. This study helps us better understand the CAM5 model behavior associated with parameter uncertainties, which will aid the next step of reducing model uncertainty via calibration of uncertain model parameters with the largest sensitivity.

aerosol↗

Community Modeling and Long-Term Predictions of the Integrated Water Cycle. Report from the September 2012 Workshop

Water is a key component of the earth and human systems due to its strong interactions with the energy cycle and its vital roles in the energy-water-land system. Uncertainties in predicting the integrated water cycle can limit our abilities to address the energy and environmental challenges today and in the future. Modeling the integrated water cycle contributes to the Department of Energy’s (DOE) core competencies in integrative modeling, drawing from unique and highly relevant research on cloud, aerosol, terrestrial ecosystem, carbon cycle, and subsurface processes, as well as climate and earth system modeling and integrated assessment modeling. Synthesizing new process knowledge and innovative computational methods in integrated models of the human-earth system can advance predictive capabilities relevant to DOE missions. This report describes the DOE workshop on Community Modeling and Long-Term Predictions of the Integrated Water Cycle, held September 2012 in Washington DC. The workshop serves as a launching point and major organizing event to identify challenges and plan the development of next-generation human-earth system models for improving long-term predictions of the regional-scale integrated water cycle. More specifically, the workshop aims to: identify core modeling capabilities while identifying key research gaps, with an emphasis on improving model fidelity; reveal relevant and critical capabilities and needs for observations, analytical frameworks, and data management that underpin the development, testing, and validation of our main models and model components; engage the research community in strategies for improving synthesis and integration; elucidate opportunities for collaborations within DOE and with other agencies and institutions that have complementary and essential expertise in specific aspects of the water cycle; and improve understanding of the nature and characteristics of long-term scientific information requirements for DOE’s energy and environmental missions and, as appropriate, for mission needs of other partner agencies. The workshop benefited from substantial inputs provided by the broad scientific community and interagency participation. The topical and crosscutting research challenges identified at the workshop have been synthesized into three overarching Science Grand Challenges and three Integrative Modeling Experiments summarized in this report. These challenges represent remarkable opportunities for interagency collaborations to improve predictions of the integrated water cycle for significant scientific and user impacts.

54 ENVIRONMENTAL SCIENCES↗

Possible Influences of Air Pollution, Dust and Sandstorms on the Indian Monsoon

In Asian monsoon countries, such as China and India, human health and safety problems caused by air pollution are becoming increasingly serious, due to the increased loading of atmospheric pollutants from waste gas emissions and from rising energy demand associated with the rapid pace of industrialization and modernization. Meanwhile, uneven distribution of monsoon rain associated with flash floods or prolonged drought, has caused major loss of human life and damage to crops and.property with devastating societal impacts. Historically, air-pollution and monsoons research are treated as separate problems. However recent studies have suggested that the two problems may be intrinsically linked and need to be studied jointly. Fundamentally, aerosols can affect precipitation through radiative effects cif suspended particles in the atmosphere (direct effect) and/or by interfering and changing: the cloud and precipitation formation processes (indirect effect). Based on their optical properties, aerosols can be classified into two types.: those that absorb solar radiation, and those that do not. Both types of aerosols scatter sunlight and reduce the amount of solar radiation from reaching the Earth's surface, causing it to cool. The surface cooling increases atmospheric stability and reduces convection potential, Absorbing aerosols, however, in addition to cooling the surface, can heat the atmosphere. The heating of the atmosphere may reduce the amount of low clouds by increased evaporation in cloud drops. The heating, however, may induce rising motion, enhance low-level moisture, convergence and, hence, increases rainfall, The latent heating from enhanced rainfall may excite feedback processes in the large-scale circulation, further amplify.the initial response to aerosol heating and producing more rain. Additionally, aerosols can increase the concentration of cloud condensation nuclei (CCN), increase cloud amount and decrease coalescence and collision rates, leading to reduced precipitation. However, in the presence of increasing moist and warm air, the reduced coalescence/collision may lead to supercooled drops at higher altitudes where ice precipitation falls and melts. The latent heat release from freezing aloft and melting below implies greater upward heat transport in polluted clouds and invigorate deep convection. In this way, aerosols may lead to increased local convection. Hence, depending on the ambient large-scale conditions and dynamical feedback processes, aerosols' effect on precipitation can be positive, negative or mixed. In the Asian monsoon and adjacent regions, the aerosol forcing and responses of the water cycle are even more complex, Both direct and indirect effects may take place locally and simultaneously, interacting with each other. in addition to local effects, monsoon rainfall may be affected by aerosols transported from other regions and intensified through large-scale circulation and moisture feedback. Thus, dust transported by the large-scale circulation from the adjacent deserts to northern India may affect rainfall over the Bay of Bengal; sulphate and black carbon front industrial pollution in central, southern China and northern India may affect the rainfall regime over the Korean peninsula and Japan; organic and black carbon front biomass burning from Indo-China may modulate the pre-monsoon rainfall regime over southern China and coastal regions, contributing to variability in differential heating and cooling of the atmosphere and to the land-sea thermal contrast. During the pre-monsoon season and monsoon breaks, it has been suggested that radiative forcing by absorbing aerosols have nearly the same order of magnitude as the forcing due to latent heating from convection and surface fluxes. The magnitude of the total aerosol radiative cooling due to sulphates and soot is of the order of 20-40 W/m2 over the Asian monsoon land region in the pre-monsoon season, compared to about 1-2 W/m2 for global warng. However, the combined forcing at the surface and in the atmosphere, including all species. if aerosols, and details of aerosol mixing, and impacts on the energy and water cycles in the monsoon land regions, are not well known.

Lau, William K. M.↗

Tight Coupling of Surface and In-Plant Biochemistry and Convection Governs Key Fine Particulate Components over the Amazon Rainforest

We report that throughout the troposphere over the Amazon rainforest, isoprene epoxydiol-secondary organic aerosols (IEPOX-SOA) are key components of submicrometer particle mass. IEPOX-SOA is thought to form by multiphase chemical pathways in the atmosphere, but using detailed model simulations, we show that these pathways are strongly inhibited by the solid particle phase state prevailing in the upper troposphere. We find that 2-methyltetrol gases formed by in-plant biochemical oxidation pathways, their partitioning to fine particles, and dissolution in cloud droplets can explain over 90% of IEPOX-SOA mass concentrations in the upper troposphere. In agreement with previous PM10 chiral measurements, our simulations indicate that plant biochemical processes are the dominant source of particulate 2-methyltetrols in the lower troposphere as well (>70%). Our results imply that in-plant biochemistry plays a central but previously unidentified role in aerosol processes and atmosphere-biosphere-climate interactions over the rainforest.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Texas A&M University Mobile Facility Measurements during TRACER (Field Campaign Report)

One of the main goals of the U.S Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Tracking Aerosol Convection Interactions Experiment (TRACER) near Houston, Texas is to improve understanding of how meteorology and aerosols impact storm dynamical and microphysical processes in deep convection to better constrain and improve their model representation. The Houston area is strongly influenced by sea- and bay-breeze circulations that generate convergence and help to initiate and organize deep convection. To properly isolate and understand the roles of varied meteorological conditions and cloud condensation nuclei (CCN) and ice nucleation particles (INP) distributions in different air masses, co-located thermodynamic, kinematic, and aerosol vertical profile observations are needed. The focus of this campaign was to provide key measurements in air masses both in front of and behind sea/bay breeze fronts moving through the greater Houston area to sample the airmass heterogeneity. The overarching scientific goal of this campaign is to understand how the vertical distributions of both CCN and INP correspond to the inflow layer of deep convection in maritime, background continental, and polluted continental air masses, and how these variations influence deep convection. To fully sample the heterogeneity in both meteorological conditions and aerosols across the sea-breeze front (SBF), Texas A&M University (TAMU) deployed a InterMet 3050A 403 MHz mobile unit launching iMet-4 radiosondes and the new Rapid Onsite Atmospheric Measurement Van (ROAM-V) for aerosol sampling during the TRACER intensive operational period (IOP) from June to September 2022. The suite of instruments deployed on ROAM-V included a condensation particle counter (CPC; GRIMM Model 5.403 CPC), scanning mobility particle sizer (SMPS; TSI 3750 detector, TSI 3082 classifier, TSI 3088 neutralizer, TSI 3081A differential mobility analyzer), cloud condensation nuclei counter (Droplet Measurement Technologies CCN counter), micropulse lidar (Droplet Measurement Technologies micropulse lidar [miniMPL]), and a Davis Rotating Uniform size-cut Monitor (DRUM; DRUMAir 4-DRUM). Before sampling at each location, the latitude and longitude were recorded using the Global Positioning System (GPS) on the phone application “My Altitude”. The DRUM data were collected as part of a closely related ARM field campaign and also supported by DOE Atmospheric System Research grant DE-SC0021047. The TAMU team sampled these airmass heterogeneities by strategically choosing deployment sites in a different airmass than the ARM fixed sites in La Porte and Guy, Texas. On days when the sea/bay breeze boundary was pushing inland, the TAMU team would usually sample the airmass on the maritime side of the SBF at a coastal site in Galveston, Texas in the early afternoon (1730-1900 UTC) and then move inland ahead of the SBF to sample the airmass on the continental side during late afternoon (2030-2230). Figure 1 shows the Galveston maritime site and the array of sites for the late afternoon continental measurements.

54 ENVIRONMENTAL SCIENCES↗

Overview of ACE-Asia Spring 2001 Investigations on Aerosol Radiative Effects and Related Aerosol Properties

A primary, ACE-Asia objective was to quantify the interactions between aerosols and radiation in the Asia-Pacific region. Toward this end, radiometric and related aerosol measurements were made from ocean, land, air and space platforms. Models that predict aerosol fields guided the measurements and are helping integrate and interpret results. Companion overview's survey these measurement and modeling components. Here we illustrate how these components were combined to determine aerosol radiative. impacts and their relation to aerosol properties. Because clouds can obscure or change aerosol direct radiative effects, aircraft and ship sorties to measure these effects depended on predicting and finding cloud-free areas and times with interesting aerosols present. Pre-experiment satellite cloud climatologies, pre-flight aerosol and cloud forecasts, and in-flight guidance from satellite imagery all helped achieve this. Assessments of aerosol regional radiative impacts benefit from the spatiotemporal coverage of satellites, provided satellite-retrieved aerosol properties are accurate. Therefore, ACE-Asia included satellite retrieval tests, as part of many comparisons to judge the consistency (closure) among, diverse measurements. Early results include: (1) Solar spectrally resolved and broadband irradiances and optical depth measurements from the C-130 aircraft and at Kosan, Korea yielded aerosol radiative forcing efficiencies, permitting comparisons between efficiencies of ACE-Asia and INDOEX aerosols, and between dust and "pollution" aerosols. Detailed results will be presented in separate papers. (2) Based on measurements of wavelength dependent aerosol optical depth (AOD) and single scattering albedo the estimated 24-h a average aerosol radiative forcing efficiency at the surface for photosynthetically active radiation (400 - 700 nm) in Yulin, China is approx. 30 W sq m per AOD(500 nm). (3) The R/V Brown cruise from Honolulu to Sea of Japan sampled an aerosol optical depth gradient, with AOD(500 nm) extremes from 0.1 to 1.1. On the Pacific transit from Honolulu to Hachijo AOD(500 nm) averaged 0.2, including increases to 0.4 after several storms, suggesting the strong impact of wind-generated seasalt. The AOD maximum, found in the Sea of Japan, was influenced by dust and anthropogenic sources. (4) In Beijing, single scattering albedo retrieved from AERONET sun-sky radiometry yielded midvisible SSA=0.88 with strong wavelength dependence, suggesting a significant black carbon component. SSA retrieved during dust episodes was approx. 0.90 and variable but wavelength neutral reflecting the presence of urban haze with the dust. Downwind at Anmyon Island SSA was considerably higher, approx. 0.94, but wavelength neutral for dust episodes and spectrally dependent during non dust periods. (5) Satellite retrievals show major aerosol features moving from Asia over the Pacific; however, determining seasonal-average aerosol effects is hampered by sampling frequency and large-scale cloud systems that obscure key parts of aerosol patterns. Preliminary calculations using, satellite-retrieved AOD fields and initial ACE-Asia aerosol properties (including sulfates, soot, and dust) yield clear-sky aerosol radiative effects in the seasonal-average ACE-Asia plume exceeding those of manmade greenhouse gases. Quantifying all-sky direct aerosol radiative effects is complicated by the need to define the height of absorbing aerosols with respect to cloud decks.

Russell, Philip B.↗

Improving Cloud and Precipitation Physics in a Seamless Regional-Global Climate Model

The objective of this project was to improve numerical simulation and forecasting of regional climate by incorporating recent advances in the understanding and modeling of atmospheric aerosols, clouds, and precipitation mechanisms in an advanced regional-global numerical model. We utilized the Ocean-Land-Atmosphere Model (OLAM), which is a global model that is partly derived from the Regional Atmospheric Modeling System (RAMS). OLAM’s global grid can be configured with a high resolution locally-refined region that provides seamless two-way communication between global and regional scales of motion. The full interaction between regional and global climate is a major improvement in accuracy and applicability over conventional regional climate models (RCMs) that are one-way nested within global climate models (GCMs). When OLAM is applied as a RCM, most computational effort is concentrated in its high-resolution region, and the lower-resolution remainder of its global domain adds relatively minor computational cost while providing significant benefits.

54 ENVIRONMENTAL SCIENCES↗

Environmental Persistence of Biological Aerosols in Outdoor and Simulated Environments

The fate of biological aerosols in the atmosphere depends on the unique and dynamic environmental conditions it is exposed to during transport. There exist many processes that can impact the effectiveness of an aerosol release, and its fate in the environment. Aerosol properties may be modified if biological particles that are released into the atmosphere interact with free radicals, volatile organic compounds(VOC), semi-volatile organic compounds, and inorganic gasphase compounds, such as NOx and SOx. Meteorological conditions such as ultraviolet(UV)- light, relative humidity(RH), and temperature have also been shown to affect biological aerosols, with interactions dependent on both the organism and aerosol's chemical make-up. Oxidation or secondary-organic aerosol (SOA) formations on the particle can also lead to changes in surface proteins and extra-cellular nucleic acids that may agent detection technologies, at a different rate than the infectivity of the agents. Once modified, agents may then be transported via many atmospheric processes such as deposition or incorporation into cloud condensation nuclei(CCN). Although these processes are known, it is unclear what the resulting form and potency ofthe bioaerosol may be after alteration by these processes.

54 ENVIRONMENTAL SCIENCES↗

Importance of heterogeneous processes to tropospheric chemistry - Studies with a one-dimensional model

A one-dimensional, time-dependent model of tropospheric air composition is developed which incorporates several heterogeneous physical and chemical processes. The model includes the interaction of gases, aerosols, and hydrometeors through the physical mechanisms of nucleation, condensation, evaporation, coagulation, coalescence, and deliquescence. Precipitation, sedimentation, and dry deposition act to remove material from the atmosphere, while chemical transformations occur both in the vapor and the condensed phases. The model also incorporates the sources and vertical diffusion of gases and particles, as well as changes in the solar intensity caused by light-scattering from aerosols and clouds. Preliminary simulations made using this model indicate that rainout and washout processes strongly influence the distributions of tropospheric gases and aerosols under certain conditions.

Turco, R. P.↗

Automated Identification of Characteristic Droplet Size Distributions in Stratocumulus Clouds Utilizing a Data Clustering Algorithm

Abstract Droplet-level interactions in clouds are often parameterized by a modified gamma fitted to a “global” droplet size distribution. Do “local” droplet size distributions of relevance to microphysical processes look like these average distributions? This paper describes an algorithm to search and classify characteristic size distributions within a cloud. The approach combines hypothesis testing, specifically, the Kolmogorov–Smirnov (KS) test, and a widely used class of machine learning algorithms for identifying clusters of samples with similar properties: density-based spatial clustering of applications with noise (DBSCAN) is used as the specific example for illustration. The two-sample KS test does not presume any specific distribution, is parameter free, and avoids biases from binning. Importantly, the number of clusters is not an input parameter of the DBSCAN-type algorithms but is independently determined in an unsupervised fashion. As implemented, it works on an abstract space from the KS test results, and hence spatial correlation is not required for a cluster. The method is explored using data obtained from the Holographic Detector for Clouds (HOLODEC) deployed during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. The algorithm identifies evidence of the existence of clusters of nearly identical local size distributions. It is found that cloud segments have as few as one and as many as seven characteristic size distributions. To validate the algorithm’s robustness, it is tested on a synthetic dataset and successfully identifies the predefined distributions at plausible noise levels. The algorithm is general and is expected to be useful in other applications, such as remote sensing of cloud and rain properties. Significance Statement A typical cloud can have billions of drops spread over tens or hundreds of kilometers in space. Keeping track of the sizes, positions, and interactions of all of these droplets is impractical, and, as such, information about the relative abundance of large and small drops is typically quantified with a “size distribution.” Droplets in a cloud interact locally, however, so this work is motivated by the question of whether the cloud droplet size distribution is different in different parts of a cloud. A new method, based on hypothesis testing and machine learning, determines how many different size distributions are contained in a given cloud. This is important because the size distribution describes processes such as cloud droplet growth and light transmission through clouds.

54 ENVIRONMENTAL SCIENCES↗

Recent results on Mars and Venus; Proceedings of Symposium 3 and the Topical Meetings of the Interdisciplinary Scientific Commission C (Meeting C1) and D (Meeting D1) of the COSPAR 28th Plenary Meeting, The Hague, Netherlands, June 25-July 6, 1990

In this volume, latest results on Mars and Phobos studies are discussed along with recent results on Venus and on Martian plasma environment. Papers are presented on the characteristics of aerosol phenomena in Martian atmosphere from KRFM-experiment data, Phobos map and Phobos globe, submicron-sized dust grains in the Martian environment, remote sensing of Venus atmospheric dynamics, the latitude structure of upper clouds of Venus, and Venus thermospheric response to short-term solar variations. Attention is also given to a comparison between the bow shocks and magnetotails of Venus and Mars, comparative studies of the solar wind interaction with weakly magnetized planets, the magnetic field environment of Mars as studied by Phobos-2, waves and cold plasmas near Mars, and multiple-ion effects at Martian plasma boundaries.

Shorthill, R. W.↗

The Surface Atmosphere Integrated Field Laboratory (SAIL) Campaign

The science of mountainous hydrology spans the atmosphere through the bedrock and inherently crosses physical and disciplinary boundaries: land-atmosphere interactions in complex terrain enhance clouds and precipitation, while watersheds retain and release water over a large range of spatial and temporal scales. Limited observations in complex terrain challenge efforts to improve predictive models of the hydrology in the face of rapid changes. The Upper Colorado River exemplifies these challenges, especially with ongoing mismatches between precipitation, snowpack, and discharge. Consequently, the U.S. Department of Energy’s (DOE) Atmospheric Radiation Measurement (ARM) user facility has deployed an observatory to the East River Watershed near Crested Butte, Colorado between September 2021 and June 2023 to measure the main atmospheric drivers of water resources, including precipitation, clouds, winds, aerosols, radiation, temperature and humidity. This effort, called the Surface Atmosphere Integrated Field Laboratory (SAIL), is also working in tandem with DOE-sponsored surface and subsurface hydrologists and other federal, state, and local partners. SAIL data can be benchmarks for model development by producing a wide range of observational information on precipitation and its associated processes, including those processes that impact snowpack sublimation and redistribution, aerosol direct radiative effects in the atmosphere and in the snowpack, aerosol impacts on clouds and precipitation, and processes controlling surface fluxes of energy and mass. Preliminary data from SAIL’s first year showcase the rich information content in SAIL’s many data-streams and support testing hypotheses that will ultimately improve scientific understanding and predictability of Upper Colorado River hydrology in 2023 and beyond.

54 ENVIRONMENTAL SCIENCES↗

TRACER-Vertical Profile of Aerosol in Convective System (TRACER-VPACS) Field Campaign Report

We investigated physicochemical properties of aerosol at different altitudes during the U.S. Department of Energy (DOE)’s Atmospheric Radiation Measurement (ARM) user facility Tracking Aerosol Convection Interactions Experiment (TRACER). We used ARM’s tethered balloon system (TBS) and multi-modal offline analysis techniques available at DOE’s Environmental Molecular Sciences Laboratory (EMSL) at Pacific Northwest National Laboratory (PNNL) and at the Advanced Light Source (ALS) at the Lawrence Berkley National Laboratory (LBNL). The main scientific aim of this project was to understand the influence of the vertical profile of aerosol composition on the properties of deep convective clouds. The effect of aerosol properties on convective activity is still poorly understood and debated. For example, previous studies suggested that higher concentration of hygroscopic aerosol may lead to lower collection efficiency and eventually delay in onset of precipitation and total amount of precipitation. However, some observations suggested that increased aerosol concentration may result in vigorous convection and a higher amount of precipitation. In addition, the radiative forcing of the ambient aerosol is strongly influenced by the vertical distribution of aerosols and their chemical composition, and not well constrained in climate models. The estimation of the indirect effect of aerosol also has a significant uncertainty due to the spatial variation of the aerosol, especially at the cloud base. Detailed size-resolved chemical composition studies of aerosol and their microphysical properties, along with in situ measurements from ARM’s mobile facilities, help to improve our understanding of the role of aerosol in deep convective cloud formation over a broad range of environmental thermodynamic and aerosol conditions.

54 ENVIRONMENTAL SCIENCES↗