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Stratospheric CCN sampling program

When Mt. St. Helens produced several major eruptions in the late spring of 1980, there was a strong interest in the characterization of the cloud condensation nuclei (CCN) activity of the material that was injected into the troposphere and stratosphere. The scientific value of CCN measurements is two fold: CCN counts may be directly applied to calculations of the interaction of the aerosol (enlargement) at atmospherically-realistic relative humidities or supersaturations; and if the chemical constituency of the aerosol can be assumed, the number-versus-critical supersaturation spectrum may be converted into a dry aerosol size spectrum covering a size region not readily measured by other methods. The sampling method is described along with the instrumentation used in the experiments.

Rogers, C. F.↗

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign and much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a) two well-characterized source of soot particles and (b) a flow reactor for controlled OH and/or O3 oxidation of relevant gas phase species to produce well-characterized SOA particles. After formation, the aerosol particles are subjected to physical and chemical processes that simulate aerosol growth and aging. A suite of instruments in our laboratory is used to characterize the physical and chemical properties of aerosol particles before and after processing. The Time of Flight Aerosol Mass Spectrometer (ToF-AMS) together with a Scanning Mobility Particle Sizer (SMPS) measures particle mass, volume, density, composition (including black carbon content), dynamic shape factor, and fractal dimension. The–ToF-AMS was developed at ARI with Boston College participation. About 120 AMS instruments are now in service (including 5 built for DOE laboratories) performing field and laboratory studies world-wide. Other major instruments include a thermal denuder, two Differential Mobility Analyzers (DMA), a Cloud Condensation Nuclei Counter (CCN), a Thermal desorption Aerosol GC/MS (TAG) and the new Soot Particle Aerosol Mass Spectrometer (SP-AMS). Optical instrumentation required for the studies have been brought to our laboratory as part of ongoing and planned collaborative projects with colleagues from DOE, NOAA and university laboratories. Optical instruments that will be utilized include a Photoacoustic Spectrometer (PAS), a Cavity Ring Down Aerosol Extinction Spectrometer (CRD-AES), a Photo Thermal Interferometer (PTI), a new 7-wavelength Aethalometer and a Cavity Attenuated Phase Shift Extinction Monitor (CAPS). These instruments are providing aerosol absorption, extinction and scattering coefficients at a range of atmospherically relevant wavelengths. During the past two years our work has continued along the lines of our original proposal. We report on 12 completed and/or continuing projects conducted during the period 08/14 to 0814/2015. These projects are described in 17 manuscripts published in refereed journals.

54 ENVIRONMENTAL SCIENCES↗

Three-Dimensional Modeling of the Explicit Chemistry of Organic Aerosols: Formation, Removal, and Comparison with Observations

The major goals of the project were to further our understanding of the formation of secondary organic aerosols (SOA) from major anthropogenic and biogenic precursors, and to evaluate the GECKO-A chemistry model in the context of three DOE-led field campaigns (GoAmazon, BBOP, and HI-SCALE) with the long-term objective of improving the treatment of organic gases and particles in three-dimensional regional and global models. The three field campaigns were selected to evaluate and improve specific aspects of GECKO-A: (i) GoAmazon to help quantify interactions of biogenic and anthropogenic emissions; (ii) BBOP to predict the UV-visible absorption properties of biomass burning aerosols (brown carbon) from explicit molecular properties; and (iii) HI-SCALE to evaluate new model components that include aqueous (cloud) processing of organic gases and aerosols.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ground-based SMART-COMMIT Measurements for Studying Aerosol and Cloud Properties

From radiometric principles, it is expected that the retrieved properties of extensive aerosols and clouds from reflected/emitted measurements by satellite (and/or aircraft) should be consistent with those retrieved from transmitted/emitted radiance observed at the surface. Although space-borne remote sensing observations cover large spatial domain, they are often plagued by contamination of surface signatures. Thus, ground-based in-situ and remote-sensing measurements, where signals come directly from atmospheric constituents, the sun, and/or the Earth-atmosphere interactions, provide additional information content for comparisons that confirm quantitatively the usefulness of the integrated surface, aircraft, and satellite data sets. The development and deployment of SMARTCOMMIT (Surface-sensing Measurements for Atmospheric Radiative Transfer - Chemical, Optical & Microphysical Measurements of In-situ Troposphere) mobile facilities are aimed for the optimal utilization of collocated ground-based observations as constraints to yield higher fidelity satellite retrievals and to determine any sampling bias due to target conditions. To quantify the energetics of the surface-atmosphere system and the atmospheric processes, SMART-COMMIT instruments fall into three categories: flux radiometer, radiance sensor and in-situ probe. In this paper, we will demonstrate the capability of SMART-COMMIT in recent field campaigns (e.g., CRYSTAL-FACE, UAE 2, BASEASIA, NAMMA) that were designed and executed to study the compelling variability in temporal scale of both anthropogenic and natural aerosols (e.g., biomass-burning smoke, airborne dust) and cirrus clouds. We envision robust approaches in which well-collocated ground-based measurements and space-borne observations will greatly advance our knowledge of extensive aerosols and clouds.

Tsay, Si-Chee↗

A Simple Model of Global Aerosol Indirect Effects

Most estimates of the global mean indirect effect of anthropogenic aerosol on the Earth’s energy balance are from simulations by global models of the aerosol lifecycle coupled with global models of clouds and the hydrologic cycle. Extremely simple models have been developed for integrated assessment models, but lack the flexibility to distinguish between primary and secondary sources of aerosol. Here a simple but more physically-based model expresses the aerosol indirect effect using analytic representations of droplet nucleation, cloud and aerosol vertical structure, and horizontal variability in cloud water and aerosol concentration. Although the simple model is able to produce estimates of aerosol indirect effects that are comparable to those from some global aerosol models using the same global mean aerosol properties, the estimates are found to be sensitive to several uncertain parameters, including the preindustrial cloud condensation nuclei concentration, primary and secondary anthropogenic emissions, the size of the primary particles, the fraction of the secondary anthropogenic emissions that accumulates on the coarse mode, the fraction of the secondary mass that forms new particles, and the sensitivity of liquid water path to droplet number concentration. Aerosol indirect effects are surprisingly linear in emissions. This simple model provides a much stronger physical basis for representing aerosol indirect effects than previous representations in integrated assessment models designed to quickly explore the parameter space of emissions-climate interactions. The model also produces estimates that depend on parameter values in ways that are consistent with results from detailed global aerosol-climate simulation models.

aerosol↗

Sea Breeze Influence on Aerosols and Convection in the Southeastern US

The goal of this research is to describe the inland penetrating sea breeze and interactions with atmospheric phenomena across multiple scales, thereby establishing a baseline of understanding. The land-ocean-atmosphere interface in the southeastern US drives regional sea breeze circulations that impact clouds, convection, and precipitation. We analyzed a variety of atmospheric observations to identify the characteristics and frequency of sea breezes. Sea breezes were identified all along the southeastern Atlantic coast (63% of days from March to September in 2019) at times impacting large areas of the southeastern US. They were found to penetrate inland to the Savannah River Site on about 27% of all days during the typical sea breeze season (March to October) from 2015 to 2020, often leaving a residual layer the following day. Future work focuses on modeling studies, analysis of additional data, and climate impacts on sea breezes.

58 GEOSCIENCES↗

Interaction of Burning Metal Particles

Multiple particle/droplet flames are ubiquitous in practical combustion systems, and thus the flame interaction processes are of great practical importance. This explains the strong current interest in interactive combustion phenomena. This research is aimed at the investigation of combustion parameters of microgravity model aerosols: relatively large uniform metal particles aerosolized in microgravity environment. An experiment consisting of creation and ignition of a metal multiparticle system in microgravity and high-speed video-recording of the combustion events will produce visual records of the development of individual particle flames, their interactions and the particle motion they induce simultaneously with the observation of the entire aerosol combustion process. Frame by frame analysis of the video-images taken using a high-speed movie camera will allow one to determine particle brightness temperatures and the decrease in particle diameter during combustion. Analysis of the experimental results and comparison with the results of single metal particle combustion experiments, conducted under similar microgravity conditions in the framework of a parallel program, will establish the relationship between single and multiple particle burning rates and combustion temperatures, concentrations at which the flame substructure forms rather than individual particle flames, efficiency of radiative heat transfer in metal aerosol combustion, what is the role of electrostatic forces in structuring the flame and the effect of that structure on the flame propagation rate. Although some details of fine particle aerosol clouds, such as the kinetics limited burning rate, radiative heat transfer in a system with a high specific surface, particle induced turbulence, etc., will probably not be very well simulated in the planned experiments, they are relatively well understood and can be accounted for using an adequate individual particle combustion model. On the other hand, the unknown particle interaction phenomena to be studied in this research program are generic and can be readily projected onto a cloud combustion model which would also incorporate a correction for particle size.

Dreizin, Edward L.↗

Overview of the MOSAiC expedition—Atmosphere

With the Arctic rapidly changing, the needs to observe, understand, and model the changes are essential. To support these needs, an annual cycle of observations of atmospheric properties, processes, and interactions were made while drifting with the sea ice across the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition from October 2019 to September 2020. An international team designed and implemented the comprehensive program to document and characterize all aspects of the Arctic atmospheric system in unprecedented detail, using a variety of approaches, and across multiple scales. These measurements were coordinated with other observational teams to explore cross-cutting and coupled interactions with the Arctic Ocean, sea ice, and ecosystem through a variety of physical and biogeochemical processes. This overview outlines the breadth and complexity of the atmospheric research program, which was organized into 4 subgroups: atmospheric state, clouds and precipitation, gases and aerosols, and energy budgets. Atmospheric variability over the annual cycle revealed important influences from a persistent large-scale winter circulation pattern, leading to some storms with pressure and winds that were outside the interquartile range of past conditions suggested by long-term reanalysis. Similarly, the MOSAiC location was warmer and wetter in summer than the reanalysis climatology, in part due to its close proximity to the sea ice edge. The comprehensiveness of the observational program for characterizing and analyzing atmospheric phenomena is demonstrated via a winter case study examining air mass transitions and a summer case study examining vertical atmospheric evolution. Overall, the MOSAiC atmospheric program successfully met its objectives and was the most comprehensive atmospheric measurement program to date conducted over the Arctic sea ice. The obtained data will support a broad range of coupled-system scientific research and provide an important foundation for advancing multiscale modeling capabilities in the Arctic.

54 ENVIRONMENTAL SCIENCES↗

Integrating Cloud Processes in the Community Atmosphere Model, Version 5.

This paper provides a description on the parameterizations of global cloud system in CAM5. Compared to the previous versions, CAM5 cloud parameterization has the following unique characteristics: (1) a transparent cloud macrophysical structure that has horizontally non-overlapped deep cumulus, shallow cumulus and stratus in each grid layer, each of which has own cloud fraction, mass and number concentrations of cloud liquid droplets and ice crystals, (2) stratus-radiation-turbulence interaction that allows CAM5 to simulate marine stratocumulus solely from grid-mean RH without relying on the stability-based empirical empty stratus, (3) prognostic treatment of the number concentrations of stratus liquid droplets and ice crystals with activated aerosols and detrained in-cumulus condensates as the main sources and evaporation-sedimentation-precipitation of stratus condensate as the main sinks, and (4) radiatively active cumulus. By imposing consistency between diagnosed stratus fraction and prognosed stratus condensate, CAM5 is free from empty or highly-dense stratus at the end of stratus macrophysics. CAM5 also prognoses mass and number concentrations of various aerosol species. Thanks to the aerosol activation and the parameterizations of the radiation and stratiform precipitation production as a function of the droplet size, CAM5 simulates various aerosol indirect effects associated with stratus as well as direct effects, i.e., aerosol controls both the radiative and hydrological budgets. Detailed analysis of various simulations revealed that CAM5 is much better than CAM3/4 in the global performance as well as the physical formulation. However, several problems were also identifed, which can be attributed to inappropriate regional tuning, inconsistency between various physics parameterizations, and incomplete model physics. Continuous efforts are going on to further improve CAM5.

CAM5↗

PACE Technical Report Series, Volume 11: The PACE Postlaunch Airborne eXperiment (PACE-PAX)

The Plankton, Aerosol, Cloud, ocean Ecosystem (PACE; https://pace.gsfc.nasa.gov) mission is NASA's latest and greatest effort to study the ocean-atmosphere system and build upon the legacy of previous satellite missions that have revolutionized our understanding of our home planet. By using advanced radiometric and polarimetric instruments to measure ocean color and key atmospheric variables, PACE aims to provide new insights into the complex interactions between the ocean, atmosphere, and biosphere. This information will be critical for improving our ability to model and predict changes in the Earth's climate, as well as to manage and conserve our planet's valuable natural resources. Performance assessments and science data product validation is a critical process for any Earth Science space-borne mission, as it involves assessing and verifying the quality of the data products generated by the mission while it is in orbit, as well as assigning uncertainties to these retrievals. More specifically, validation efforts are essential for assessing the accuracy of instrument data and the derived science products across varied spatial and temporal scales and ensuring their reliability and consistency with the mission's scientific goals and objectives. The overall plan for validation of PACE data is described in “PACE Science Data Product Validation Plan” (see, e.g., https://pace.gsfc.nasa.gov), and among range of post-launch activities, it describes the need and requirements for a post-launch airborne field campaign in support of PACE validation. This volume outlines the plans and requirements of the PACE Postlaunch Airborne eXperiment (PACE-PAX). The main goal of PACE-PAX is to gather validation and assessment data for the PACE mission, using a variety of airborne and ground-based assets. These assets will be coordinated to obtain complementary measurements of key ocean and atmospheric variables, such as ocean color, aerosols, and clouds. By collecting data from multiple sources, PACE-PAX will help to validate and refine the data products generated by the PACE mission, as well as to identify any potential errors or biases in the measurements. This will be essential for ensuring the accuracy and reliability of the PACE data products, and for maximizing the scientific value of the mission.

Kirk D Knobelspiesse↗

A Downscaling Analysis of the Urban Influence on Rainfall: TRMM Satellite Component AMS Conference on Satellite Meteorology and Oceanography

A recent publication by Shepherd et al. (2002) demonstrated the feasibility of using TRMM precipitation radar (PR) estimates to identify precipitation anomalies caused by urbanization. The approach is particularly useful for investigating this global process because TRMM data span large portions of the globe and comprise an extended temporal dataset. Recent literature suggests that urbanized regions of Houston, Texas may be influencing lightning and precipitation formation over and downwind of the city. Possible mechanisms include: (1) enhanced convergence through interactions between the sea breeze, Galveston bay breeze, and urban heat island circulations, (2) enhanced convergence due to increased surface roughness over the city and/or destabilization of the boundary layer by the UHI, or (3) enhanced cloud condensation nuclei due to urban and industrial aerosol sources. In this study, a downscaling analysis of spatial and temporal trends in rainfall around the Houston Area is being conducted. The downscaling analysis concept involves identifying and quantifying urban rainfall anomalies at progressively smaller spatial and temporal scales using the TRMM satellite, ground-based radar, and a dense network of rain gauges. The goal is to test the hypothesis that the Houston urban district and regions in the climatological downwind region of the city exhibit enhanced rainfall amounts relative to the climatological upwind regions. TRMM was launched in 1997 and currently operates in a low-inclination (35 deg), non-sun-synchronous orbit at an altitude of 402 km (350 km prior to August 2001). The satellite analysis follows the methodologies described in Shepherd et al. (2002). Nearly five years of TRMM PR-derived mean monthly rainfall estimates are utilized to produce annual and warm season isohyetal analyses around Houston. Early results indicate that rainfall rates (mm/h) for the entire period are largest within 100 km northeast and east of Houston (e.g. the "hypothesized downwind region"). The mean rainfall rate over the Houston urban center is 30.5% larger than the upwind control region. The mean rainfall rate in the downwind region is 34.4% larger than the upwind region. An analysis of a parameter called the urban rainfall ratio (URR) illustrates that 65% (88%) of the satellite-derived rainfall rates in the downwind (upwind control) region are greater (less) than the mean background rainfall rate of the entire study region. When the data is stratified by summer months from 1998 to 2001 (June-August), even greater influence over and downwind of the urban area is observed in the statistics. This result is consistent with published reports of urban-generated rainfall being more prevalent in the warm season. The research demonstrates that the evolving TRMM satellite climatology is a credible way to detect mesoscale precipitation signatures that may be linked to urbanization. Early results also corroborate recent findings on Houston-induced convection/drainfall anomalies. Burian and Shepherd will report on other aspects of the downscaling analysis in future forums, but early rain gauge results are consistent with the satellite-based observations.

Shepherd, J. Marshall↗

Biomass-burning Aerosols in South East-Asia: Smoke Impact Assessment(BASE-ASIA)

Biomass burning has been a regular practice for land clearing and land conversion in many countries, especially in Africa, South America, and South East Asia. Significant global sources of greenhouse gases (e.g., CO2, CH4), chemically active gases (e.g., NO, CO, HC, CH3Br), and atmospheric aerosols are produced by biomass-burning processes, which influence the Earth-atmosphere energetics and hence impact both global climate and tropospheric chemistry. Some gases and aerosols can serve as active cloud condensation nuclei, which play important role in determining the net radiation budget, precipitation rate, and cloud lifetime. Biomass burning also affects the biogeochemical cycling of nitrogen and carbon compounds from the soil to the atmosphere; the hydrological cycle (i.e., run off and evaporation); the reflectivity and emissivity of the land; and the stability of ecosystems and ecosystem biodiversity. Compared to Africa and South America, the climatology in South East Asia reveals quite different characteristics, showing distinct large-scale smoke and cloud sources and interaction regimes. The fresh water distribution in this region is highly dependent on monsoon rainfall; in fact, the predictability of the tropical climate system is much reduced during the boreal spring, which is associated with the peak season of biomass burning activities. Estimating the burning fuel (e.g., bark, branches, and wood), an important part of studying regional carbon cycle, may rely on utilizing a wide range of distinctive spectral features in the shortwave and longwave regions. Therefore, to accurately assess the impact of smoke aerosols in this region requires continuous observations from satellites, aircraft, networks of ground-based instruments and dedicated field experiments. A new initiative will be proposed and discussed.

Tsay, Si-Chee↗

Laboratory and field studies of ice-nucleating particles from open-lot livestock facilities in Texas

Abstract. In this work, an abundance of ice-nucleating particles (INPs) from livestock facilities was studied through laboratory measurements from cloud-simulation chamber experiments and field investigation in the Texas Panhandle. Surface materials from two livestock facilities, one in the Texas Panhandle and another from McGregor, Texas, were selected as dust proxies for laboratory analyses. These two samples possessed different chemical and biological properties. A combination of aerosol interaction and dynamics in the atmosphere (AIDA) measurements and offline ice spectrometry was used to assess the immersion freezing mode ice nucleation ability and efficiency of these proxy samples at temperatures above −29 ∘C. A dynamic filter processing chamber was also used to complement the freezing efficiencies of submicron and supermicron particles collected from the AIDA chamber. For the field survey, periodic ambient particle sampling took place at four commercial livestock facilities from July 2017 to July 2019. INP concentrations of collected particles were measured using an offline freezing test system, and the data were acquired for temperatures between −5 and −25 ∘C. Our AIDA laboratory results showed that the freezing spectra of two livestock dust proxies exhibited higher freezing efficiency than previously studied soil dust samples at temperatures below −25 ∘C. Despite their differences in composition, the freezing efficiencies of both proxy livestock dust samples were comparable to each other. Our dynamic filter processing chamber results showed on average approximately 50 % supermicron size dominance in the INPs of both dust proxies. Thus, our laboratory findings suggest the importance of particle size in immersion freezing for these samples and that the size might be a more important factor for immersion freezing of livestock dust than the composition. From a 3-year field survey, we measured a high concentration of ambient INPs of 1171.6 ± 691.6 L−1 (average ± standard error) at −25 ∘C for aerosol particles collected at the downwind edges of livestock facilities. An obvious seasonal variation in INP concentration, peaking in summer, was observed, with the maximum at the same temperature exceeding 10 000 L−1 on 23 July 2018. The observed high INP concentrations suggest that a livestock facility is a substantial source of INPs. The INP concentration values from our field survey showed a strong correlation with measured particulate matter mass concentration, which supports the importance of size in ice nucleation of particles from livestock facilities.

58 GEOSCIENCES↗

Cloud Ozone Dust Imager (CODI): Investigation and Technical Plan - Volume 1

The Cloud Ozone Dust Imager (CODI) is proposed to investigate the current climatic balance of the Mars atmosphere, with particular emphasis on the important but poorly understood roles which dust and water ice aerosols play in this balance. The large atmospheric heating (20-50 K) resulting from global dust storms around Mars perihelion is well recognized. However, groundbased observations of Mars atmospheric temperatures, water vapor, and clouds since the Viking missions have identified a much colder, cloudier atmosphere around Mars aphelion that may prove as important as global dust storms in determining the interannual and long-term behavior of the Mars climate. The key climate issues CODI is designed to investigate are: 1) the degree to which non-linear interactions between atmospheric dust heating, water vapor saturation, and cloud nucleation influence the seasonal and interannual variability of the Mars atmosphere, and 2) whether the strong orbital forcing of atmospheric dust loading, temperatures and water vapor saturation determines the long-term balance of Mars water, as reflected in the north-south hemispheric asymmetries of atmospheric water vapor and polar water ice abundances. The CODI experiment will measure the daily, seasonal and (potentially) interannual variability of atmospheric dust and cloud opacities, and the key physical properties of these aerosols which determine their role in the climate cycles of Mars. CODI is a small (1.2 kg), fixed pointing camera, in which four wide-angle (+/- 70 deg) lenses illuminate fixed filters and CCD arrays. Simultaneous sky/surface imaging of Mars is obtained at an angular resolution of 0.28 deg/pixel for wavelengths of 255, 336, 502, and 673 nm (similar to Hubble Space Telescope filters). These wavelengths serve to measure atmospheric ozone (255 and 336 nm), discriminate ice and dust aerosols (336 and 673 nm), and construct color images (336, 502, and 673 nm). The CODI images are detected on four 512 x 512 pixel arrays, as partitioned on two 1024 x 1024 CCD's operated in frame transfer mode. The center of the CODI field-of-view is canted 40 deg from the zenith direction to obtain sky brightness measurements and a 20 deg surface field-of-view. Daily image observations will be conducted when the Sun is greater than or equal to 5 deg outside the edge of the CODI field-of-view, and twilight and nighttime imaging will obtained on a weekly basis. The 673 nm channel includes a polarizer wheel to obtain sky/surface polarimetry. A dust cover protects the entire lens assemblies of all four CODI channels. This opaque dust cover, which is normally opened for CODI imaging, includes a small fixed mirror and transparent window positioned above the 673 nm lens, to redirect the 673 nm field-of-view to the surface for descent imaging. Fixed pointing, internal data buffering, low operating power (2-4 W for less than or equal to 30 seconds), selective data transmission, and simple operational characteristics of the CODI experiment place minimum resource and operational demands on the Mars Surveyor 1998 lander. The CODI science goals are optimized for, but not restricted to, a low-latitude landing site (20 deg S-30 deg N). The primary CODI measurement objectives are the opacities, wave forms, particle properties (size, shape, and alignment), and heights of clouds; the opacities, particle properties, and vertical distribution of dust; and the opacity and vertical distribution of ozone. The variability of cloud, ozone, and dust opacities will be determined on diurnal, daily, and seasonal timescales. Wind velocities will be determined from cloud motions and wave characteristics; and the temporal variability of atmospheric water vapor, with limited altitude information, will be inferred from the CODI ozone observations. Secondary measurement objectives include limited descent imaging capability, surface uv-visible photometry and polarimetry, photochemistry, and meteorite infall rates.

Clancy, R. Todd↗

A three-dimensional sectional representation of aerosol mixing state for simulating optical properties and cloud condensation nuclei

Light absorption by black carbon (BC) particles emitted from fossil fuel combustion depends on the how thickly they are coated with non-refractory species such as ammonium, sulfate, nitrate, organics, and water. The cloud condensation nuclei (CCN) activation property of a particle depends on its dry size and the hygroscopicities of all the individual species mixed together. It is therefore necessary to represent both size and mixing state of aerosols to reliably predict their climate-relevant properties in atmospheric models. Here we describe and evaluate a novel sectional framework in the Model for Simulating Aerosol Interactions and Chemistry, referred to as MOSAIC-mix, that represents the mixing state by resolving aerosol dry size (D dry ), BC dry mass fraction (w BC ), and hygroscopicity (κ). Using ten idealized urban plume scenarios in which different types of aerosols evolve over 24 hours under a range of atmospherically relevant environmental conditions, we examine errors in CCN concentrations and optical properties with respect to a more explicit aerosol mixing state representation. We find that only a small number of w BC and κ bins are needed to achieve significant reductions in the errors, and propose a configuration consisting of 24 D dry bins, 2 w BC bins, and 2 κ bins that gives 24-hour average errors of about 5% or less in CCN concentrations and optical properties, 3-4 times lower than those from size-only-resolved simulations. Here, these results show that MOSAIC-mix is suitable for use in regional and global models to examine the effects of evolving aerosol mixing states on aerosol-radiation-cloud feedbacks.

54 ENVIRONMENTAL SCIENCES↗

The significant impact of aerosol vertical structure on lower atmosphere stability and its critical role in aerosol–planetary boundary layer (PBL) interactions

The aerosol–planetary boundary layer (PBL) interaction was proposed as an important mechanism to stabilize the atmosphere and exacerbate surface air pollution. Despite the tremendous progress made in understanding this process, its magnitude and significance still have large uncertainties and vary largely with aerosol distribution and meteorological conditions. In this study, we focus on the role of aerosol vertical distribution in thermodynamic stability and PBL development by jointly using micropulse lidar, sun photometer, and radiosonde measurements taken in Beijing. Despite the complexity of aerosol vertical distributions, cloud-free aerosol structures can be largely classified into three types: well-mixed, decreasing with height, and inverse structures. The aerosol–PBL relationship and diurnal cycles of the PBL height and PM 2.5 associated with these different aerosol vertical structures show distinct characteristics. The vertical distribution of aerosol radiative forcing differs drastically among the three types, with strong heating in the lower, middle, and upper PBL, respectively. Such a discrepancy in the heating rate affects the atmospheric buoyancy and stability differently in the three distinct aerosol structures. Absorbing aerosols have a weaker effect of stabilizing the lower atmosphere under the decreasing structure than under the inverse structure. As a result, the aerosol–PBL interaction can be strengthened by the inverse aerosol structure and can be potentially neutralized by the decreasing structure. Moreover, aerosols can both enhance and suppress PBL stability, leading to both positive and negative feedback loops. This study attempts to improve our understanding of the aerosol–PBL interaction, showing the importance of the observational constraint of aerosol vertical distribution for simulating this interaction and consequent feedbacks.

54 ENVIRONMENTAL SCIENCES↗

Uncertain role of clouds in shaping summertime atmosphere-sea ice connections in reanalyses and CMIP6 models

Downwelling longwave radiation (DLR) driven by the atmospheric and cloud conditions in the troposphere is suggested to be a dominant factor to determine the summertime net surface energy budget over the Arctic Ocean and thus plays a key role to shape the September sea ice. We use reanalyses and the self-organizing map (SOM) method to distinguish CMIP6 model performance in replicating the observed strong atmosphere-DLR connection. We find all models can reasonably simulate the linkage between key atmosphere variables and the clear sky DLR but behave differently in replicating the atmosphere-DLR connection due to cloud forcing. In ERA5 and strongly coupled models, tropospheric high pressure is associated with decreased clouds in the mid- and high-levels and increased clouds near the surface. This out-of-phase structure indicates that DLR cloud forcing is nearly neutral, making the clear sky DLR more important to bridge JJA circulation to late-summer sea ice. In MERRA-2 and weakly coupled models, tropospheric clouds display a vertically homogeneous reduction; the cloud DLR is thus strongly reduced due to the cooling effect, which partially cancels out the clear sky DLR and makes the total DLR less efficient to translate circulation forcing to sea ice. The differences of cloud vertical distribution in CMIP6 appear to be differentiated by circulation related relative humidity. Therefore, a better understanding of the discrepancy of different reanalyses and remote sensing products is critical to comprehensively evaluate simulated interactions among circulation, clouds, sea ice and energy budget at the surface in summer.

54 ENVIRONMENTAL SCIENCES↗

Observed Variability in Convective Cell Characteristics and Near-Storm Environments across the Sea- and Bay-Breeze Fronts in Southeast Texas

Abstract During the DOE Atmospheric Radiation Measurement (ARM) Tracking Aerosol Convection Interactions Experiment (TRACER) IOP spanning June–September 2022, two fixed ARM sites and a mobile team concurrently sampled the airmass heterogeneity across sea- and bay-breeze fronts around the greater Houston metropolitan region. Here, we quantify the spatiotemporal variability between maritime (coastal/bay side of breeze fronts) and continental (inland side of breeze fronts) air masses over 15 IOP days characterized by strong sea-breeze forcing. We analyze environmental profile data from 177 radiosondes and use S- and C-band radar data to track and quantify the variability in attributes of more than 2300 shallow and transitioning cells across different air masses. The composite analysis of environmental profiles indicates that during the early afternoon, the sea-breeze maritime air mass exhibits lower convective available potential energy (CAPE) than the bay-breeze maritime air mass. As the sea breeze advances inland with time, CAPE within the maritime air mass exceeds that of the continental air mass to the north of the breeze fronts. In general, maritime cells have a larger mean composite reflectivity and cell widths than continental cells; however, the response varies between shallow and transitioning cells. Mean composite 20-dB Z echo-top heights, however, are similar across air masses for both shallow and transitioning cells. The continental and maritime inflow air mass for transitioning cells has significantly different mean values for mixed-layer entrainment CAPE, lifted condensation level, level of free condensation, boundary layer depth, and diluted equilibrium level. For shallow cells, only total precipitable water shows a significant difference. Significance Statement The greater Houston metropolitan area is a natural laboratory for understanding the individual impacts of background meteorology and aerosols on convective clouds. Due to its proximity to the Gulf Coast and Galveston Bay, the Houston region experiences a diurnal precipitation cycle in the summer, driven by convection triggered from sea- and bay-breeze fronts. These fronts act as a boundary between air masses with distinct thermodynamic and environmental characteristics. Convergence along these fronts and interactions between storm outflow and the fronts facilitate convection initiation in different mesoscale air masses. This study quantifies the heterogeneity among these air masses while investigating their influence on cloud microphysics. We find that the effect of airmass heterogeneity is more pronounced for the bulk microphysical properties in shallow clouds.

Sharma, Milind↗