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Radiative Characteristics of Clouds Embedded in Smoke Derived from Airborne Multiangular Measurements

Clouds in the presence of absorbing aerosols result in their apparent darkening, observed at the top of atmosphere (TOA), which is associated with the radiative effects of aerosol absorption. Owing to the large radiative effect and potential impacts on regional climate, above-cloud aerosols have recently been characterized in multiple satellite-based studies. While satellite data are particularly useful in showing the radiative impact of above-cloud aerosols at the TOA, recent literature indicates large uncertainties in satellite retrievals of above-cloud aerosol optical depth (AOD) and single scattering albedo (SSA), which are among the most important parameters in the assessment of associated radiative effects. In this study, we analyze radiative characteristics of clouds in the presence of wildfire smoke using airborne data primarily from NASA's Cloud Absorption Radiometer, collected during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites campaign in Canada during the 2008 summer season. We found a strong positive reflectance (R) gradient in the UV-visible (VIS)-near infrared (NIR) spectrum for clouds embedded in dense smoke, as opposed to an (expected) negative gradient for cloud-free smoke and a flat spectrum for smoke-free cloud cover. Several cases of clouds embedded in thick smoke were found, when the aircraft made circular/spiral measurements, which not only allowed the complete characterization of angular distribution of smoke scattering but also provided the vertical distribution of smoke and clouds (within 0.5-5 km). Specifically, the largest darkening by smoke was found in the UV/VIS, with R(sub 0.34 microns) reducing to 0.2 (or 20%), in contrast to 0.8 at NIR wavelengths (e.g., 1.27 microns). The observed darkening is associated with large AODs (0.5-3.0) and moderately low SSA (0.85-0.93 at 0.53 microns), resulting in a significantly large instantaneous aerosol forcing efficiency of 254 +/- 47 W/sq m/τ. Our observations of smoke-cloud radiative interactions were found to be physically consistent with theoretical plane-parallel 1-D and Monte Carlo 3-D radiative transfer calculations, capturing the observed gradient across UV-VIS-NIR. Results from this study offer insights into aerosol-cloud radiative interactions and may help in better constraining satellite retrieval algorithms.

absorbing aerosols↗

ARM: KASACRCFRQC

The Ka-Band Scanning ARM Cloud Radar (KASACR) records cloud properties. ARM's scanning cloud radars are dual-frequency, dual-polarization Doppler radars mounted on a common scanning pedestal. Each pedestal includes a Ka-band radar (2kW peak power) and the deployment location determines whether the second radar is a W-band (1.7 kW peak power) or an X-band (20 kW peak power). Beamwidths for Ka-bands paired with W-bands are roughly matched at 0.3 degrees. The X-band beamwidth is approximately 1 degree. Due to the narrow antenna beamwidth, ARM’s scanning cloud radars use scanning strategies unlike typical weather radars. Rather than focusing on plan position indicator, or PPI, scans, the KASACR uses range height indicator, or RHI, scans at numerous azimuths to obtain cloud volume data. Measurements collected with the KASACR are copolar and cross-polar radar reflectivity, Doppler velocity, spectra width and spectra when not scanning, and linear depolarization ratio. KASACR data from the 2018–2019 Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign in Argentina are now available as b1-level products. Building on the original CACTI operational data, the b1-level products feature improved data quality resulting from extensive analyses and corrections. The data are cross-calibrated to a common point, datastreams are corrected for operational issues that occurred during the campaign, and several data quality masks and basic derived products are incorporated. For more information, read the CACTI radar b1-level processing report.

54 ENVIRONMENTAL SCIENCES↗

Influences of the South American Low-Level Jet on the Convective Environment in Central Argentina Using a Convection-Permitting Simulation

This study documents the spatial and temporal distribution of the South American low-level jet (SALLJ) and quantifies its impact on the convective environment using a 6.5-month convection-permitting simulation during the Remote Sensing of Electrification, Lightning, And Mesoscale/Microscale Processes with Adaptive Ground Observations and Clouds, Aerosols, and Complex Terrain Interactions (RELAMPAGO-CACTI) campaigns. Overall, the simulation reproduces the observed SALLJ characteristics in central Argentina near the Sierras de Córdoba (SDC), a focal point for terrain-focused upscale growth. SALLJs most frequently occur in the summer with maxima to the northwest and east of the SDC and minima over the higher terrain. The shallower SALLJs (<1750 m) have a strong overnight skew, while the elevated jets are more equally spread throughout the day. SALLJ periods often have higher amounts of low-level moisture and instability compared to non-SALLJ periods, with these impacts increasing over time when the SALLJ is present and decreasing afterward. The SALLJ may enhance low-level wind shear magnitudes (particularly when accounting for the jet height); however, enhancement is somewhat limited due to the presence of speed shear in most situations. SALLJ periods are associated with low-level directional shear favorable for organized convection and an orientation of cloud-layer wind shear parallel to the terrain, which could favor upscale growth. A case study is shown in which the SALLJ influenced both the magnitude and direction of wind shear concurrent with convective upscale growth near the SDC. This study highlights the complex relationship between the SALLJ and its impacts during periods of widespread convection.

54 ENVIRONMENTAL SCIENCES↗

Convection-Permitting Ensembles of an Isolated Mountain Thunderstorm during RELAMPAGO/CACTI

Abstract The north–south-oriented Sierras de Córdoba (SDC) ridge in central Argentina is noted for initiating thunderstorms that may grow into intense mesoscale convective systems (MCSs). It also initiates more isolated, shorter-lived cells under weaker synoptic forcing. These cells are less impactful than MCSs but may be difficult to predict in convective-scale numerical weather prediction (NWP) due to their strong sensitivities to subgrid and partially resolved processes. To study the mechanisms and predictability of such cells, convection-permitting ensemble simulations were conducted of an isolated, diurnally forced SDC thunderstorm during Cloud, Aerosol, and Complex Terrain Interactions (CACTI)/Remote Sensing of Electrification, Lightning, and Mesoscale/Microscale Processes with Adaptive Ground Observations (RELAMPAGO). The rich observational data facilitated detailed ensemble verification, where dry biases in the surface energy balance and soil moisture were identified. These biases promoted rapid removal of convective inhibition and an early onset of precipitating cells over the SDC that were shallower and weaker than the observed cell. Correction, and then overcorrection, of the soil moisture bias in two successive ensembles was required to rectify the surface energy balance and improve the representation of the SDC cell. Nevertheless, substantial ensemble variability in convective precipitation was found, with some members producing more widespread convection than observed and others producing no deep convection at all. This variability was largely explained by a combination of thermodynamic and dynamic mechanisms, dominated by a positive sensitivity of convective precipitation to preconvective moist instability over the ridge. Secondary sensitivities were found to low-level upward mass flux and midlevel cross-barrier winds, the latter of which caused gravity waves with elevated downdrafts that tended to suppress incipient clouds.

Lopez, Andres [Department of Atmospheric and Ocean↗

A Public-Private-Acadmic Partnership to Advance Solar Power Forecasting

The National Center for Atmospheric Research (NCAR) is pleased to have led a partnership to advance the state-of-the-science of solar power forecasting by designing, developing, building, deploying, testing, and assessing the SunCast™ Solar Power Forecasting System. The project has included cutting edge research, testing in several geographically- and climatologically-diverse high penetration solar utilities and Independent System Operators (ISOs), and wide dissemination of the research results to raise the bar on solar power forecasting technology. The partners include three other national laboratories, six universities, and industry partners. This public-private-academic team has worked in concert to perform use-inspired research to advance solar power forecasting through cutting-edge research to advance both the necessary forecasting technologies and the metrics for evaluating them. The project has culminated in a year-long, full-scale demonstration of provide irradiance and power forecasts to utilities and ISOs to use in their operations. The project focused on providing elements of a value chain, beginning with the weather that causes a deviation from clear sky irradiance and progresses through monitoring and observations, modeling, forecasting, dissemination and communication of the forecasts, interpretation of the forecast, and through decision-making, which produces outcomes that have an economic value. The system has been evaluated using metrics developed specifically for this project, which has provided rich information on model and system performance. Research was accomplished on the very short range (0-6 hours) Nowcasting system as well as on the longer term (6-72 hour) forecasting system. The shortest range forecasts are based on observations in the field. The shortest range system, built by Brookhaven National Laboratory (BNL) and based on Total Sky Imagers (TSIs) is TSICast, which operates on the shortest time scale with a latency of only a few minutes and forecasts that currently go out to about 15 min. This project has facilitated research in improving the hardware and software so that the new high definition cameras deployed at multiple nearby locations allow discernment of the clouds at varying levels and advection according to the winds observed at those levels. Improvements over “smart persistence” are about 29% for even these very short forecasts. StatCast is based on pyranometer data measured at the site as well as concurrent meteorological observations and forecasts. StatCast is based on regime-dependent artificial intelligence forecasting techniques and has been shown to improve on “smart persistence” forecasts by 15-50%. A second category of short-range forecasting systems employ satellite imagery and use that information to discern clouds and their motion, allowing them to project the clouds, and the resulting blockage of irradiance, in time. CIRACast (the system produced by the Cooperative Institute for Atmospheric Research [CIRA] at Colorado State University) was already one of the more advanced cloud motion systems, which is the reason that team was brought to this project. During the project timeframe, the CIRA team was able to advance cloud shadowing, parallax removal, and implementation of better advecting winds at different altitudes. CIRACast shows generally a 25-40% improvement over Smart Persistence between sunrise and approximately 1600 UTC (Coordinated Universal Time) . A second satellite-based system, MADCast (Multi-sensor Advective Diffusive foreCast system), assimilates data from multiple satellite imagers and profilers to assimilate a fully three-dimensional picture of the cloud into the dynamic core of WRF. During 2015, MADCast (provided at least 70% improvement over Smart Persistence, with most of that skill being derived during partly cloudy conditions. That allows advection of the clouds via the Weather Research and Forecasting (WRF) model dynamics directly. After WRF-Solar™ showed initial success, it was also deployed in nowcasting mode with coarser runs out to 6 hours made hourly. It provided improvements on the order of 50-60% over Smart Persistence for forecasts up to 1600 UTC. The advantages of WRF-Solar-Nowcasting and MADCast were then blended to develop the new MAD-WRF model that incorporates the most important features of each of those models, both assimilating satellite cloud fields and using WRF-So far physics to develop and dissipate clouds. MAE improvements for MAD-WRF for forecasts from 3-6 hours are improved over WRF-Solar-Now by 20%. While all the Nowcasting system components by themselves provide improvement over Smart Persistence, the largest benefit is derived when they are smartly blended together by the Nowcasting Integrator to produce an integrated forecast. The development of WRF-Solar™ under this project has provided the first numerical weather prediction (NWP) model specifically designed to meet the needs of irradiance forecasting. The first augmentation improved the solar tracking algorithm to account for deviations associated with the eccentricity of the Earth’s orbit and the obliquity of the Earth. Second, WRF-Solar™ added the direct normal irradiance (DNI) and diffuse (DIF) components from the radiation parameterization to the model output. Third, efficient parameterizations were implemented to either interpolate the irradiance in between calls to the expensive radiative transfer parameterization, or to use a fast radiative transfer code that avoids computing three-dimensional heating rates but provides the surface irradiance. Fourth, a new parameterization was developed to improve the representation of absorption and scattering of radiation by aerosols (aerosol direct effect). A fifth advance is that the aerosols now interact with the cloud microphysics, altering the cloud evolution and radiative properties, an effect that has been traditionally only implemented in atmospheric computationally costly chemistry models. A sixth development accounts for the feedbacks that sub-grid scale clouds produce in shortwave irradiance as implemented in a shallow cumulus parameterization Finally, WRF-Solar™ also allows assimilation of infrared irradiances from satellites to determine the three dimensional cloud field, allowing for an improved initialization of the cloud field that increases the performance of short-range forecasts. We find that WRF-Solar™ can improve clear sky irradiance prediction by 15-80% over a standard version of WRF, depending on location and cloud conditions. In a formal comparison to the NAM baseline, WRF-Solar™ showed improvements in the Day-Ahead forecast of 22-42%. The SunCast™ system requires substantial software engineering to blend all of the new model components as well as existing publically available NWP model runs. To do this we use an expert system for the Nowcasting blender and the Dynamic Integrated foreCast (DICast®) system for the NWP models. These two systems are then blended, we use an empirical power conversion method to convert the irradiance predictions to power, then apply an analog ensemble (AnEn) approach to further tune the forecast as well as to estimate its uncertainty. The AnEn module decreased RMSE (root mean squared error) by 17% over the blended SunCast™ power forecasts and provided skill in the probabilistic forecast with a Brier Skill Score of 0.55. In addition, we have also developed a Gridded Atmospheric Forecast System (GRAFS) in parallel, leveraging cost share funds. An economic evaluation based on Production Cost Modeling in the Public Service Company of Colorado showed that the observed 50% improvement in forecast accuracy will save their customers $819,200 with the projected MW deployment for 2024. Using econometrics, NCAR has scaled this savings to a national level and shown that an annual expected savings for this 50% forecast error reduction ranges from $11M in 2015 to $43M expected in 2040 with increased solar deployment. This amounts to a $455M discounted savings over the 26 year period of analysis.

14 SOLAR ENERGY↗

Investigating the Relative Roles of INPs and CCN in a Simulated Thunderstorm Using a New Immersion Freezing Algorithm

Microphysical processes in deep convective clouds are sensitive to the number concentrations of cloud condensation nuclei (CCN) and ice nucleating particles (INPs), but the effects of INPs are less studied. Modeling studies investigating the effects of INPs and/or CCN on deep convection typically retain a volume‐dependent raindrop freezing relation. The resulting neglect of aerosol accumulation in raindrops via drop collisions has likely produced unrealistic storm responses to INPs in past studies. To address this deficiency, a new immersion freezing algorithm was developed and embedded in a bulk microphysics scheme that freezes both cloud drops and raindrops using the same immersion freezing INP (IF‐INP) activity spectrum based on measurements. Multiple idealized simulations of a single case of deep convection observed during the Clouds, Aerosols, and Complex Terrain Interactions (CACTI) field campaign were conducted, with microphysical differences produced by independently altering IF‐INP temperature dependencies and CCN number concentrations from their observed values. Surface precipitation in all simulations resulted almost exclusively from riming graupel that melted upon descending to the surface. Rainfall and cold pools were substantially and systematically weakened with increased CCN due to decreased graupel riming rates but were relatively insensitive to variations in the magnitude and slope of IF‐INP spectra due to compensating depletion of supercooled liquid water. These compensating processes were a consequence of the accumulation of IF‐INPs in raindrops, encouraging caution in studying IF‐INP effects upon thunderstorms using traditional volume‐dependent drop freezing relationships.

CCN↗

Use of Aerosol Observations From Aircraft in Satellite Remote Sensing and Modelling Comparisons

Aerosol extensive and intensive properties vary throughout the world and remain one of the largest uncertainties in determining future climate both because of difficulties in their measurement and their modelled behaviors. Here we highlight the contributions of airborne sampling by the sunphotometer 4STAR (Spectrometers for Sky-Scanning Sun Tracking Atmospheric Research) from two different parts of the world; Korean peninsula and region during the KORUS-AQ experiment (KORean-US Air Quality in May-June 2016) and over the South East Atlantic during ORACLES (ObseRvations of CLouds above Aerosols and their intEractionS in August-September-October 2016, 2017, and 2018) field campaign. The high temporal and spatial resolution, afforded by airborne sampling during KORUS-AQ, are used to determine the variability of aerosol intensive and extensive properties, which is a metric than can be compared in between multiple different observations and models, even over varying surfaces and spanning multiple different aerosol emission sources. We show the consistency over spatial scales of the AOD (Aerosol Optical Depth), and the aerosol intensive properties (Angstrom exponent - AE, fine mode fraction - FMF) observed by 4STAR, GOCI (Geostationary Ocean Color Imager Yonsei aerosol retrieval v2), MERRA-2 reanalysis (Modern-Era Retrospective Analysis for Research and Applications, v2), and from airborne in situ aerosol optical measurements by LARGE (NASA Langley Aerosol Research Group Experiment). The majority of AODs due to fine mode aerosol is observed at altitudes lower than 2 km and is dependent on the prevailing meteorological conditions. AE and FMF are found to be more spatially variable than AOD during all of KORUS-AQ, even when accounting for potential sampling biases. This may indicate that microphysical processes like aerosol particle formation, growth, and coagulation impact the dominant aerosol size at shorter scales than their combined effect on the aerosol optical depth by the aerosol emission, transport, and removal. Averaging between measurements and model, the distance at which the correlation to itself is reduced by 15% is 65 km for AOD, and 22.7 km for AE. Vertically resolved measurement from an aircraft enable the direct measurements of aerosols overlying clouds. When aerosol overlie bright clouds, their radiative impact on the incident light can be either positive or negative. This difference in radiative impact promotes difficulties in remote sensing aerosol properties, which have shown biases in AOD retrievals when clouds are underneath. The AOD above clouds measured by 4STAR during ORACLES are used to build and improve upon the current Near-Real-Time MODACAERO algorithm for above cloud AOD from MODIS, into a continuity product for NASA EOS/SNPP/JPSS.

Aerosol↗

Drivers of Seasonal Variability in Marine Boundary Layer Aerosol Number Concentration Investigated Using a Steady State Approach

Marine boundary layer (MBL) aerosol particles affect the climate through their interaction with MBL clouds. Although both MBL clouds and aerosol particles have pronounced seasonal cycles, the factors controlling seasonal variability of MBL aerosol particle concentration are not well-constrained. In this paper an aerosol budget is constructed representing the effects of wet deposition, free-tropospheric entrainment, primary surface sources, and advection on the MBL accumulation mode aerosol number concentration (N a ). These terms are further parameterized, and by assuming that on seasonal timescales N a is in steady state, the budget equation is rearranged to form a diagnostic equation for N a based on observable variables. Using data primarily collected in the subtropical northeast Pacific during the MAGIC campaign (Marine ARM (Atmospheric Radiation Measurement) GPCI (GCSS Pacific Cross-section Intercomparison) Investigation of Clouds), estimates of both mean summer and winter N a concentrations are made using the simplified steady-state model and seasonal mean observed variables, and are found to match well with the observed N a . To attribute the modeled difference between summer and winter aerosol concentrations to individual observed variables (e.g. precipitation rate, free-tropospheric aerosol number concentration), a local sensitivity analysis is combined with the seasonal difference in observed variables. This analysis shows that despite wintertime precipitation frequency being lower than summer, the higher winter precipitation rate accounted for approximately 60% of the modeled seasonal difference in N a , which emphasizes the importance of marine stratocumulus precipitation in determining MBL aerosol concentrations on longer time scales.

54 ENVIRONMENTAL SCIENCES↗

Theoretical Studies of Microphysics of Marine Boundary-Layer Clouds

This project is aimed at better understanding the role that aerosols play in altering the properties of stratus clouds. This interaction, termed the indirect effect of aerosols on climate, is a major subject a of study since the radiative forcing involved may rival that of greenhouse gases, but may be of the opposite sign. Our goal was to create numerical models of the phenomena, test them with data, and thereby gain insight into the physical processes occurring. Below we list the papers that we have produced during this grant. We then discuss these papers.

Toon, Owen B.↗

The Coupling Between Tropical Meteorology, Aerosol Lifecycle, Convection, and Radiation, During the Clouds, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex)

The NASA Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex) employed the NASA P-3, Stratton Park Engineering Company (SPEC) Learjet 35, and a host of satellites and surface sensors to characterize the coupling of aerosol processes, cloud physics, and atmospheric radiation within the Maritime Continent’s complex southwest monsoonal environment. Conducted in the late summer of 2019 from Luzon Philippines in conjunction with the Office of Naval Research Propagation of Intraseasonal Tropical OscillatioNs (PISTON) experiment with its R/VSally Ride stationed in the North Western Tropical Pacific, CAMP2Ex documented diverse biomass burning, industrial and natural aerosol populations and their interactions with small to congestus convection. The 2019 season exhibited El Nino and associated drought, high biomass burning emissions, and an early monsoon transition allowing for observation of pristine to massively polluted environments as they advected through intricate diurnal mesoscale and radiative environments into the monsoonal trough. CAMP2Ex’s preliminary results indicate 1) increasing aerosol loadings tend to invigorate congestus convection in height and increase liquid water paths; 2) lidar, polarimetry, and geostationary Advanced Himawari Imager remote sensing sensors have skill in quantifying diverse aerosol and cloud properties and their interaction; and 3) high resolution remote sensing technologies are able to greatly improve our ability to evaluate the radiation budget in complex cloud systems. Through the development of innovative informatics technologies, CAMP2Ex provides a benchmark dataset of an environment of extremes for the study of aerosol, cloud and radiation processes as well as a crucible for the design of future observing systems.

CAMP2Ex↗

Weak, shallow, dry convection over Angola increases offshore stratocumulus cloud droplet number concentrations

Boundary-layer cloud interactions involving shortwave-absorbing aerosols remain one of the least understood aerosol influences on climate. Here, we find the highest stratocumulus cloud droplet number concentrations over the southeast Atlantic occur when agricultural fires coincide with synoptically-weakened surface warming over Angola, occurring June-early August. Dry convection fills a shallow continental boundary layer with smoke, and a nighttime (local solar time 2-9) land breeze transports the aerosol into the marine boundary layer. Offshore aerosol transport is strengthened by low-level easterlies from a continental pressure high southeast of Angola. Simultaneously, the South Atlantic subtropical high is weaker, allowing extensive dispersal of aerosol offshore into the boundary layer, obscuring cloud brightening from shipping. Meteorological co-variation at synoptic scales compensates for cloud brightening by the smoke. Outgoing shortwave radiation increases by 15–20% of the monthly mean in June and July when offshore droplet numbers are less but the stratocumulus deck is more developed.

54 ENVIRONMENTAL SCIENCES↗

Assessing the Effects of Anthropogenic Aerosols on Pacific Storm Track Using a Multiscale Global Climate Model

Atmospheric aerosols impact weather and global general circulation by modifying cloud and precipitation processes, but the magnitude of cloud adjustment by aerosols remains poorly quantified and represents the largest uncertainty in estimated forcing of climate change. Here we assess the impacts of anthropogenic aerosols on the Pacific storm track using a multi-scale global aerosol-climate model (GCM). Simulations of two aerosol scenarios corresponding to the present day and pre-industrial conditions reveal long-range transport of anthropogenic aerosols across the north Pacific and large resulting changes in the aerosol optical depth, cloud droplet number concentration, and cloud and ice water paths. Shortwave and longwave cloud radiative forcing at the top of atmosphere are changed by - 2.5 and + 1.3 W m-2, respectively, by emission changes from pre-industrial to present day, and an increased cloud-top height indicates invigorated mid-latitude cyclones. The overall increased precipitation and poleward heat transport reflect intensification of the Pacific storm track by anthropogenic aerosols. Hence, this work provides for the first time a global perspective of the impacts of Asian pollution outflows from GCMs. Furthermore, our results suggest that the multi-scale modeling framework is essential in producing the aerosol invigoration effect of deep convective clouds on the global scale.

aerosol-cloud-climate interaction↗

Mechanical and Thermal Forcing for Upslope Flows and Cumulus Convection over the Sierras de Córdoba

Abstract The upslope flow processes affecting the vertical extent of orographic cumulus convection are examined using observations from the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign. Specifically, clear air returns from the U.S. Department of Energy (DOE) second-generation C-band scanning Atmospheric Radiation Measurement (ARM) precipitation radar (CSAPR2) are used to characterize the structure and variability of the ridge-normal (i.e., up/downslope) flow components, which transport mass to the crest of Argentina’s Sierras de Córdoba and contribute to convective initiation. Data are compiled for the entire CACTI period (October–April), including days with clear skies, shallow cumuli, cumulus congestus, and deep convection. To examine shared variability among >70 000 radar scans, we use (i) a principal component analysis (PCA) to isolate modes of variability in the upslope flow and (ii) composite analysis based on convective outcomes, determined from GOES-16 satellite observations. These data are contextualized with observed surface sensible heat fluxes, thermodynamic profiles, and synoptic-scale analysis. Results indicate distinct thermally and mechanically forced upslope flow modes, modulated by diurnal heating and synoptic-scale variations, respectively. In some instances, there is a superposition of thermal and mechanical forcing, yielding either deeper or shallower upslope flow. The composite analyses based on satellite data show that successively deeper convective outcomes are associated with successively deeper upslope flow layers that more readily transport mass to the ridge crest in conjunction with lower lifting condensation levels, facilitating convective initiation. These results help to isolate the forcing mechanisms for orographic convection and thus provide a foundation for parameterizing orographic convective processes in coarse resolution models.

Meteorology & Atmospheric Sciences↗

Development and Rigorous Validation of Modules for Predicting Organic Aerosol CCN Activity from Molecular Properties

The indirect interaction of anthropogenic aerosols with clouds (aerosol indirect forcing) represents one of the main uncertainties in climate projections, and reducing this uncertainty requires improved understanding of the aerosol life cycle, including atmospheric aging and the ability to nucleate cloud droplets or crystals. A key parameter that links the chemical properties of aerosol to its nucleating properties, and ultimately to aerosol indirect forcing, is its hygroscopicity (ability to uptake water). One way to compare and systematize the ability of various chemical compounds or particle types to nucleate cloud drops is via the hygroscopicity parameter κ, which can be used directly in global models to simulate aerosol indirect forcing. In this project we further investigated the relationships between the chemical composition of organic aerosol particles, which are known to be important components of atmospheric particulate matter, and their ability to serve as cloud condensation nuclei (CCN). In particular, we isolated the role of viscosity on κ by applying methods similar to those we used previously in our DOE/ASR research. Our motivation for the focus on viscosity was through its link to particle phase state. Particle phase affects water uptake on timescales relevant to the laboratory and also likely relevant to atmospheric processes, with reduced apparent hygroscopicities for semisolid and solid particles, compared with liquid particles. Water uptake itself affects viscosity, an important feedback that we explored in this project. The objectives of the project were as follows: (1) measure the effects of molecular structure, temperature, and relative humidity on the viscosity of organic aerosol formed via controlled laboratory experiments, (2) measure the effects of organic aerosol viscosity on water uptake and CCN activity above and below water saturation, (3) further develop the κ parameterization of organic aerosol hygroscopicity to include viscosity/phase, and (4) experimentally validate the κ parameterization for organic aerosol with chemical composition ranging from relatively simple to complex. It was proposed that particle viscosity exerts a kinetic control on equilibrium water uptake. High viscosity was expected to delay water uptake based on diffusional limitations. This would manifest itself in reduced observed CCN activity or κ. Understanding the interplay between water content and viscosity (composition control on particle viscosity) and between viscosity and equilibrium water content (diffusional control on water uptake) were the overall science objectives of this grant. Targeted experiments were carried out to test the kinetic control hypothesis. These experiments included studies that explicitly measured the equilibration time scale of water uptake, and experiments that tested the role of viscous particle coatings on the observed CCN activity. From the combined work, it is concluded that mass transfer limitations by glassy organic particles are unlikely to affect cloud droplet activation near laboratory temperatures. This implies that viscosity does not need to be included in parameterizations that link particle chemical composition and κ. A parameterization to predict κ through the UNIFAC group contribution method was developed with previous ASR funding. As planned, this computational module was further developed and validated here through targeted laboratory studies. The computational module has been made available as free software under the GNU public license. A database of κ-values to aid model development has been compiled and is available online via an open access model. In conducting this work, significant effort was made to understand how aerosol composition, including the associated aerosol water content, affects viscosity. This included a study detailing the influence of functional group composition on organic aerosol viscosity. We identified a strong link between volatility and viscosity. Functional groups responsible for low vapor pressure also promote high viscosity. Specifically, carboxylic acid and hydroxyl groups were identified as major contributors to high viscosity. Several studies were carried out to characterize the link between composition and the glass-to-liquid phase transition. Compositions tested include models of organic/inorganic particles and models of complex organic aerosol formed through secondary processes. A simple computational model to predict the amorphous phase diagram was developed and tested. Excellent agreement between model and measurements was obtained for organic/inorganic mixtures. The computational model is simple enough to be included in global model simulations. However, constraints of input parameters such as the Gordon-Taylor constant for binary mixtures for a wide range of complex mixtures have not yet been fully evaluated. Combined, the performed work provides new constraints on the amorphous phase state of organic aerosols.

54 ENVIRONMENTAL SCIENCES↗

Aircraft Video Camera (CAM-AIR) Instrument Handbook

The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) Aerial Facility (AAF) video cameras are installed in the cockpit of ARM’s research aircraft looking forward and in the belly of the plane looking down at the ground. Prior to the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign in the Azores during 2017, the P1344 camera was flown in the forward (cockpit) position and the P1347 camera was flown in the nadir (belly) position. Since only the forward camera was flown for ACE-ENA and the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign in Argentina during 2018–2019, the camera with the higher resolution (P1347) was moved to the cockpit.

47 OTHER INSTRUMENTATION↗

Evaluating and Improving Convective Parameterization for GCMs Using ARM Observations. Final report

This technical report summarizes the achievements during the project period funded by the Atmospheric System Research (ASR) program. The general goal of the project is to improve the representation of atmospheric deep convection in global climate models. By using DOE Atmospheric Radiation Measurement (ARM) program observations and a hierarchy of models from cloud-resolving to global climate models, we evaluated and improved many aspects of convection parameterization schemes, such as the trigger function for convection and closure condition to determine the amount of convection. We also incorporated the stochasticity of convection into a convection scheme. These improvements, when implemented into the National Center for Atmospheric Research (NCAR) Community Earth System Model (CESM) and the DOE Exascale Energy Earth System Model (E3SM), led to improved simulation of precipitation characteristics, including precipitation intensity, Intertropical Convergence Zone, and Madden-Julian oscillation. The project also improved the representation of microphysical processes in convective clouds. It enables the interaction of cloud microphysics with aerosols in weather and climate models.

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.

54 ENVIRONMENTAL SCIENCES↗

MOSAiC Radar b1 Processing: Corrections, Calibrations, and Processing Report

The U.S. Department of Energy’s (DOE) Atmospheric Radiation Measurement (ARM) user facility deployed many instruments on board a German ice breaker, the Research Vessel (RV) Polarstern, for one year from October 2019 to October 2020. The purpose of the Multidisciplinary Drifting Observatory for the Study of Arctic Climate (MOSAiC) field campaign was to study the decline in the sea-ice pack around the North Pole, and what factors may be at play. After the campaign ended, efforts were undertaken to provide a calibrated radar data set for future studies. MOSAiC presented new challenges to this process, as existing methodologies often were not applicable for the frozen environment with little to no ground clutter, and concurrent engineering updates or calibrations could not be accomplished once the ship set off. Like the previous Cloud, Aerosol, and Complex Terrain Interactions (CACTI) and Cold-air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) documentation (Hardin et al. 2020, Matthews et al. 2023), the data correction and calibration process is known in ARM as creating a “b1” datastream. This means that the radar datastreams have been well characterized to the best possible quality. This report will detail the status of the raw “a1” level data sets during the MOSAiC campaign, the corrections that were applied to create the “b1” data files, and the details of the applied methods.

54 ENVIRONMENTAL SCIENCES↗