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Improved Simulations of Biomass Burning Aerosol Optical Properties and Lifetimes in the NASA GEOS Model during the ORACLES-I Campaign

In order to improve aerosol representation in the NASA Goddard Earth Observing System (GEOS) model, we evaluated simulations of the aerosol properties and transport over the southern African biomass burning source and outflow region using observations made during the first deployment of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) field campaign in September 2016. An example case study of September 24 was analyzed in detail, during which aircraft-based in-situ and remote sensing observations showed the presence of a multi-layered smoke plume structure with significant vertical variation in single scattering albedo (SSA). Our baseline GEOS simulations were not able to represent the observed SSA variation, nor the observed organic aerosol-to-black carbon ratio (OA : BC). Analyzing the simulated smoke age suggests that the higher altitude, less absorbing smoke plume was younger (~4 days), while the lower altitude and more absorbing smoke plume was older (~7 days). We hypothesize a chemical or microphysical loss process exists to explain the change in aerosol absorption as the smoke plume ages, and we apply a simple 6-day e-folding loss rate to the model hydrophilic biomass burning OA to mimic this process. Adding this loss process required some adjustment to the model assumed scaling factors of aerosol emissions to conserve the regional aerosol loading and further improve the simulated OA : BC ratio. Accordingly, we have increased our biomass burning emissions of OA by 60 % and biomass burning BC by 15 %. We also utilized the ORACLES airborne observations to better constrain the simulation of aerosol optical properties, adjusting the assumed particle size, hygroscopic growth, and absorption. Our final GEOS model simulation with additional OA loss and updated optics showed a better performance in simulating AOD and SSA compared to independent ground and space-based retrievals for the entire month of September 2016, including the OMI Aerosol Index. In terms of radiative implications of our model adjustments, the final GEOS simulation suggested a decreased atmospheric warming of about 10 % (~2 W m -2 ) over the south-east Atlantic region and above the stratocumulus cloud decks compared to the model baseline simulations. These results improve the representation of the smoke age, transport, and optical properties in Earth system models.

aerosols↗

A13H-2546: Intercomparison of biomass burning aerosol properties from in-situ and remote-sensing instruments in ORACLES-2016

The magnitude of the cumulative effects of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in our understanding of anthropogenic radiative forcing on the climate. The magnitude of aerosol effects in any given region will depend on not just the aerosol concentration, but also on the characteristics of the aerosol under consideration. The NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in 2016-2018 over three deployments in the Southeast Atlantic Ocean (SEA), with the goal of making observations of seasonal biomass burning (BB) smoke plumes overlying persistent stratocumulus cloud decks. During the first ORACLES deployment (September 2016), two NASA aircraft (a P-3 and an ER-2) were flown with a suite of aerosol, cloud, radiation, and meteorological instruments for remote-sensing and in-situ observations. In ORACLES, data collected by eight different instrument teams are used to derive aerosol properties over this region by independent methods. Here we present a comparison of results from the different instrument retrievals with a focus on the measures of aerosol absorption. We focus on specific cases with near-coincident measurements from in-situ (PSAP or PTI for aerosol absorption combined with a nephelometer for aerosol scattering) and remote sensing (4STAR, AirMSPI, RSP, and SSFR) instruments from coordinated flights between the two aircraft. We use the single scattering albedo (SSA), a measure of the relative absorption versus total extinction by aerosols, as the main comparable property between the various remote sensing and in-situ methods. For the remote sensing instruments, we see general good agreement in the total aerosol loading (aerosol optical depth, AOD), though see some differences in the absorbing component (AAOD). We report values for the retrieved aerosol parameters measured in the ORACLES flights and comment upon the observed variability between different instruments. Finally, we discuss these ORACLES results in the context of previous measurements of BB aerosol over the SEA.

Kristina Pistone↗

Above-Cloud Aerosol Radiative Effects based on ORACLES 2016 and ORACLES 2017 Aircraft Experiments

Determining the direct aerosol radiative effect (DARE) of absorbing aerosols above clouds from satellite observations alone is a challenging task, in part because the radiative signal of the aerosol layer is not easily untangled from that of the clouds below. In this study, we use aircraft measurements from the NASA ObseRvations of CLouds above Aerosols and their intEractionS (ORACLES) project in the southeastern Atlantic to derive it with as few assumptions as possible. This is accomplished by using spectral irradiance measurements (Solar Spectral Flux Radiometer, SSFR) and aerosol optical depth (AOD) retrievals (Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research, 4STAR) during vertical profiles (spirals) that minimize the albedo variability of the underlying cloud field – thus isolating aerosol radiative effects from those of the cloud field below. For two representative cases, we retrieve spectral aerosol single scattering albedo (SSA) and the asymmetry parameter (g) from these profile measurements and calculate DARE given the albedo range measured by SSFR on horizontal legs above clouds. For mid-visible wavelengths, we find SSA values from 0.80 to 0.85 and a significant spectral dependence of g. As the cloud albedo increases, the aerosol increasingly warms the column. The transition from a cooling to a warming top-of-aerosol radiative effect occurs at an albedo value (critical albedo) just above 0.2 in the mid-visible wavelength range. In a companion paper, we use the techniques introduced here to generalize our findings to all 2016 and 2017 measurements and parameterize aerosol radiative effects.

Cloud aerosol↗

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 (AIE) using analytic representations of cloud and aerosol distributions and processes. Although the simple model is able to produce estimates of AIEs that are comparable to those from some global aerosol models using the same global mean aerosol properties, the estimates by the simple model are sensitive to preindustrial cloud condensation nuclei concentration, preindustrial accumulation mode radius, width of the accumulation mode, size of primary particles, cloud thickness, primary and secondary anthropogenic emissions, 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. Estimates of present-day AIEs as low as 5 W/sq m and as high as 0.3 W/sq m are obtained for plausible sets of parameter values. Estimates are surprisingly linear in emissions. The estimates depend on parameter values in ways that are consistent with results from detailed global aerosol-climate simulation models, which adds to understanding of the dependence on AIE uncertainty on uncertainty in parameter values.

Clouds↗

Influence of Cloud, Fog, and High Relative Humidity during Pollution Transport Events in South Korea: Aerosol Properties and PM2.5 Variability

This investigation examines aerosol dynamics during major fine mode aerosol transboundary pollution events in South Korea primarily during the KORUS-AQ campaign from May 1 – June 10, 2016, particularly when cloud fraction was high and/or fog was present to quantify the change in aerosol characteristics due to near-cloud or fog interaction. We analyze the new AERONET Version 3 data that have significant changes to cloud screening algorithms, allowing many more fine-mode observations in the near vicinity of clouds or fog. Case studies for detailed investigation include May 25–26, 2016 when cloud fraction was high over much of the peninsula, associated with a weak frontal passage and advection of pollution from China. These cloud-influenced Chinese transport dates also had the highest aerosol optical depth (AOD), surface PM2.5 concentrations and fine mode particle sizes of the entire campaign. Another likewise cloud/high relative humidity (RH) case is June 9 and 10, 2016 when fog was present over the Yellow Sea that appears to have affected aerosol properties well downwind over the Korean peninsula. In comparison we also investigated aerosol properties on air stagnation days with very low cloud cover and relatively low RH (May 17 & 18, 2016), when local Korean emissions dominated. Aerosol volume size distributions show marked differences between the transport days (with high RH and cloud influences) and the local pollution stagnation days, with total column-integrated particle fine mode volume being an order of magnitude greater on the pollution transport dates. The PM2.5 over central Seoul were significantly greater than for coastal sites on the transboundary transport days yet not on stagnation days, suggesting addi-tional particle formation from gaseous urban emissions in cloud/fog droplets and/or in the high RH humidified aerosol environment. Many days had KORUS-AQ research aircraft flights that provided observations of aerosol absorption, particle chemistry and vertical profiles of extinction. AERONET retrievals and aircraft in situ mea-surements both showed high single scattering albedo (weak absorption) on the cloudy or cloud influenced days, plus aircraft profile in situ measurements showed large AOD enhancements (versus dried aerosol) at ambient relative humidity (RH) on the pollution transport days, consistent with the significantly larger fine mode particle radii and weak absorption.

Aerosol↗

An Assessment of the Surface Longwave Direct Radiative Effect of Airborne Dust in Zhangye China During the Asian Monsoon Year Field Experiment (2008)

Tiny suspensions of solid particles or liquid droplets, called aerosols, hover in earth's atmosphere and can be found over just about anywhere including oceans, deserts, vegetated areas, and other global regions. Aerosols come in a variety of sizes, shapes, and compositions which depend on such factors as their origin and how long they have been in the atmosphere (i.e., their residence time). Some of the more common types of aerosols include mineral dust and sea salt which get lifted from the desert and ocean surfaces, respectively by mechanical forces such as strong winds. Depending on their size, aerosols will either fall out gravitationally, as in the case of larger particles, or will remain resident in the atmosphere where they can undergo further change through interactions with other aerosols and cloud particles. Not only do aerosols affect air quality where they pose a health risk, they can also perturb the distribution of radiation in the earth-atmosphere system which can inevitably lead to changes in our climate. One aerosol that has been in the forefront of many recent studies, particularly those examining its radiative effects, is mineral dust. The large spatial coverage of desert source regions and the fact that dust can radiatively interact with such a large part of the electromagnetic spectrum due to its range in particle size, makes it an important aerosol to study. Dust can directly scatter and absorb solar and infrared radiation which can subsequently alter the amount of radiation that would otherwise be present in the absence of dust at any level of the atmosphere like the surface. This is known as radiative forcing. At the surface dust can block incoming solar energy, however at infrared wavelengths, dust acts to partially compensate the solar losses. Evaluating the solar radiative effect of dust aerosols is relatively straightforward due in part to the relatively large signal-to-noise ratio in the measurements. At infrared wavelengths, on the other hand, the effect is rather difficult to ascertain since the measured dust signal level is on the same order as the instrumental uncertainties. Although the radiative impact of dust is much smaller in the infrared, it can still have a noticeable influence on the distribution of energy in the Earth-atmosphere system. This is mainly attributed to the strong light-absorptive properties commonly found in many earth minerals.

Hansell, Richard A.↗

Vertical Structure of a Springtime Smoky and Humid Troposphere Over the Southeast Atlantic From Aircraft and Reanalysis

The springtime atmosphere over the southeast Atlantic Ocean (SEA) is subjected to a consistent layer of biomass burning (BB) smoke from widespread fires on the African continent. An elevated humidity signal is coincident with this layer, consistently proportional to the amount of smoke present. The combined humidity and BB aerosol has potentially significant radiative and dynamic impacts. Here, we use aircraft-based observations from the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) deployments in conjunction with reanalyses to characterize covariations in humidity and BB smoke across the SEA. The observed plume–vapor relationship, and its agreement with the European Centre for Medium-Range Weather Forecasts (ECMWF) Reanalysis version 5 (ERA5) and Copernicus Atmosphere Monitoring Service (CAMS) reanalysis, persists across all observations, although the magnitude of the relationship varies as the season progresses. Water vapor is well represented by the reanalyses, while CAMS tends to underestimate carbon monoxide especially under high BB. While CAMS aerosol optical depth (AOD) is generally overestimated relative to ORACLES AOD, the observations show a consistent relationship between carbon monoxide (CO) and aerosol extinction, demonstrating the utility of the CO tracer to understanding vertical aerosol distribution. We next use k-means clustering of the reanalyses to examine multi-year seasonal patterns and distributions. We identify canonical profile types of humidity and of CO, allowing us to characterize changes in vapor and BB atmospheric structures, and their impacts as they covary. While the humidity profiles show a range in both total water vapor concentration and in vertical structure, the CO profiles primarily vary in terms of maximum concentration, with similar vertical structures in each. The distribution of profile types varies spatiotemporally across the SEA region and through the season, ranging from largely one type in the northeast and southwest to more evenly distributed between multiple types where air masses meet in the middle of the SEA. These distributions follow patterns of transport from the humid, smoky source region (greatest influence in the northeast of the SEA) and the seasonal changes in both humidity and smoke (increasing and decreasing through the season, respectively). With this work, we establish a framework for a more complete analysis of the broader radiative and dynamical effects of humid aerosols over the SEA.

Kristina Pistone↗

Low-level liquid cloud properties during ORACLES retrieved using airborne polarimetric measurements and a neural network algorithm

In this study we developed a neural network (NN) that can be used to retrieve cloud microphysical properties from multiangular and multispectral polarimetric remote sensing observations. This effort builds upon our previous work, which explored the sensitivity of neural network input, architecture, and other design requirements for this type of remote sensing problem. In particular this work introduces a framework for appropriately weighting total and polarized reflectances, which have vastly different magnitudes and measurement uncertainties. The NN is trained using an artificial training set and applied to research scanning polarimeter (RSP) data obtained during the ORACLES field campaign (ObseRvations of Aerosols above CLouds and their intEractionS). The polarimetric RSP observations are unique in that they observe the same cloud from a very large number of angles within a variety of spectral bands, resulting in a large dataset that can be explored rapidly with a NN approach. The usefulness of applying a NN to a dataset such as this one stems from the possibility of rapidly obtaining a retrieval that could be subsequently applied as a first guess for slower but more rigorous physical-based retrieval algorithms. This approach could be particularly advantageous for more complicated atmospheric retrievals – such as when an aerosol layer lies above clouds like in ORACLES. For RSP observations obtained during ORACLES 2016, comparisons between the NN and standard parametric polarimetric (PP) cloud retrieval give reasonable results for droplet effective radius (r(e): R=0.756, RMSE=1.74 µm) and cloud optical thickness (τ: R=0.950, RMSE=1.82). This level of statistical agreement is shown to be similar to comparisons between the two most well-established cloud retrievals, namely, the polarimetric and the bispectral total reflectance cloud retrievals. The NN retrievals from the ORACLES 2017 dataset result in retrievals of r(e) (R=0.54, RMSE=4.77 µm) and τ (R=0.785, RMSE=5.61) that behave much more poorly. In particular we found that our NN retrieval approach does not perform well for thin (τ<3), inhomogeneous, or broken clouds. We also found that correction for above-cloud atmospheric absorption improved the NN retrievals moderately – but retrievals without this correction still behaved similarly to existing cloud retrievals with a slight systematic offset.

SPECTRAL-RESOLUTION LIDAR↗

Multi-Angle Polarimetry: The Once and Future King of Aerosol Remote Sensing

Although aerosols (and their interactions with clouds) are widely known to be one of the most uncertain components of the climate, they remain largely unconstrained in climate simulations. This is because global observations of all the parameters relevant to such simulations - quantity, size, shape, optical properties and chemical composition - are very difficult to simultaneously retrieve from existing remote sensing instruments. The problem can be addressed by maximizing the scene information gathered by a remote sensing instrument, by the use of (passive) multi-spectral, multi-angle and polarimetrically sensitive sensors. These observations, coupled with a radiative transfer model, can be inverted to solve for aerosol parameters. However, the choices to be made when designing an such an observing system and retrieval algorithm are complex, and a variety of approaches have been undertaken by the scientific community. I will review the various multi-spectral, multi-angle, polarimetric observation systems employed for aerosol remote sensing and their corresponding retrieval algorithms. This includes the French Polarization and Directionality of Earth Reflectance (POLDER) instrument, which has been the only such instrument successfully deployed in orbit thus far (most recently from 2004-2013), the NASA Aerosol Polarimetry Sensor (APS) on the ill-fated NASA Glory Mission (launch failure in 2011), potential or planned polarimeters on the NASA Aerosol-Cloud-Ecosystem (ACE) and Pre-Aerosol, Clouds and ocean Ecosystems (PACE) missions, and airborne prototypes from around the world.

Knobelspiesse, Kirk↗

Convective Biases in the US DOE Global Storm‐Resolving Model: Insights From Regionally Refined Simulations During the CACTI Campaign

Accurately simulating convective processes in complex terrain remains a critical challenge for global storm-resolving models (GSRMs). This study systematically evaluates moist convective biases in the Regionally Refined Mesh configuration of the U.S. Department of Energy Simple Cloud-Resolving E3SM Atmosphere Model (RRM-SCREAM) using comprehensive observations and large-eddy simulations from the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) campaign in the mountainous area of central Argentina. Comparisons of simulations with high-resolution observations and reanalysis data indicate that RRM-SCREAM effectively captures large-scale meteorological patterns, including regional atmospheric gradients and diurnal variability. However, RRM-SCREAM disproportionately produces smaller precipitation clusters referred to as “popcorn convection,” and exaggerated rainfall intensities compared to observations and reference models. Detailed examination of a representative orographic shallow-to-deep convective transition case shows that RRM-SCREAM delays initial shallow convection growth due to lower-tropospheric dryness and sustained convective inhibition, but once triggered, deep convection becomes overly vigorous with excessively strong vertical velocities and elevated cloud ice content, linked to a thermodynamic structure characterized by suppressed low-level moistening and excessive upper-level moisture retention. Our results highlight specific deficiencies in the model representation of convective vertical velocity, cloud microphysical processes, and convective precipitation organization within RRM-SCREAM. Addressing these biases is essential for improving the predictions of convective clouds and precipitation in the global high-resolution atmospheric models.

Su, Tianning [Lawrence Livermore National Laborato↗

EPCAPE Mt. Soledad In Situ Ozone Field Campaign Report

The focus of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE) is to characterize the extent, radiative properties, aerosol interactions, and precipitation characteristics of stratocumulus clouds in the Eastern Pacific Ocean across all four seasons at a coastal location, the Scripps Pier and the Scripps Institution of Oceanography Mt. Soledad sites in La Jolla, California. An important enhancement in support of this study was the measurement of ozone at the Scripps Mt. Soledad site to help in distinguishing in situ sampling of air parcels originating from regional polluted and clean marine sources.

54 ENVIRONMENTAL SCIENCES↗

EPCAPE Field: Final Campaign Report

The focus of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE) was to characterize the extent, radiative properties, aerosol interactions, and precipitation characteristics of stratocumulus clouds in the Eastern Pacific across all four seasons at a coastal location. DOE ARM AMF1 with AOS was successfully deployed from February 14, 2023, through February 14, 2024, in La Jolla, California, at Scripps Pier and Mt. Soledad.

54 ENVIRONMENTAL SCIENCES↗

A13H-2537: Above Cloud Aerosol Optical Properties in the South East Atlantic from airborne observations during ORACLES

Aerosol overlying marine stratocumulus clouds is a persistent feature in the southeast Atlantic during the biomass burning season, July through November. We sampled aerosol and cloud from an airborne research platform, the NASA P3, during the deployments of ObseRvations of CLouds above Aerosols and their intEractionS (ORACLES) encompassing the peak biomass burning season. We used the Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) to quantify the aerosol’s optical properties, notably the aerosol optical depth (AOD) by directly measuring the amount of light attenuation. We present an overview of very recent AOD measurements and contrast those to previous deployments. We observed an average AOD at 500 nm of 0.33 (0.30) in September 2016 (August 2017), with similar spatial dependence as observed by the MODIS instrument on board the TERRA and AQUA satellites. We also show full spectral vertical dependence of AOD from flight profiles, which compares favorably to the integrated aerosol extinction profile obtained by the active remote sensing High Spectral Resolution Lidar-2 (HSRL-2). We also present a quantification of the gap extent separating cloud top and aerosol layer bottom. Using hyperspectral transmitted light measurements from 4STAR, in conjunction with hyperspectral hemispheric irradiance measurements from the Solar Spectral Flux Radiometers (SSFR), we retrieved aerosol intensive properties (asymmetry parameter, single scattering albedo), aerosol size distributions, cloud optical depth (COD), cloud particle effective radius, and cloud thermodynamic phase. Cloud properties, also presented here, are obtained from 4STAR measurements of scattered light below clouds.

Samuel E LeBlanc↗

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↗

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↗

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↗

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.↗