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Particle size distributions from TRACER-MAP

Particle size distributions measured using a custom scanning mobility analyzer (SMPS) and a TSI, Inc. aerodynamic particle sizer (APS). The size distributions measured with the two instruments were merged during data inversion to produce a single distribution spanning a diameter range from approximately 19 nanometers to 15 micrometers. Size-dependent cloud condensation nuclei (CCN) activity measured with a CCN counter operated in parallel to the condensation particle counter in the SMPS are reported separately. The measurements were made from the Baylor University/University of Houston Mobile Air Quality Laboratory (MAQL) between July 5 and August 30, 2022 during the TRACER-MAP project. The trailer moved between five sites in the Houston regions as follows: Aldine: 7/5-7/8, 7/21-7/26, 8/15-8/24 University of Houston: 7/8-7/16, 8/8-8/15 San Jacinto monument: 7/16-7/21 Jones State Forest: 7/26-8/1; 8/24-8/30 AMF site in La Porte: 8/1-8/8

54 ENVIRONMENTAL SCIENCES↗

Vertical Gradient of Size-Resolved Aerosol Compositions over the Arctic Reveals Cloud Processed Aerosol in-Cloud and above Cloud

Arctic aerosols play a significant role in the aerosol-radiation and aerosol-cloud interactions, but ground-based measurements are insufficient to explain the interaction of aerosols and clouds in a vertically stratified Arctic atmosphere. This study shows the vertical variability of aerosol particle composition via tethered balloon system at Oliktok Point, Alaska, in August 2019, at different cloud layers for two case studies (background aerosol condition and polluted condition). Multi-modal micro-spectroscopy analysis of samples during the background case reveals a broadening of chemically specific size distribution above cloud top with a high abundance of sulfate and core-shell morphology, suggesting possible cloud processing of aerosols. The pollution case also indicates a broadening of size distribution at the upper cloud layer with the dominance of carbonaceous aerosol, which suggests the potential of carbonaceous aerosols for Arctic cloud formation. Here this study provides insights into the vertical profile of Arctic aerosols on cloud formation.

54 ENVIRONMENTAL SCIENCES↗

Factors controlling marine aerosol size distributions and their climate effects over the northwest Atlantic Ocean region

Abstract. Aerosols over Earth's remote and spatially extensive ocean surfaces have important influences on planetary climate. However, these aerosols and their effects remain poorly understood, in part due to the remoteness and limited observations over these regions. In this study, we seek to understand factors that shape marine aerosol size distributions and composition in the northwest Atlantic Ocean region. We use the GEOS-Chem model with the TwO-Moment Aerosol Sectional (TOMAS) microphysics algorithm model to interpret measurements collected from ship and aircraft during the four seasonal campaigns of the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) conducted between 2015 and 2018. Observations from the NAAMES campaigns show enhancements in the campaign-median number of aerosols with diameters larger than 3 nm in the lower troposphere (below 6 km), most pronounced during the phytoplankton bloom maxima (May/June) below 2 km in the free troposphere. Our simulations, combined with NAAMES ship and aircraft measurements, suggest several key factors that contribute to aerosol number and size in the northwest Atlantic lower troposphere, with significant regional-mean (40–60∘ N and 20–50∘ W) cloud-albedo aerosol indirect effect (AIE) and direct radiative effect (DRE) processes during the phytoplankton bloom. These key factors and their associated simulated radiative effects in the region include the following: (1) particle formation near and above the marine boundary layer (MBL) top (AIE: −3.37 W m−2, DRE: −0.62 W m−2); (2) particle growth due to marine secondary organic aerosol (MSOA) as the nascent particles subside into the MBL, enabling them to become cloud-condensation-nuclei-sized particles (AIE: −2.27 W m−2, DRE: −0.10 W m−2); (3) particle formation and growth due to the products of dimethyl sulfide, above and within the MBL (−1.29 W m−2, DRE: −0.06 W m−2); (4) ship emissions (AIE: −0.62 W m−2, DRE: −0.05 W m−2); and (5) primary sea spray emissions (AIE: +0.04 W m−2, DRE: −0.79 W m−2). Our results suggest that a synergy of particle formation in the lower troposphere (particularly near and above the MBL top) and growth by MSOA contributes strongly to cloud-condensation-nuclei-sized particles with significant regional radiative effects in the northwest Atlantic. To gain confidence in radiative effect magnitudes, future work is needed to understand (1) the sources and temperature dependence of condensable marine vapors forming MSOA, (2) primary sea spray emissions, and (3) the species that can form new particles in the lower troposphere and grow these particles as they descend into the marine boundary layer.

54 ENVIRONMENTAL SCIENCES↗

Size dependence in chord characteristics from simulated and observed continental shallow cumulus

Abstract. In this study we compare long-term Doppler and Raman lidar observations against a full month of large eddy simulations of continental shallow cumulus clouds. The goal is to evaluate if the simulations can reproduce the mean observed vertical velocity and moisture structure of cumulus clouds and their associated subcloud circulations, as well as to establish if these properties depend on the size of the cloud. We propose methods to compare continuous chords of cloud detected from Doppler and Raman lidars with equivalent chords derived from 1D and 3D model output. While the individual chords are highly variable, composites of thousands of observed and millions of simulated chords contain a clear signal. We find that the simulations underestimate cloud size and fraction but successfully reproduce the observed structure of vertical velocity and moisture perturbations. There is a clear scaling of vertical velocity and moisture anomalies below the chords with chord size, but the moisture anomalies are only 1 %–2 % higher than the horizontal mean values. The differences between the observations and simulations are smaller than the difference in sampling the modeled chords in time or space. The shape of the vertical velocity and moisture anomalies from cloud chords sampled spatially from 3D model snapshots is almost perfectly symmetric. In contrast, the chords sampled temporally from the lidar observations and 1D model output have a marked asymmetry, with stronger updrafts and higher moisture anomalies occurring earlier on.

54 ENVIRONMENTAL SCIENCES↗

Rapid growth of anthropogenic organic nanoparticles greatly alters cloud lifecycle in the Amazon rainforest

Atmospheric nanoparticles can significantly influence Earth’s climate if they grow to sizes large enough to nucleate cloud droplets. While the contribution of extremely low volatility vapors to nanoparticle growth has been discussed extensively, the role of semivolatile organics has been largely overlooked. Here we examine the growth and impacts of air pollution nanoparticles from an isolated metropolis amidst the Amazon rainforest. Although extremely low volatility organics are necessary for the initial growth of nanoparticles, model analysis suggests that dynamic gas-particle partitioning of semivolatile oxidation products of anthropogenic and natural hydrocarbons is predominantly responsible for the observed rapid growth to 50 nm. Furthermore, cloud-resolving simulations demonstrate that the grown particles appreciably modify shallow cloud droplet size distribution, suppress precipitation, and enhance the transition to deep clouds. With condensable semivolatile organics typically formed in greater proportion, similar nanoparticle growth and impacts on clouds could likely occur in heavily urbanized forested regions globally.

Zaveri, Rahul A↗

DATASET: Rapid growth of anthropogenic organic nanoparticles greatly alters cloud lifecycle in the Amazon rainforest

Atmospheric nanoparticles can significantly influence Earth’s climate if they grow to sizes large enough to nucleate cloud droplets. While the contribution of extremely low volatility vapors to nanoparticle growth has been discussed extensively, the role of semivolatile organics has been largely overlooked. Here we examine the growth and impacts of air pollution nanoparticles from an isolated metropolis amidst the Amazon rainforest. Although extremely low volatility organics are necessary for the initial growth of nanoparticles, model analysis suggests that dynamic gas-particle partitioning of semivolatile oxidation products of anthropogenic and natural hydrocarbons is predominantly responsible for the observed rapid growth to 50 nm. Furthermore, cloud-resolving simulations demonstrate that the grown particles appreciably modify shallow cloud droplet size distribution, suppress precipitation, and enhance the transition to deep clouds. With condensable semivolatile organics typically formed in greater proportion, similar nanoparticle growth and impacts on clouds could likely occur in heavily urbanized forested regions globally.

Zaveri, Rahul A↗

Reduced‐Order Modeling for Linearized Representations of Microphysical Process Rates

Abstract Representing cloud microphysical processes in large scale atmospheric models is challenging because many processes depend on the details of the droplet size distribution (DSD, the spectrum of droplets with different sizes in a cloud). While full or partial statistical moments of droplet size distributions are the typical variables used in bulk models, prognostic moments are limited in their ability to represent microphysical processes across the range of conditions experienced in the atmosphere. Microphysical parameterizations employing prognostic moments are known to suffer from structural uncertainty in their representations of inherently higher dimensional cloud processes, which limit model fidelity and lead to forecasting errors. Here we investigate how data‐driven reduced‐order modeling can be used to learn predictors for microphysical process rates in bulk microphysics schemes in an unsupervised manner from higher dimensional bin distributions. Using simulations characteristic of marine stratiform clouds, we simultaneously learn lower dimensional representations of droplet size distributions and predict the evolution of the microphysical state of the system. Droplet collision‐coalescence, the main process for generating warm rain, is estimated to have an intrinsic dimension of three. This intrinsic dimension provides a lower limit on the number of degrees of freedom needed to accurately represent collision‐coalescence in models. We demonstrate how deep learning based reduced‐order modeling can be used to discover intrinsic coordinates describing the microphysical state of the system, where process rates such as collision‐coalescence are globally linearized. These implicitly learned representations of the DSD retain more information about the DSD than typical moment‐based representations.

54 ENVIRONMENTAL SCIENCES↗

Designing a Convection‐Cloud Chamber for Collision‐Coalescence Using Large‐Eddy Simulation With Bin Microphysics

Abstract Collisional growth of cloud droplets is an essential yet uncertain process for drizzle and precipitation formation. To improve the quantitative understanding of this key component of cloud‐aerosol‐turbulence interactions, observational studies of collision‐coalescence in a controlled laboratory environment are needed. In an existing convection‐cloud chamber (the Pi Chamber), collisional growth is limited by low liquid water content and short droplet residence times. In this work, we use numerical simulations to explore various configurations of a convection‐cloud chamber that may intensify collision‐coalescence. We employ a large‐eddy simulation (LES) model with a size‐resolved (bin) cloud microphysics scheme to explore how cloud properties and the intensity of collision‐coalescence are affected by the chamber size and aspect ratio, surface roughness, side‐wall wetness, side‐wall temperature arrangement, and aerosol injection rate. Simulations without condensation and evaporation within the domain are first performed to explore the turbulence dynamics and wall fluxes. The LES wall fluxes are used to modify the Scalar Flux‐budget Model, which is then applied to demonstrate the need for non‐uniform side‐wall temperature (two side walls as warm as the bottom and the two others as cold as the top) to maintain high supersaturation in a tall chamber. The results of LES with full cloud microphysics reveal that collision‐coalescence is greatly enhanced by employing a taller chamber with saturated side walls, non‐uniform side‐wall temperature, and rough surfaces. For the conditions explored, although lowering the aerosol injection rate broadens the droplet size distribution, favoring collision‐coalescence, the reduced droplet number concentration decreases the frequency of collisions.

54 ENVIRONMENTAL SCIENCES↗

Quantifying vertical wind shear effects in shallow cumulus clouds over Amazonia

Abstract. This study analyses and quantifies the effects of vertical wind shear (VWS) on the properties of shallow cumulus cloud fields over Central Amazonia. We perform idealised simulations with high resolution (50 m horizontally and 20 m vertically) using the Dutch Atmospheric Large-Eddy Simulation (DALES) model, changing the initial conditions and large-scale forcing of VWS. The resulting cloud field is analysed by applying a cloud tracking algorithm to generate Lagrangian datasets of the life cycle of individual clouds as well as their time-varying core and margin dimensions. The reference run has no wind speed or directional shear and represents a typical day in the local dry season. Numerical experiments with moderate and high wind speed shear are simulated by adding linear increases in the wind speed of 1.2 and 2.4 m s−1 km−1, respectively. Three additional runs are made by adding 90∘ of wind rotation between the surface and the top of the domain (5 km) on top of the three wind speed shear conditions. We find that clouds developing in a sheared environment have horizontal equivalent diameter increased by up to 100 m on average, but the cloud depth is reduced. Our quantification shows that VWS tends to increase the size of the cloud cores but reduces their relative area, volume, and mass fractions compared to the overall cloud dimensions. The addition of 2.4 m s−1 km−1 of VWS decreases the relative core area by about 0.03 (about 10 % of the overall average) and its volume and mass ratios by about 0.05 (10 %–25 % in relative terms). Relevant for the cloud transport properties is that the updraught speed and the liquid water content are lower within the cores, and consequently so is the upward mass flux. All quantifications of mean cloud properties point to the inhibition of convective strength by VWS, therefore hampering the shallow-to-deep transition. However, open questions still remain given that the individually deepest clouds were simulated under high environmental shear, even though they occur in small numbers. This could indicate other indirect effects of VWS that have opposite effects on cloud development if found to be significant in the future.

54 ENVIRONMENTAL SCIENCES↗

Evaluating Shallow Convection Parameterization Assumptions With a q t – w Quadrant Analysis

Abstract Uncertainties associated with the response of shallow clouds to global warming remain a great challenge for climate projection. Due to the small size of these clouds, parameterizations are required to represent them in both current‐ and next‐generation climate models. We present a quantitative evaluation of several important assumptions used in both mass‐flux and Assumed‐PDF Higher‐Order Closure parameterizations of shallow convection. We use large‐eddy simulations (LESs) of four different shallow convection regimes as benchmarks and apply a q t (total moisture)– w (vertical velocity) quadrant analysis technique to identify the “coherent structures” of moist and dry up/down‐drafts. The statistics of these coherent structures and the environment are then used to evaluate commonly used assumptions in mass‐flux parameterizations related to (a) the convective downdrafts and (b) the subplume variability of convective updrafts. For quantitative evaluation of the PDF closure used in AP‐HOCs, we perform offline calculations with the PDF closure used in the Cloud Layers Unified By Bi‐normals and the Simplified Higher‐Order Closure schemes by supplying the closure with statistical quantities directly calculated from the LESs. Then, the impact of parameterization assumptions embedded in the PDF closure in the same two categories is analyzed and understood through comparisons of the output from the closure with the statistics of the moist and dry up/down‐drafts from the LESs.

54 ENVIRONMENTAL SCIENCES↗

Simulating Marine Stratocumulus Clouds using Lagrangian Superdroplet Method in ERF

This study investigates the simulation of marine stratocumulus (stratoCu) clouds – common in many offshore and coastal wind energy regions - using Lagrangian Superdroplet Method (SDM) implemented in Energy Research and Forecasting (ERF) model. Developed by the Wind Energy Technologies Office (WETO), ERF is a high-resolution atmospheric modeling tool that relies on traditional bulk microphysics schemes. Under an LLNL-led Laboratory Directed Research and Development (LDRD) project, SDM was integrated into ERF to improve cloud process fidelity by explicitly tracking individual “superdroplets”. This enables a realistic representation of the droplet size spectrum, cloud-atmosphere interactions, and potential feedbacks from wind plants on atmospheric flow and cloud structure.

54 ENVIRONMENTAL SCIENCES↗

Cloud Condensation Nuclei Closure Study Using Airborne Measurements Over the Southern Great Plains

Abstract Airborne measurements of non‐refractory bulk aerosol chemical composition, aerosol size distributions, and cloud condensation nuclei (CCN) were conducted onboard a research aircraft during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems field campaign in the spring and summer of 2016. A CCN closure study for the entire campaign period was performed where measured CCN concentrations at 0.24% and 0.46% supersaturation were compared with the predicted CCN concentrations calculated using κ ‐Köhler theory, three different assumptions of aerosol mixing state, and various assumptions about hygroscopicity, density, and the insoluble fraction of organic particles. We found that the Closure Ratio (CR), calculated as the ratio of predicted to measured CCN concentrations, was equal to one under two different aerosol mixing state assumptions: (a) all particles are composed of 100% organic particles, and (b) particles are externally mixed and composed of pure sulfates, nitrates, and organic particles assuming hygroscopicity values for organic particles ( ) between 0.04 and 0.17. The use of internal mixing state assumption often led to overprediction of CCN concentrations but the agreement within ±20% with the measured CCN concentrations was observed under certain closure permutations. A similar agreement, that is, within ±20%, was also observed using permuted parameters concerning density (1 and 1.5 g cm −3 ) and an insoluble fraction (0% and 20%) of organic particles. These findings may provide constraints on to predict CCN concentrations at a remote continental Southern Great Plains site.

54 ENVIRONMENTAL SCIENCES↗

Scaling of Turbulence and Microphysics in a Convection–Cloud Chamber of Varying Height

Abstract The convection–cloud chamber enables measurement of aerosol and cloud microphysics, as well as their interactions, within a turbulent environment under steady‐state conditions. Increasing the size of a convection–cloud chamber, while holding the imposed temperature difference constant, leads to increased Rayleigh, Reynolds and Nusselt numbers. Large–eddy simulation coupled with a bin microphysics model allows the influence of increased velocity, time, and spatial scales on cloud microphysical properties to be explored. Simulations of a convection–cloud chamber, with fixed aspect ratio and increasing heights of H = 1, 2, 4, and (for dry conditions only) 8 m are performed. The key findings are: Velocity fluctuations scale as H 1/3 , consistent with the Deardorff expression for convective velocity, and implying that the turbulence correlation time scales as H 2/3 . Temperature and other scalar fluctuations scale as H −3/7 . Droplet size distributions from chambers of different sizes can be matched by adjusting the total aerosol injection rate as the horizontal cross‐sectional area (i.e., as H 2 for constant aspect ratio). Injection of aerosols at a point versus distributed throughout the volume makes no difference for polluted conditions, but can lead to cloud droplet size distribution broadening in clean conditions. Cloud droplet growth by collision and coalescence leads to a broader right tail of the distribution compared to condensation growth alone, and this tail increases in magnitude and extent monotonically as the increase of chamber height. These results also have implications for scaling within turbulent, cloudy mixed‐layers in the atmosphere, such as fog layers.

54 ENVIRONMENTAL SCIENCES↗

Observed and Bin Model Simulated Evolution of Drop Size Distributions in High-Based Cumulus Congestus Over the United Arab Emirates

This study examines microphysical processes in developing high-based cumulus congestus over the United Arab Emirates using aircraft observations and a large-eddy-simulation model with bin microphysics. A notable feature of this case is the lack of mm-sized drops despite having a liquid cloud layer >3.5 km deep, contrasting with copious large drops observed in maritime tropical cumulus congestus having a similar vertical extent. Modeled drop size distributions are similar to observations at various temperatures between 9.5 and –12°C, including the lack of mm-sized drops. Cloud dilution leads to low-to-moderate liquid water contents (~0.5–1.5 g m –3 ) in most of the cloud core, several times smaller than adiabatic values. Dilution is enhanced in the inflowing branch of the toroidal circulations associated with individual cloud thermals, which are favored regions for secondary droplet activation (activation above cloud base). Secondary activation in general contributes substantially to the droplet population. Turning it off leads to a sharp decrease in droplet concentration and increase in mean size aloft, but does little to increase rain drop production. Warm rain generation (or lack thereof) in this case is therefore determined more by the sub-cloud aerosol and the cloud base droplet size distribution (DSD) than DSD evolution aloft from secondary droplet activation. Decreasing the aerosol concentration by a factor of 10 greatly increases production of large drops via collision-coalescence. Thus, despite its high base (low temperatures) and substantial dilution, the simulated cloud is thermodynamically and dynamically capable of rapidly producing copious mm-sized drops from collision-coalescence under pristine aerosol conditions.

54 ENVIRONMENTAL SCIENCES↗

Limitations of Separate Cloud and Rain Categories in Parameterizing Collision-Coalescence for Bulk Microphysics Schemes

Warm rain collision-coalescence has been persistently difficult to parameterize in bulk microphysics schemes. We use a flexible bulk microphysics scheme with bin scheme process parameterizations, called AMP, to investigate reasons for the difficulty. AMP is configured in a variety of ways to mimic bulk schemes and is compared to simulations with the bin scheme upon which AMP is built. We find that an important limitation in traditional bulk schemes is the use of separate cloud and rain categories. When the drop size distribution is instead represented by a continuous distribution, the simulation of cloud-to-rain conversion is substantially improved. We also find large sensitivity to the threshold size to distinguish cloud and rain in traditional schemes; substantial improvement is found by decreasing the threshold from 40 to 25 μm. Neither the use of an assumed functional form for the size distribution nor the choice of predicted distribution moments has a large impact on the ability of AMP to simulate rain production. When predicting four total moments of the liquid drop size distribution, either with a traditional two-category, two-moment scheme with a reduced size threshold, or a four-moment single-category scheme, errors in the evolution of mass and the cloud size distribution are similar, but the single-category scheme has a substantially better representation of the rain size distribution. Optimal moment combinations for the single-category approach are investigated and appear to be linked more to the information content they provide for constraining the size distributions than to their correlation with collision-coalescence rates.

54 ENVIRONMENTAL SCIENCES↗

What Controls Crystal Diversity and Microphysical Variability in Cirrus Clouds?

Abstract Variability of ice microphysical properties like crystal size and density in cirrus clouds is important for climate through its impact on radiative forcing, but challenging to represent in models. For the first time, recent laboratory experiments of particle growth (tied to crystal morphology via deposition density) are combined with a state‐of‐the‐art Lagrangian particle‐based microphysics model in large‐eddy simulations to examine sources of microphysical variability in cirrus. Simulated particle size distributions compare well against balloon‐borne observations. Overall, microphysical variability is dominated by variability in the particles' thermodynamic histories. However, diversity in crystal morphology notably increases spatial variability of mean particle size and density, especially at mid‐levels in the cloud. Little correlation between instantaneous crystal properties and supersaturation occurs even though the modeled particle morphology is directly tied to supersaturation based on laboratory measurements. Thus, the individual thermodynamic paths of each particle, not the instantaneous conditions, control the evolution of particle properties.

54 ENVIRONMENTAL SCIENCES↗