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DOE OSTI2024

Influence of open ocean biogeochemistry on aerosol and clouds: Recent findings and perspectives

Aerosols and clouds are key components of the marine atmosphere, impacting the Earth’s radiative budget with a net cooling effect over the industrial era that counterbalances greenhouse gas warming, yet with an uncertain amplitude. Here we report recent advances in our understanding of how open ocean aerosol sources are modulated by ocean biogeochemistry and how they, in turn, shape cloud coverage and properties. We organize these findings in successive steps from ocean biogeochemical processes to particle formation by nucleation and sea spray emissions, further particle growth by condensation of gases, the potential to act as cloud condensation nuclei or ice nucleating particles, and finally, their effects on cloud formation, optical properties, and life cycle. We discuss how these processes may be impacted in a warming climate and the potential for ocean biogeochemistry—climate feedbacks through aerosols and clouds.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Aircraft-derived particle fluxes distinguish entrainment zone and decoupled layer nucleation in marine boundary layers

The vertical distribution of freshly nucleated aerosol particles in the marine boundary layer remains poorly constrained, limiting our ability to represent new particle formation in climate models. Here we characterize 3–10 nm particle events, termed small particle events (SPEs), by deriving their vertical turbulent fluxes from aircraft measurements during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. To overcome stationarity limitations of traditional eddy covariance methods, we applied continuous wavelet transform analysis to data collected during June–July 2017 and January–February 2018 flights over the Azores. Our flux-based analysis revealed two distinct SPE scenarios with different vertical structures and spatial extents. The first featured nucleation in the entrainment zone, where free tropospheric air entrains into the boundary layer. The second showed nucleation in the decoupled layer, a stratified region between the well-mixed surface layer and cloud-topped upper boundary layer. In both cases, convergence of air masses from different layers diluted preexisting aerosol surface area to very low levels, creating conditions favorable for nucleation and generating strong downward particle fluxes. SPEs occurred in 15 % of flights, challenging prevailing theoretical expectations that new particle formation should rarely occur in marine boundary layers due to high condensation and coagulation sink capacity of sea spray aerosols. Aircraft-derived particle fluxes provide first observational constraints on the vertical location and source strength of likely nucleation regions in the remote marine boundary layer, improving aerosol source representations in climate models and reducing uncertainties in aerosol-cloud interactions.

Rasheeda Satheesh, Ajmal [North Carolina State Uni↗

DOE OSTI2024

Baselining the Indirect Effect by Improving Quantification of Sea Spray and Marine Sources at Ascension Island (Final Report)

Oceans cover two-thirds of the Earth and understanding the interactions of aerosols with clouds in these large marine regions requires quantifying the man-made contributions to the budget of cloud-drop forming particles (known as cloud condensation nuclei, or CCN) relative to the non-manmade “baseline” conditions and understanding the meteorology of boundary layer clouds. Modeling studies have shown substantial uncertainties and sensitivities to natural marine CCN sources, meaning that to reduce uncertainties in indirect effects we must be able to better quantify the CCN budget in ocean regions. While models provide important constraints on these uncertainties, actually reducing uncertainties requires substantial observations in open-ocean and coastal regions in order to establish the baseline on which manmade emissions are added. The tropical South Atlantic Ocean is one of the least-sampled regions of the planet, making the comprehensive measurements of the Department of Energy Atmospheric Radiation Measurement Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign provides the longest record of aerosol size distribution measurements from a differential mobility analyzer in a cloud-influenced marine location in the ARM database, with 17 months of ground-based aerosol size distribution measurements. This project addressed the research topic of Aerosol-Cloud Interactions (ACI) by supporting three publications from the LASIC measurements: 1. The ARM measurements were combined with a new value-added technique that was pioneered by the Russell group for quantifying sea salt. This quantification of sea salt uses supermicron scattering measurements for retrieving reasonable sea spray mass concentrations, providing the best-available, observationally-constrained estimate of the sea spray mode properties when supermicron size distribution measurements are not available. 2. The fitted modes of the distribution were used to investigate the signatures of cloud processing for very clean to very smoky aerosol conditions, revealing not only differences in the particles that activate in clouds but also in the mechanisms that control that droplet formation process. In clean air, the size required to form a cloud droplet is influenced by the number of particles, as well as how quickly particles take up water during growth in cloud. 3. Building on this aerosol characterization, cloud and meteorological conditions were used to evaluate aerosol-related changes in cloud albedo and optical depth. We introduced a new method of decomposing the impact of aerosols on clouds known as the Twomey effect by incorporating retrieved supersaturation from two independent sets of observations to constrain the feedback of aerosol particles on cloud properties. The method quantifies the reduction of the Twomey effect at high aerosol concentrations, which has never been explained quantitatively by observations. In addition, the results provide the first direct validation for the conditions observed in the tropical South Atlantic of a parcel-based approach that is embedded in many climate models. Together these findings illustrate how ARM extended field campaigns in stratocumulus-covered regions can be used to constrain ACI processes with direct observations, providing specific radiative effects without models. By making such process-specific constraints available to improve ACI in global climate models, ARM observations play a key role in supporting model development.

58 GEOSCIENCES↗

DOE OSTI2025

Coalescence-Induced Spontaneous Shedding of Microdroplets on Superhydrophobic Surfaces Featuring Enclosed Micropillars with Hierarchical Roughness

This study investigated water vapor condensation on superhydrophobic surfaces (SHSs) featuring micropillars enclosed by wall lattices and having three-tier hierarchical roughness. A total of five samples were created with three (NW-J, W200-J and W400-J samples) having large micropillar depth (~6 μm) and two (NW-S and W200-S samples) having small micropillar depth (~1 μm). Two distinct condensate removal modes were observed during condensation: coalescence-induced jumping on samples with large micropillar depth and coalescence-induced shedding on samples with small micropillar depth. The results showed that the diameter of the shedding droplet on the W200-S sample having small micropillar depth could be as small as 107 μm, as compared to the theoretical critical diameter of 267 μm for gravitational shedding on the same sample. The enhanced functionality of the three-tier nanotextures on the W200-S sample could effectively suppress localized pinning of the three-phase contact line and Wenzel neck formation during the growth of condensate droplets. Consequently, during multidroplet coalescence, the released surface energy easily overcomes the solid–liquid adhesion, leading to spontaneous shedding of merged droplets. The inclusion of the wall lattice aids condensate growth by the droplet self-alignment along the walls and promoting coalescence. As a result, the W200-S sample exhibited the highest condensate collection as well. In conclusion, the proposed surface design has great potential for scaling up and implementation in heating, ventilation, and air-conditioning equipment due to the simplicity of the surface morphology and the facile spray-coating method used to achieve hierarchical roughness.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

A multiphase flow model of water droplets dielectrophoretic-induced air dehumidification phenomena

Air humidity in indoor spaces plays a critical role in human comfort and health. Dehumidification systems are used for building humidity controls, but they can take significant energy consumption, especially in geographic locations with high outdoor humidity and warm climates. Consequently, there is a growing demand for innovative dehumidification processes that consume minimal energy. Dielectrophoretic air dehumidification represents one such promising approach. However, it has not garnered significant attention due to the absence of engineering models and simulation tools capable of evaluating its performance and limitations at large-scale airflows. A new numerical multiphase CFD model, which is also experimentally validated, is developed in a customized Reacting Foam solver based on OpenFOAM® version 9. The newly developed model seeks to decrease substantial energy consumption and lower costs by leveraging the dielectrophoretic phenomenon to regulate moisture levels in the air. The solver integrates a hybrid Eulerian-Lagrangian framework to track the droplet's trajectory and growth rate while solving the continuum equations for the moist air. An electrospray produces electrically charged droplets, which grow during their in-flight trajectories as water vapor condenses onto their surfaces. The role of electrostatic forces in promoting vapor condensation within a high-gradient electrical field is investigated, and the dielectrophoretic vapor nucleation process on charged water droplets is discussed. The CFD model was validated against results from the literature and from proof-of-concept experiments conducted by the authors, which showed a 2 % air dehumidification with a single electrospray and airflow rate of 5 cubic feet per minute. The simulation results indicated that augmenting the number of electrically charged spray droplets increased the dehumidification of the air to 25 %. The initial mean droplet diameter, the orientation of the injector and relative humidity significantly influence the assessment of dehumidification. As a result, scaling up this approach to larger airflow volumes is identified as a potential future research direction.

42 ENGINEERING↗

DOE OSTI2025

Analysis of soot formation from aviation fuels in laminar counterflow flames

Combustion emissions from aviation contribute to the formation of condensation trail (contrail) that can lead to the formation of anthropogenic cirrus clouds. Ice particles that form contrails are observed to have a linear correlation with soot particle number density. Synthetic aviation fuels (SAFs) offer a promising route to mitigate the production of soot particles while also increasing energy security. Although studies have focused on combustion and spray behavior, the detailed investigation of soot formation processes for different jet fuels and their impact on models for computational fluid dynamics (CFD) applications is not well understood. Moreover, experimental measurements of soot for canonical flames using Synthetic aviation fuels (SAF) for model validation remain scarce. To address this, we use employed the Lawrence Livermore National Laboratory (LLNL) detailed soot model based on the discrete sectional method. Additionally, we develop two reduced chemical mechanisms for Jet-A and Alcohol-to-Jet (C1) that are suitable for turbulent flame simulations and couple them with the Hybrid Method of Moments (HMOM). The detailed and reduced model frameworks are validated against experimental measurements of soot volume fraction (ƒ ν ) from a counterflow burner experiment previously reported in the literature. Given the good agreement between modeling results and experimental measurements for the (1) spatial distribution of ƒ ν and (2) the non-linear variation of peak ƒ ν with strain rate, we further investigate the modeled sub-processes (nucleation, condensation, surface growth, and oxidation) using the LLNL model to analyze the assumptions in the reduced model framework. Furthermore, the results indicate a significant contribution from resonant radicals to the surface growth of soot particles, which are not accounted for in the current implementation of HMOM and could help reconcile soot predictions by the reduced model with observations.

Counterflow↗

DOE OSTI2025

Shoreline wave breaking strongly enhances the coastal sea spray aerosol population: Climate and air quality implications

Sea spray aerosol (SSA) emission is a major source of atmospheric aerosols, influencing global climate and coastal air quality. Much of our knowledge about SSA derives from coastal observations near shorelines, but whether and when these observations accurately represent open oceans remain unclear. Here, we show that strong nearshore SSA production during high-wave periods greatly enhances downwind cloud condensation nuclei (CCN) and aerosol mass concentrations. Strong shoreline wave breaking is widespread globally, and swell waves, which are decoupled from local winds, play a dominant role in many coastal regions. Therefore, extrapolating results based on coastal measurements to open oceans may significantly overestimate SSA concentration and its contribution to CCN and, by extension, the impact of SSA on clouds and climate. Additionally, the strong enhancement of coastal aerosol population by shoreline wave breaking and its environmental impact on coastal communities cannot be captured by current regional models, which do not parameterize nearshore SSA generation using wave energy or completely neglect it.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Aerosol size distribution properties associated with cold-air outbreaks in the Norwegian Arctic

The aerosol particles serving as cloud condensation and ice nuclei contribute to key cloud processes associated with cold-air outbreak (CAO) events but are poorly constrained in climate models due to sparse observations. Here we retrieve aerosol number size distribution modes from measurements at Andenes, Norway, during the Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) and at Zeppelin Observatory, approximately 1000 km upwind from Andenes at Svalbard. During CAO events at Andenes, the sea-spray-mode number concentration is correlated with strong over-ocean winds with a mean of 8±4 cm −3 that is 71 % higher than during non-CAO conditions. Additionally, during CAO events at Andenes, the mean Hoppel minimum diameter is 6 nm smaller than during non-CAO conditions, though the estimated supersaturation is lower, and the mean number concentration of particles that likely activated in-cloud is 109±61 cm −3 with no statistically significant difference from the non-CAO mean of 99±66 cm −3 . For CAO trajectories between Zeppelin Observatory and Andenes, the upwind-to-downwind change in number concentration is the largest for the accumulation mode with a mean decrease of 93±95 cm −3 , likely attributable primarily to precipitation scavenging. These characteristic properties of aerosol number size distributions during CAO events provide guidance for evaluating CAO aerosol–cloud interaction processes in models.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Chemical Composition and Mixing State of Wintertime Aerosol from the European Arctic Site of Ny-Ålesund, Svalbard

The Arctic is rapidly warming, and aerosols play an increasingly important role by scattering and absorbing sunlight and by participating in cloud formation. Their optical and cloud-forming properties depend on the mixing state and chemical composition, but observations of these features remain limited. This study comprehensively characterizes 25,254 individual particles collected at Ny-Ålesund, Svalbard (November −December 2020), using microspectroscopy techniques to investigate their size, morphology, mixing state, and chemical composition. Fresh sea salt aerosols (SSA) were identified as the most abundant (∼85%), of the total observed aerosol population, with potential sources from sea spray and blowing snow. Air masses originating from the Arctic Ocean surrounding Svalbard likely contribute to increased concentrations of sub-micrometer “Fresh SSA” particles. “Aged SSA” particles (7.4%) are enriched in sulfur and nitrogen, compared to “Fresh SSA”. These elevated ratios may result from various atmospheric aging processes including the uptake of sulfuric and nitric acids. Here, our results suggest that aged SSA, with sizes larger than 300 nm, likely underwent chlorine depletion by sulfuric and nitric acids during transport. Additionally, elemental analysis reveals that both fresh and aged SSA can mix with dust particles, regardless of the SSA size (49.9% in sub-micrometer size and 50.1% in super-micrometer size, respectively). Dust particles are efficient ice-nucleating particles (INPs), and SSA is known to act as cloud condensation nuclei (CCN), and therefore, their mixtures may inherit both properties. The non-negligible number (4.4%) of SSA-dust mixtures underscores the importance of these particles as potential sources of CCN and INP in the Arctic atmosphere.

Arctic↗