Aerosol Composition, Mixing State, and Phase State of Free Tropospheric Particles and Their Role in Ice Cloud Formation
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54 ENVIRONMENTAL SCIENCES↗
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Cloud condensation nuclei activity of internally mixed particle populations at a remote marine free troposphere site in the North Atlantic Ocean
Here, this study reports results from research conducted at the Observatory of Mount Pico (OMP), 2225 m above mean sea level on Pico Island in the Azores archipelago in June and July 2017. We investigated the chemical composition, mixing state, and cloud condensation nuclei (CCN) activities of long-range transported free tropospheric (FT) particles. FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) simulations reveal that most air masses that arrived at the OMP during the sampling period originated in North America and were highly aged (average plume age > 10 days). We probed size-resolved chemical composition, mixing state, and hygroscopicity parameter ($\mathcal{κ}$) of individual particles using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX). Based on the estimated individual particle mass from elemental composition, we calculated the mixing state index, $χ$. During our study, FT particle populations were internally mixed ($χ$ of samples are between 53% and 87%), owing to the long atmospheric aging time. We used data from a miniature Cloud Condensation Nucleus Counter (miniCCNC) to derive the hygroscopicity parameter, $\mathcal{κ}$ CCNC . Combining $\mathcal{κ}$ CCNC and FLEXPART, we found that air masses recirculated above the North Atlantic Ocean with lower mean altitude had higher $\mathcal{κ}$ CCNC due to the higher contribution of sea salt particles. We used CCSEM-EDX and phase state measurements to predict single-particle $\mathcal{κ}$ ($\mathcal{κ}$ CCSEM-EDX ) values, which overlap with the lower range of $\mathcal{κ}$ CCNC measured below 0.15 % SS. Therefore, CCSEM-EDX measurements can be useful in predicting the lower bound of $\mathcal{κ}$, which can be used in climate models to predict CCN activities, especially in remote locations where online CCN measurements are unavailable.
54 ENVIRONMENTAL SCIENCES↗
Surfactants and cloud droplet activation: A systematic extension of Köhler theory based on analysis of droplet stability
The activation of aerosol particles to form cloud droplets, a necessary first step in cloud formation, controls much of the impact that aerosols have on clouds and climate. Recently, there has been a surge of interest in extending the Köhler theory of cloud droplet activation to include surface active (typically organic) as well as water-soluble (typically inorganic) aerosol components, but a systematic framework for doing this has yet to be developed. Here, we apply a droplet stability analysis to this end. Ideal and Szyszkowski–Langmuir surfactant models are analyzed to demonstrate the new approach, but the underlying theoretical framework is fundamental and model free. A key finding is that superficial densities at the cloud activation threshold (Köhler maximum) are significantly sub-monolayer, with fractional coverage ranging from 69% to 85% for the organic compounds and mixtures studied. The result, significant for model inventories of cloud condensation nuclei, is a weakening of the surfactant effect relative to expectations based on bulk sample measurements. Analytical results are obtained for the loci of Köhler maxima and applied to aerosol mixtures containing an arbitrary number of water-soluble and surfactant components.
54 ENVIRONMENTAL SCIENCES↗
New particle formation in the remote marine boundary layer
Marine low clouds play an important role in the climate system, and their properties are sensitive to cloud condensation nuclei concentrations. While new particle formation represents a major source of cloud condensation nuclei globally, the prevailing view is that new particle formation rarely occurs in remote marine boundary layer over open oceans. Here we present evidence of the regular and frequent occurrence of new particle formation in the upper part of remote marine boundary layer following cold front passages. The new particle formation is facilitated by a combination of efficient removal of existing particles by precipitation, cold air temperatures, vertical transport of reactive gases from the ocean surface, and high actinic fluxes in a broken cloud field. The newly formed particles subsequently grow and contribute substantially to cloud condensation nuclei in the remote marine boundary layer and thereby impact marine low clouds.
54 ENVIRONMENTAL SCIENCES↗
High concentrations of ice: Investigations using polarimetric radar observations combined with in situ measurements and cloud modeling (Final Report)
This DOE-funded joint project had the over-arching goal of understanding the reasons for observed size distributions of ice particles in cold clouds. Its approach involves the use of cloud models and field observations by radar and aircraft of real storms. The project addresses three major research objectives: (1) Utilize a novel polarimetric radar technique to retrieve size distributions and amounts of ice from radar data collected during the previous DOE ARM field campaigns; (2) Evaluate the results of ice microphysical retrievals using available in situ aircraft measurements and other remote sensors (e.g., vertically pointing cloud radars and wind profilers); (3) Improve the treatment of microphysical processes leading to cloud glaciation and ice multiplication in numerical cloud models. The study was performed by three research organizations: University of Oklahoma, The Hebrew University of Jerusalem, Israel, and Lund University, Sweden. The Israel and Swedish partners were funded by the sub-awards from the University of Oklahoma. Cloud modeling studies have been performed by the research teams at The Hebrew University of Jerusalem (HUJ) and Lund University to identify the origins of high concentrations of cloud ice in areas of high ice water content (HIWC). The Hebrew University Cloud Model (HUCM) with full spectral bin microphysics and the Lund University aerosol-cloud (AC) model with a hybrid bin / bulk microphysics scheme complementing HUCM were utilized for simulations. Both research teams had particular focus on secondary ice production (SIP) as one of the possible sources of enhanced ice concentration. The HUJ group suggested a novel concept of ice multiplication during droplet freezing. It is assumed that splintering and droplet fragmentation during droplet freezing takes place because of dendritic growth within a supercooled drop. The resulting simulations of SIP generated small ice in concentrations exceeding hundreds per liter similar to what was observed in the HIWC regions of the tropical storms. The Lund team explored the SIP mechanisms such as breakup of ice particles due to ice-ice collisions and ice sublimation that are expected to dominate the continental storms. They also quantified the impact of homogeneous nucleation of cloud droplets on the total number concentration of ice at very low temperatures near the tops of the clouds. Additionally, the Lund AC model is able to simulate the effect of aerosols of various types (including biological) on the cloud life cycle and the corresponding ice production. The HUCM / AC model was used to simulate one of the “golden” cases of the DOE MC3E campaign on 20 May 2011. The model output was converted into the fields of polarimetric radar variables using the polarimetric radar forward operator developed at the University of Oklahoma and compared with radar observations and in situ microphysical measurements onboard research aircraft. It was demonstrated that specific differential phase KDP is the best radar parameter to identify the HIWC areas and quantify the corresponding ice parameters. For the first time, the shape of the vertical profile of KDP was realistically reproduced by the cloud model with the KDP maximum in the dendritic growth layer (DGL) centered at the -15°C isotherm. The University of Oklahoma team has developed a methodology for polarimetric radar retrievals of such microphysical parameters of ice as ice water content (IWC), mean volume diameter (Dm), and total number concentration (Nt) of ice particles. These retrievals have been validated using in situ aircraft measurements during 6 field campaigns and proved to be quite robust and reliable. This allowed to build the first climatology of the vertical profiles of polarimetric radar variables and retrieved microphysical parameters for the three types of weather systems: continental MCSs, maritime MCSs, and tropical cyclones / hurricanes (Hu and Ryzhkov 2022). The data were collected by a multitude of the WSR-88D radars in 13 continental and 10 maritime MCSs and 11 landfalling hurricanes. The HIWC areas were identified within the examined storms and the corresponding “HIWC statistics” was compared with the “background” one without HIWC. An overarching conclusion of the study is that maritime tropical storms (MCSs and hurricanes) are characterized by smaller size ice in higher concentration compared to the continental MCSs. High ice water content in the HIWC areas is primarily caused by a strong jump in a number concentration of ice particles rather than the increase of their size compared to the “background” environment. This may point to the homogeneous nucleation of excessive amounts of supercooled droplets and / or secondary ice production as the possible origins of HIWC. Such a climatology provides a good observational reference for the modelers to evaluate the performance of their models. As an example, the in-depth analysis of the 20 May 2011 MC3E case shows that the advanced cloud models developed in the course of this study still tend to underestimate the number concentration of ice in the HIWC areas although they succeed in reproducing realistically looking vertical profiles of IWC and Nt. The results of the project research are summarized in 13 journal papers.
54 ENVIRONMENTAL SCIENCES↗
Vertical Structure and Ice Production Processes of Shallow Convective Postfrontal Clouds over the Southern Ocean in MARCUS. Part I: Observational Study
A study of the vertical structure of postfrontal shallow clouds in the marine boundary layer over the Southern Ocean is presented here. The central question of this two-part study regards cloud phase (liquid/ice) of precipitation, and the associated growth mechanisms. In this first part, data from the Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS) field campaign are analyzed, starting with a 75-h case with continuous sea surface-based thermal instability, modest surface heat fluxes, an open-cellular mesoscale organization, and very few ice nucleating particles (INPs). The clouds are mostly precipitating and shallow (tops mostly around 2 km above sea level), with weak up- and downdrafts, and with cloud-top temperatures generally around –18° to –10°C. Further, the case study is extended to three other periods of postfrontal shallow clouds in MARCUS. While abundant supercooled liquid water is commonly present, an experimental cloud-phase algorithm classifies nearly two-thirds of clouds in the 0° to –5°C layer as containing ice (cloud ice, snow, or mixed phase), implying that much of the precipitation grows through cold-cloud processes. The best predictors of ice presence are cloud-top temperature, cloud depth, and INP concentration. Measures of convective activity and turbulence are found to be poor indicators of ice presence in the studied environment. The water-phase distribution in this cloud regime is explored through numerical simulations in Part II. Significance Statement: Climate models generally predict a lower albedo than observed over the Southern Ocean, and this is largely attributed to a lack of cloudiness, especially in the postfrontal cold sector of midlatitude cyclones. This in turn may be due to an excess of ice in these simulated clouds, resulting in rapid precipitation fallout and an overly brief cloud lifespan. The objective of this study is to examine whether shallow postfrontal clouds over the Southern Ocean are dominated by supercooled drops, or by snow and ice, using data collected by a U.S. Department of Energy Atmospheric Radiation Measurement Mobile Facility deployed aboard an Australian Antarctic supply vessel. We find that these clouds contain much supercooled liquid, even though cloud-top temperatures generally are around –18° to –8°C, and that about two-thirds of the clouds just above the freezing level contain ice. Much of the precipitation appears to grow through cold-cloud processes above the freezing level, rather than drizzle/rain. Updrafts and/or turbulence in convection or in cloud-top generating cells do not initiate much ice, compared to observations elsewhere in a similar temperature range. This may be attributable to the extremely low concentration of ice nucleating particles in this environment. Ultimately, the deepest clouds with the coldest cloud tops are most likely to be ice dominated.
54 ENVIRONMENTAL SCIENCES↗
Coulomb expansion of a thin dust cloud observed experimentally under afterglow plasma conditions
The Coulomb expansion of a thin cloud of charged dust particles was observed experimentally, in a plasma afterglow. This expansion occurs due to mutual repulsion among positively charged dust particles, after electrons and ions have escaped the chamber volume. In the experiment, a two-dimensional cloud of dust particles was initially levitated in a glow-discharge plasma. The power was then switched off to produce afterglow conditions. The subsequent fall of the dust cloud was slowed by reversing the electric force, to an upward direction, allowing an extended observation. At early time, measurements of the Coulomb expansion in the horizontal direction are found to be accurately modeled by the equation of state for a uniformly charged thin disk. Finally, bouncing from the lower electrode was found to be avoided by lowering the impact velocity <100 mm/s.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Dampening of the Precipitation Response to Aerosol Pollution From Turbulence in Cumulus Clouds
Using aircraft observations and a cloud model with particle‐based microphysics, it is shown that the enhancement of drop collision‐coalescence from turbulence in clouds not only leads to earlier onset of rain in warm cumulus clouds as past studies have suggested, but also significantly dampens the precipitation susceptibility to aerosol loading. Enhanced drop coalescence from turbulence substantially increases the production of drizzle embryos just above cloud base, which in turn act as seeds that accelerate rain drop growth at mid and upper cloud levels even in highly polluted conditions. In contrast, pollution aerosols strongly inhibit rainfall when the commonly assumed gravitational‐only collision kernel is used and turbulent coalescence is neglected. Overall, turbulence‐enhanced drop coalescence strongly influences the response of warm cumulus clouds and precipitation to aerosol loading, suggesting that the effects of turbulent coalescence should be included in Earth system model representations of aerosol‐cloud‐precipitation interactions and aerosol indirect radiative forcing.
Chandrakar, Kamal Kant [NSF National Center for At↗
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↗
Understanding Aitken Mode Aerosol Variability over the Southern Ocean and Antarctica: Insights from Cloud Condensation Nuclei Data
Aitken mode aerosol particles play an important role influencing cloud properties and sustenance, acting as a reservoir of potential cloud condensation nuclei against precipitation scavenging. However, there is limited data on Aitken mode aerosols. In this study, we develop a method to estimate Aitken mode aerosol concentrations and size distribution using cloud condensation nuclei measurements (CCN) and κ-Köhler theory. The performance of this method is evaluated using scanning mobility particle sizer (SMPS) data from recent field campaigns to demonstrate its skills and applicability. The method reasonably estimates Aitken- and accumulation-mode aerosol concentrations, achieving correlations of 0.7–0.9 with only modest biases (mean fractional bias within ±23% for Aitken mode and ±34% for accumulation-mode). This method is further applied to measurements collected over the Southern Ocean and Antarctica in recent years from multiple platforms, including ground sites, aircraft, and ships, to derive Aitken and accumulation-mode aerosol concentrations. Using the derived data, we examine the seasonal cycle, latitudinal variations, and vertical distribution of aerosols. Aitken mode aerosol concentrations are elevated over the Southern Ocean and Antarctica during the austral summer similar to the accumulation mode. In the austral summer, the free troposphere has more Aitken mode aerosols and fewer accumulation mode aerosols than the boundary layer, and thus likely serves as an important source of cloud-forming aerosol while also diluting the accumulation mode.
Kang, Litai [University of Washington] (ORCID:0000↗
Variability in Ice Nucleating Particles Across Greater Houston Texas
The concentration and cloud-forming potential of a region's ice nucleating particle (INP) population have uncertain impacts on deep convective clouds. Specifically, ice nucleating particles (INPs) may affect various cloud properties related to the formation, lifetime, and precipitation of deep convective clouds. As part of the U.S. Department of Energy's TRacking Aerosol and Convection interaction ExpeRiment (TRACER) campaign, researchers from Texas A&M University deployed three Davis Rotating-drum Universal-size-cut Monitoring (DRUM) samplers throughout Greater Houston, Texas from June through September 2022. Ambient particles, collected at the surface with the DRUM samplers in four aerodynamic diameter size ranges (>3, 3–1.2, 1.2–0.34, and 0.34–0.15 μm), were analyzed in offline cold-stage ice nucleation experiments. The INP population in Greater Houston is complex, varying by site and day, but can be generalized by a weak to moderately efficient mode of INPs at −24°C and an efficient mode at −15°C. Analysis reveals that supermicron particles are largely responsible for ice nucleation warmer than −20°C across the region while submicron particles dominate at temperatures colder than −20°C. Additionally, significant spatial diversity in the INP population was observed, with differences in mean nucleation temperature between sites for nearly every size cut. Although INP concentrations were typically ∼0.08 L −1 at −20°C throughout the campaign, a notable region-wide increase in INP concentration for particles freezing at temperatures warmer than −20°C occurred from mid-August to mid-September. This comprehensive characterization of Greater Houston's INP population, including spatial, temporal, and particle size variations, can help constrain ice microphysics parameterizations in weather and climate models.
Thompson, Seth A. [Texas A & M Univ., College Stat↗
Modeling impacts of ice-nucleating particles from marine aerosols on mixed-phase orographic clouds during 2015 ACAPEX field campaign
Abstract. A large fraction of annual precipitation over the western United States comes from wintertime orographic clouds associated with atmospheric rivers (ARs). Transported African and Asian dust and marine aerosols from the Pacific Ocean may act as ice-nucleating particles (INPs) to affect cloud and precipitation properties over the region. Here we explored the effects of INPs from marine aerosols on orographic mixed-phase clouds and precipitation at different AR stages for an AR event observed during the 2015 ACAPEX field campaign under low dust (<0.02 cm−3) conditions. Simulations were conducted using the chemistry version of the Weather Research and Forecasting Model coupled with the spectral-bin microphysics at 1 km grid spacing, with ice nucleation connected with dust and marine aerosols. By comparing against airborne and ground-based observations, accounting for marine INP effects improves the simulation of AR-precipitation. The marine INPs enhance the formation of ice and snow, leading to less shallow warm clouds but more mixed-phase and deep clouds, as well as to a large spillover effect of precipitation after AR landfall. The responses of cloud and precipitation to marine INPs vary with the AR stages, with more significant effects before AR landfall and post-AR than after AR landfall, mainly because the moisture and temperature conditions change with the AR evolution. This work suggests weather and climate models need to consider the impacts of marine INPs since their contribution is notable under low dust conditions despite the much lower relative ice nucleation efficiency of marine INPs.
54 ENVIRONMENTAL SCIENCES↗
ARMing the Edge: Designing Edge Computing–Capable Machine Learning Algorithms to Target ARM Doppler Lidar Processing
Abstract There is a need for long-term observations of cloud and precipitation fall speeds in validating and improving rainfall forecasts from climate models. To this end, the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility Southern Great Plains (SGP) site at Lamont, Oklahoma, hosts five ARM Doppler lidars that can measure cloud and aerosol properties. In particular, the ARM Doppler lidars record Doppler spectra that contain information about the fall speeds of cloud and precipitation particles. However, due to bandwidth and storage constraints, the Doppler spectra are not routinely stored. This calls for the automation of cloud and rain detection in ARM Doppler lidar data so that the spectral data in clouds can be selectively saved and further analyzed. During the ARMing the Edge field experiment, a Waggle node capable of performing machine learning applications in situ was deployed at the ARM SGP site for this purpose. In this paper, we develop and test four algorithms for the Waggle node to automatically classify ARM Doppler lidar data. We demonstrate that supervised learning using a ResNet50-based classifier will classify 97.6% of the clear-air images and 94.7% of cloudy images correctly, outperforming traditional peak detection methods. We also show that a convolutional autoencoder paired with k -means clustering identifies 10 clusters in the ARM Doppler lidar data. Three clusters correspond to mostly clear conditions with scattered high clouds, and seven others correspond to cloudy conditions with varying cloud-base heights.
54 ENVIRONMENTAL SCIENCES↗
Tracking Aerosol Convection Interactions Experiment (TRACER) Field Campaign Report
Convective clouds serve a critical role in the Earth’s energy and water cycles through their transport of heat, moisture, momentum, and chemical species through the troposphere driving the global circulation (e.g., Hartmann et al. 1984, Del Genio et al. 2012, Su et al. 2014). On more local scales, convective clouds impact the atmospheric heating profile through diabatic heating effects, removal of water from the atmospheric column through precipitation, and conditioning of the local environment impacting further development of clouds (e.g., Sullivan and Voigt 2021). These critical roles underscore the importance of realistic representation of convective processes across scales of models from large-eddy simulation (LES), to convection-permitting models (CPM; e.g., Kendon et al. 2020, Marinescu et al. 2021), to numerical weather prediction (NWP) models used for operational weather forecasting, to Earth system models used to predict climate sensitivity (Sanderson et al. 2011, Sherwood et al. 2014, Tomassini et al. 2014, Zhao et al. 2016, Cronin et al. 2017). A key component of improving model representation of convective clouds is better quantification and parameterization of updraft microphysics and dynamics, including their interactions with the surrounding environment and storm organization (Bony et al. 2015, Hagos and Houze 2016, Donner et al. 2016, Morrison et al. 2020). Aerosol is an important environmental factor that could affect convective clouds and precipitation since cloud droplet and ice formation processes are initiated by it. Andrae et al. (2004) hypothesized that aerosols associated with increased biomass burning particles acting as cloud condensation nuclei (CCN) result in smaller and more monodisperse cloud droplets leading to suppression of warm rain formation, ultimately leading to more cloud water being lofted above the freezing level based on observations in the Amazon region. The subsequent increase in latent heat release increases the buoyancy of rising convective parcels invigorating the deep convection. This work was followed by a description of the theoretical basis for this “cold-phase invigoration” by Rosenfeld et al. (2008), who argued that it could have a significant effect for deep convective clouds with warm cloud-bases. Several modeling studies (e.g., Khain et al. 2005, 2009, van den Heever et al. 2006, Fan et al. 2007, 2009, 2012, Lee et al. 2008, Storer et al. 2010, Lebo et al. 2012, Storer and van den Heever 2013, Chen et al. 2020, Dagan et al. 2022) have investigated these aerosol-convection interactions and the environmental factors that influence their relative importance and magnitude. More recently, several studies have indicated that “warm-phase invigoration”, the enhancement of convection through condensational heating, also appears to play a role in enhancing both shallow cumuli (Seiki and Nakajima 2014, Saleeby et al 2015) and deeper tropical convection (Lebo and Seinfeld 2011, Khain et al. 2012, Sheffield et al 2015, Fan et al. 2018, Igel and van den Heever 2021), as well as Houston thunderstorms (Fan et al. 2007, 2020). However, still other studies have provided additional evidence of systematic biases in simulated convective outflow ice size distribution properties, which are consistent with a lack of poorly understood secondary ice production within convective updrafts (e.g., Fridlind et al. 2017). To help address these critical gaps in our understanding of cloud processes, aerosol processes and aerosol-cloud interactions, the Tracking Aerosol Convection Interactions Experiment was designed building upon efforts by the Aerosol, Cloud, Precipitation and Climate (ACPC) Initiative (http://acpcintiative.org/), a joint effort of the International Geosphere-Biosphere Programme (IGBP) and the World Climate Research Program (WCRP) that focused on resolving uncertainties in the interactions between aerosol and clouds towards better understanding the role that these interactions play in the climate system. The TRACER campaign was motivated by recommendations from a number of pilot studies undertaken by ACPC (van den Heever et al. 2017, Fridlind et al. 2019, Hu et al. 2019, Fan et al. 2020, Marinescu et al. 2021, Hernandez-Deckers et al. 2022) that pointed towards the southeastern Texas region as a locale where aerosol-convection interactions could be studied owing to the copious occurrence of isolated convection during the summer months accompanied by diverse and significant sources of aerosols from both anthropogenic and natural sources. The TRACER campaign began on 01 October 2021 and extended through 30 September 2022 with an intensive operational period (IOP) during June-September 2022. Three main sites (Table 1) were managed by the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility.
54 ENVIRONMENTAL SCIENCES↗
New Particle Formation and Growth to Climate-Relevant Aerosols at a Background Remote Site in the Western Himalaya
New particle formation (NPF) can influence the Earth’s radiative budget when the newly formed particles grow to climate-relevant sizes. Here, we present analysis of 21-months of continuous aerosol size distribution measurements at a background remote site in the western Himalaya and provide observational evidence that newly formed particles grow to cloud condensation nuclei (CCN)-active sizes (i.e. >20-100 nm in diameter). Out of total 55 NPF events, 38 (66%) events occurred in the pre-monsoon season (March-May). NPF events were classified into those with and without pollution influence as polluted and cleaner, respectively, using black carbon data. The analysis of air mass age, based on the ratio of number concentration of Aitken to accumulation mode aerosols, indicated that NPF occurred in the relatively cleaner air masses reaching to the site. The median formation rate of 10 nm particles and particle growth rates for cleaner events were three-fold and two-fold, respectively, higher than polluted events. We present the first estimates of the survival probability of newly formed particles to 50 nm and 100 nm size, which was not attempted in an Indian environment previously. The survival probability to 50 nm particles ranged from 44 to 98%, with a mean and standard deviation of 82 ± 18%. On average, ~60% of the particles surviving to 50 nm survived to 100 nm, making the overall survival probability of 100 nm to 53 ± 31%. This indicates that the probability of nucleated particles growing to CCN-active sizes under a large source of condensing vapor (transported from nearby lower-altitude regions) and low pre-existing particle concentrations (background mountain site) is high compared to the previous studies. These findings highlight the importance of the efficiency of nucleation events for producing CCN, which is a critical basis of aerosol indirect effects.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Vertical Aerosol Profiling during SAIL (VAPS) Field Campaign Report
To more fully address the science goals of the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility’s Surface Atmosphere Integrated Field Laboratory (SAIL) campaign, particularly the key science question of “How strongly do aerosols affect the surface energy and water balance by altering clouds, precipitation, and surface albedo, and how do these impacts vary seasonally?”, our campaign added instrumentation to planned tethered balloon system (TBS) flights in May and July of 2022. A key aspect of aerosol-cloud interactions is understanding cloud condensation nuclei (CCN) and ice nucleating particle (INP) populations, and how they vary seasonally and spatially. Because the interactions between aerosols and clouds is the target of this work, vertical distributions are particularly important to evaluate. Measurements of aerosol at ground level, below-cloud, and in-cloud will allow a better understanding of the airmasses that are feeding cloud-active particles into low- and mid-level clouds. Measurements of INP and aerosol populations often differ between the ground and aloft, with relationships that likely depend on regional and seasonal. Because of this, collocated measurements of aerosol, CCN, and INP, across different seasons, are crucial to reducing uncertainties in relationships between ground-level and cloud-base aerosol populations. Our campaign added online measurements of CCN using a compact CCN counter and offline filter collections for measurement of INP populations to the SAIL campaign TBS flights in May and July of 2022. The CCN instrument, the CloudPuck, flew and successfully collected data for a total of eight flights across both campaign periods. The IcePuck flew for most flights during the same period. Both instruments have continued to be used for other campaign requests in the SAIL domain. Analysis of this data was proposed through a concurrent DOE Atmospheric System Research (ASR) project submission, which was not funded in 2022. A similar proposal, which would involve analysis of the samples and data collected from this campaign, has been resubmitted in 2023 but a funding decision has not yet been made. If the proposal is again declined, we will seek other resources to ensure that this data can be analyzed.
54 ENVIRONMENTAL SCIENCES↗
Evaluation of ARM tethered-balloon system instrumentation for supercooled liquid water and distributed temperature sensing in mixed-phase Arctic clouds
A tethered-balloon system (TBS) has been developed and is being operated by Sandia National Laboratories (SNL) on behalf of the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) User Facility in order to collect in situ atmospheric measurements within mixed-phase Arctic clouds. Periodic tethered-balloon flights have been conducted since 2015 within restricted airspace at ARM's Advanced Mobile Facility 3 (AMF3) in Oliktok Point, Alaska, as part of the AALCO (Aerial Assessment of Liquid in Clouds at Oliktok), ERASMUS (Evaluation of Routine Atmospheric Sounding Measurements using Unmanned Systems), and POPEYE (Profiling at Oliktok Point to Enhance YOPP Experiments) field campaigns. The tethered-balloon system uses helium-filled 34 m 3 helikites and 79 and 104 m 3 aerostats to suspend instrumentation that is used to measure aerosol particle size distributions, temperature, horizontal wind, pressure, relative humidity, turbulence, and cloud particle properties and to calibrate ground-based remote sensing instruments. Supercooled liquid water content (SLWC) sondes using the vibrating-wire principle, developed by Anasphere Inc., were operated at Oliktok Point at multiple altitudes on the TBS within mixed-hase clouds for over 200 h. Sonde-collected SLWC data were compared with liquid water content derived from a microwave radiometer, Ka-band ARM zenith radar, and ceilometer at the AMF3, as well as liquid water content derived from AMF3 radiosonde flights. The in situ data collected by the Anasphere sensors were also compared with data collected simultaneously by an alternative SLWC sensor developed at the University of Reading, UK; both vibrating-wire instruments were typically observed to shed their ice quickly upon exiting the cloud or reaching maximum ice loading. Temperature sensing measurements distributed with fiber optic tethered balloons were also compared with AMF3 radiosonde temperature measurements. Combined, the results indicate that TBS-distributed temperature sensing and supercooled liquid water measurements are in reasonably good agreement with remote sensing and radiosonde-based measurements of both properties. From these measurements and sensor evaluations, tethered-balloon flights are shown to offer an effective method of collecting data to inform and constrain numerical models, calibrate and validate remote sensing instruments, and characterize the flight environment of unmanned aircraft, circumventing the difficulties of in-cloud unmanned aircraft flights such as limited flight time and in-flight icing.
47 OTHER INSTRUMENTATION↗
Physical science research needed to evaluate the viability and risks of marine cloud brightening
Marine cloud brightening (MCB) is the deliberate injection of aerosol particles into shallow marine clouds to increase their reflection of solar radiation and reduce the amount of energy absorbed by the climate system. From the physical science perspective, the consensus of a broad international group of scientists is that the viability of MCB will ultimately depend on whether observations and models can robustly assess the scale-up of local-to-global brightening in today’s climate and identify strategies that will ensure an equitable geographical distribution of the benefits and risks associated with projected regional changes in temperature and precipitation. To address the physical science knowledge gaps required to assess the societal implications of MCB, we propose a substantial and targeted program of research—field and laboratory experiments, monitoring, and numerical modeling across a range of scales.
54 ENVIRONMENTAL SCIENCES↗