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At least 127 records · Page 7

Aerosol–Ice Formation Closure: A Southern Great Plains Field Campaign

Prediction of ice formation in clouds presents one of the grand challenges in the atmospheric sciences. Immersion freezing initiated by ice-nucleating particles (INPs) is the dominant pathway of primary ice crystal formation in mixed-phase clouds, where supercooled water droplets and ice crystals coexist, with important implications for the hydrological cycle and climate. However, derivation of INP number concentrations from an ambient aerosol population in cloud-resolving and climate models remains highly uncertain. We conducted an aerosol–ice formation closure pilot study using a field-observational approach to evaluate the predictive capability of immersion freezing INPs. The closure study relies on collocated measurements of the ambient size-resolved and single-particle composition and INP number concentrations. The acquired particle data serve as input in several immersion freezing parameterizations, which are employed in cloud-resolving and climate models, for prediction of INP number concentrations. We discuss in detail one closure case study in which a front passed through the measurement site, resulting in a change of ambient particle and INP populations. We achieved closure in some circumstances within uncertainties, but we emphasize the need for freezing parameterization of potentially missing INP types and evaluation of the choice of parameterization to be employed. Overall, this closure pilot study aims to assess the level of parameter details and measurement strategies needed to achieve aerosol–ice formation closure. Furthermore, the closure approach is designed to accurately guide immersion freezing schemes in models, and ultimately identify the leading causes for climate model bias in INP predictions.

58 GEOSCIENCES↗

Dataset for "Development of heterogeneous ice nucleation rate coefficient parameterizations from ambient measurements"

Ice nucleating particles (INPs) are a rare subset of particles that can have an outsized impact relative to their prevalence. To simulate INP variability, models require parameterizations for the most important sources of INPs. Most parameterizations in the literature were developed from laboratory experiments that used proxies for ambient particles. Whether these laboratory models effectively represent ambient aerosol is still not well understood and parameterizations developed from field measurements may be more atmospherically relevant. Expanding on previous work in which we used an ice chamber and an single particle mass spectrometer (SPMS) to characterize INP composition, we use the combined measurements to calculate heterogeneous ice nucleation rate coefficients for ambient particles. We find good agreement between our results for dust and sea spray aerosol with previous results. We also determine the relative contribution of each measurement to the total measurement uncertainty using a Monte Carlo approach and find that the biggest source of uncertainty is the sampling efficiency of the SPMS.

Cornwell, Gavin C↗

“Experimental investigation of the governing parameters of atmospheric ice nucleation using field-collected and laboratory generated aerosol particles and its application in cloud resolving models” (Final Report)

The objective of this research project is to improve our understanding of the role of aerosol particles acting as ice-nucleating particles (INPs) which in turn define the mixed-phase and cirrus cloud radiative properties and thus climate. The focus is placed on how the physicochemical particle population properties determine the particles’ ability to initiate ice nucleation. This research project combined micro-spectroscopic particle analysis, experimental ice nucleation studies, and model sensitivity studies to advance our predictive capability of the formation of mixed-phase and cirrus clouds. These project activities have led to new ice nucleation data from laboratory generated and ambient (authentic) aerosol particles furthering process-level understanding, insights in the role of organic aerosol in ice formation, and advancements in the interpretation and parameterization of ice nucleation.

54 ENVIRONMENTAL SCIENCES↗

Stochastic nucleation processes and substrate abundance explain time-dependent freezing in supercooled droplets

Atmospheric immersion freezing (IF), a heterogeneous ice nucleation process where an ice nucleating particle (INP) is immersed in supercooled water, is a dominant ice formation pathway impacting the hydrological cycle and climate. Implementation of IF derived from field and laboratory data in cloud and climate models is difficult due to the high variability in spatio-temporal scales, INP composition, and morphological complexity. We demonstrate that IF can be consistently described by a stochastic nucleation process accounting for uncertainties in the INP surface area. This approach accounts for time-dependent freezing, a wide range of surface areas and challenges phenomenological descriptions typically used to interpret IF. The results have an immediate impact on the current description, interpretation, and experiments of IF and its implementation in models. The findings are in accord with nucleation theory, and thus should hold for any supercooled liquid material that nucleates in contact with a substrate.

54 ENVIRONMENTAL SCIENCES↗

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↗

Impacts of secondary ice production on Arctic mixed-phase clouds based on ARM observations and CAM6 single-column model simulations

For decades, measured ice crystal number concentrations have been found to be orders of magnitude higher than measured ice-nucleating particle number concentrations in moderately cold clouds. This observed discrepancy reveals the existence of secondary ice production (SIP) in addition to the primary ice nucleation. However, the importance of SIP relative to primary ice nucleation remains highly unclear. Furthermore, most weather and climate models do not represent SIP processes well, leading to large biases in simulated cloud properties. This study demonstrates a first attempt to represent different SIP mechanisms (frozen raindrop shattering, ice–ice collisional breakup, and rime splintering) in a global climate model (GCM). The model is run in the single column mode to facilitate comparisons with the Department of Energy (DOE)'s Atmospheric Radiation Measurement (ARM) Mixed-Phase Arctic Cloud Experiment (M-PACE) observations. We show the important role of SIP in four types of clouds during M-PACE (i.e., multilayer, single-layer stratus, transition, and frontal clouds), with the maximum enhancement in ice crystal number concentrations up to 4 orders of magnitude in moderately supercooled clouds. We reveal that SIP is the dominant source of ice crystals near the cloud base for the long-lived Arctic single-layer mixed-phase clouds. The model with SIP improves the occurrence and phase partitioning of the mixed-phase clouds, reverses the vertical distribution pattern of ice number concentrations, and provides a better agreement with observations. The findings of this study highlight the importance of considering SIP in GCMs.

54 ENVIRONMENTAL SCIENCES↗

Annual cycle observations of aerosols capable of ice formation in central Arctic clouds

The Arctic is warming faster than anywhere else on Earth, prompting glacial melt, permafrost thaw, and sea ice decline. These severe consequences induce feedbacks that contribute to amplified warming, affecting weather and climate globally. Aerosols and clouds play a critical role in regulating radiation reaching the Arctic surface. However, the magnitude of their effects is not adequately quantified, especially in the central Arctic where they impact the energy balance over the sea ice. Specifically, aerosols called ice nucleating particles (INPs) remain understudied yet are necessary for cloud ice production and subsequent changes in cloud lifetime, radiative effects, and precipitation. Here, we report observations of INPs in the central Arctic over a full year, spanning the entire sea ice growth and decline cycle. Further, these observations are size-resolved, affording valuable information on INP sources. Our results reveal a strong seasonality of INPs, with lower concentrations in the winter and spring controlled by transport from lower latitudes, to enhanced concentrations of INPs during the summer melt, likely from marine biological production in local open waters. This comprehensive characterization of INPs will ultimately help inform cloud parameterizations in models of all scales.

54 ENVIRONMENTAL SCIENCES↗

Freezing Processes in Southern Ocean Mixed Phase Clouds (Final Technical Report)

Southern Ocean (SO) low-level clouds remain a challenge for Earth system models to represent accurately. This project utilized DOE ARM observations and the Community Atmosphere Model (CAM) to improve process-level understanding of aerosol-cloud interactions and cloud microphysics for SO mixed-phase clouds. Specifically, our efforts include two main topics: 1) investigate the SO aerosol, cloud condensation nuclei (CCN), and ice nucleating particle (INP) population based on observations and determine predictive skill of simulating SO INPs, and 2) assess the ice formation pathways, including ice nucleation and secondary ice production, in SO mixed phase clouds utilizing a combination of observations and modeling tools. Studies focused on SO aerosol and INP resulted four manuscripts. Ice formation pathways in SO mixed phase clouds were investigated, revealing observed evidence of SIP active across all mixed phase temperatures. However, a key finding of this project is that despite significant progress in predicting SO INPs, the role of INP variability in SO cloud phase, precipitation, and radiative properties remain unknown due to challenges in microphysics parameterizations.

54 ENVIRONMENTAL SCIENCES↗

Primary and secondary ice production: interactions and their relative importance

A discrepancy of up to 5 orders of magnitude between ice crystal and ice nucleating particle (INP) number concentrations was found in the measurements, indicating the potentially important role of secondary ice production (SIP) in the clouds. However, the interactions between primary and SIP processes and their relative importance remain unexplored. In this study, we implemented five different ice nucleation schemes as well as physical representations of SIP processes (i.e., droplet shattering during rain freezing, ice-ice collisional break-up, and rime splintering) in the Community Earth System Model version 2 (CESM2). We ran CESM2 in the single column mode for model comparisons with the DOE Atmospheric Radiation Measurement (ARM) Mixed-Phase Arctic Cloud Experiment (M-PACE) observations. We found that the model experiments with aerosol-aware ice nucleation schemes and SIP processes yield the best simulation results for the M-PACE single-layer mixed-phase clouds. We further investigated the relative importance of ice nucleation and SIP to ice number and cloud phase as well as interactions between ice nucleation and SIP in the M-PACE single-layer mixed-phase clouds. Our results show that SIP contributes 80 % to the total ice formation and transforms ~30 % of pure liquid-phase clouds simulated in the model experiments without considering SIP into mixed-phase clouds. The SIP is not only a result of ice crystals produced from ice nucleation, but also competes with the ice nucleation by reducing the number concentrations of cloud droplets and cloud-borne dust INPs. Conversely, strong ice nucleation also suppresses SIP by glaciating mixed-phase clouds and thereby reducing the amount of precipitation particles (rain and graupel).

54 ENVIRONMENTAL SCIENCES↗

Characterization and application of a high-resolution microfluidic device in atmospheric ice nucleation research and integrated science teaching

Ambient ice-nucleating particles (INPs) represent an important subset of aerosol particles that facilitate heterogeneous formation of ice crystals in the atmosphere, which can impact Earth system and energy. In this work, we developed an affordable high-resolution platform to replicate atmospheric immersion freezing through the unique capabilities of microfluidics to measure INP concentration of known ice nucleation active materials, as well as high-latitude soil samples. The new instrument produced comparable and extended freezing efficiency data for a multitude of samples over the temperature range of -5 to -35 °C as compared to an existing freezing assay within known uncertainties. Moreover, the new assay was integrated into science teaching at a primarily undergraduate and Hispanic-serving institute, contributing to fostering a deeper understanding of ice nucleation processes among college students, instilling their enthusiasm for science, and addressing the critical need for a well-informed citizenry. Student research assistants were involved in both research and pedagogical development processes. Three students from our team visited the Pacific Northwest National Laboratory to help characterize physicochemical properties of our test samples and to test modeling of atmospheric ice nucleation using a box model as well as a global climate model (E3SM) for the regional-scale conditions over the North Slope of Alaska (NSA) and Southern Great Plains (SGP). We also assessed student learning experience via hands-on training, research processes, and development of educational materials. On pre- and post-participation surveys and in exit interviews, students reported personal growth as advancements in breadth of experience, research-related skill sets, and regarding their educational and career goals. They also affirmed that the methods enacted incorporated the NASA Minority University Research and Education Program (MUREP) STEM Engagement Best Practices.

58 GEOSCIENCES↗

Ice Nucleation Spectrometer (INS) Instrument Handbook

The Ice Nucleation Spectrometer (INS) is an offline analytical measurement system used to process filter samples for freezing temperature spectra of immersion-mode ice nucleating particle (INP) number concentrations. It is almost identical to the CSU Ice Spectrometer (IS) design. While basic immersion freezing methods have been applied for decades, recent intercomparison studies (DeMott et al. 2017, 2018b) with other methods for sampling ambient INPs support the method’s utility. Use of the INS with filters produces spectra spanning wide dynamic ranges of temperature and, hence, INP concentration (e.g., six orders of magnitude). The INS is supported with well-established experimental protocols and has been applied in many diverse scenarios.

54 ENVIRONMENTAL SCIENCES↗

Arctic Ice Nucleation Sampling during MOSAiC (INPMOSAIC2) Field Campaign Report

The accelerated rate of warming in the Arctic is of great concern due to potential impacts that include release of greenhouse gases from permafrost, melting glacial ice contributing to sea level rise, and declining sea ice cover exposing the darker ocean surface. These processes induce positive feedbacks and contribute to further warming that affects climate globally. Clouds play a crucial role in regulating the energy reaching the sea ice and snow surfaces, but the magnitude of their effects on surface temperature is not well constrained in the Arctic. Aerosols are an important contributor by serving as seeds for cloud particle formation, but even less is known about their overall impact and origin. In particular, aerosols that serve as ice nucleating particles (INPs) are vastly understudied, especially above the central Arctic Ocean. However, INPs likely play a significant role in arctic mixed-phase cloud (AMPC) microphysics and the resulting impacts of such clouds on the surface energy budget over the sea ice.

54 ENVIRONMENTAL SCIENCES↗

Effects of Pollen on Hydrometeors and Precipitation in a Convective System

Anemophilous (wind-driven) pollen is one type of primary biological aerosol particle, which can rupture under high humidity conditions and form smaller sub-pollen particles (SPPs). Both pollen and SPPs can reach the upper troposphere under convective conditions, acting as cloud condensation nuclei (CCN) and ice nucleating particles (INPs), thus influencing cloud formation and precipitation. However, the impacts of these biological aerosols on cold cloud formation and local climate remain unclear as there are large uncertainties on their emission flux and ice nucleating abilities. Here, we incorporate pollen emission and rupture processes in the Weather Research and Forecasting Model with Chemistry (WRF-Chem) simulations and update the Morrison microphysics scheme within WRF-Chem using aerosol-aware INP parameterizations to account for pollen in addition to other anthropogenic and biogenic aerosol. INP parameterizations for pollen and SPP are derived from laboratory experiments. When including pollen rupture rates as observed in a series of chamber studies, SPP concentrations increase, leading to an increase of cloud ice and water by up to 50% and potentially extending the duration of the convective system. Among all simulated hydrometeors, graupel and raindrops exhibit the largest enhancements from the inclusion of SPPs, with intensifying precipitation at the backside of the convective system and a greater spatial extent. Sensitivity simulations indicate that SPPs have a greater effect on cloud microphysical processes than whole pollen grains, and further observational evidence is needed to constrain these processes.

54 ENVIRONMENTAL SCIENCES↗

High Supersaturation in the Wake of Falling Hydrometeors: Implications for Cloud Invigoration and Ice Nucleation

Aerosol particles, cloud droplets, and ice crystals, coupled through the supersaturation field, play an important role in the buoyancy and life cycle of convective clouds. This letter reports laboratory observations of copious cloud droplets and ice crystals formed in the wake of a warm, falling water drop, which is a laboratory surrogate for a relatively warm hydrometeor in atmospheric clouds, such as a graupel particle in the wet growth regime. Aerosols were activated in the regions of very high supersaturation due to mixing in the wake. A mechanism is explored for attaining very high supersaturations capable of activating significant fractions of the interstitial aerosols within the lifetime of a convective cloud. The latent heat released from the activation of interstitial aerosols and subsequent growth may provide an additional source of buoyancy for cloud invigoration and may lead to larger concentrations of ice crystals.

54 ENVIRONMENTAL SCIENCES↗

The prevalence of precipitation from polar supercooled clouds

Abstract. Supercooled clouds substantially impact polar surface energy budgets, but large-scale models often underestimate their occurrence, which motivates accurately establishing metrics of basic processes. An analysis of long-term measurements at Utqiaġvik, Alaska, and McMurdo Station, Antarctica, combines lidar-validated use of soundings to identify supercooled cloud layers and colocated ground-based profiling radar measurements to quantify cloud base precipitation. We find that more than 85 % (75 %) of sampled supercooled layers are precipitating over the Arctic (Antarctic) site, with more than 75 % (50 %) precipitating continuously to the surface. Such high frequencies can be reconciled with substantially lesser spaceborne estimates by considering differences in radar hydrometeor detection sensitivity. While ice precipitation into supercooled clouds from aloft is common, we also find that the great majority of supercooled cloud layers without ice falling into them are themselves continuously generating precipitation. Such sustained primary ice formation is consistent with continuous activation of immersion-mode ice-nucleating particles (INPs), suggesting that supercooled cloud formation is a principal gateway to ice formation at temperatures greater than ∼-38 ∘C over polar regions. The prevalence of weak precipitation fluxes is also consistent with supercooled cloud longevity and with well-observed and widely simulated case studies. An analysis of colocated microwave radiometer retrievals suggests that weak precipitation fluxes can be nonetheless consequential to moisture budgets for supercooled clouds owing to small liquid water paths. The results here also demonstrate that the observed abundance of mixed-phase clouds can vary substantially with instrument sensitivity and methodology. Finally, we suggest that these ground-based precipitation rate statistics offer valuable guidance for improving the representation of polar cloud processes in large-scale models.

54 ENVIRONMENTAL SCIENCES↗

Discrimination between individual dust and bioparticles using aerosol time-of-flight mass spectrometry

Ice nucleating particles (INPs) impact cloud properties and precipitation processes through their ability to trigger cloud glaciation. Dust and bioparticles are two important sources of INPs that have markedly different atmospheric loadings and ice nucleating efficiencies. In situ identification of the sources of INPs in clouds has been accomplished using single particle mass spectrometry (SPMS). However, external mixtures of dust and bioparticles present a unique challenge as they have overlapping mass spectral ion signatures, complicating their unambiguous identification. This study presents a detailed discussion of dust and bioparticle SPMS signatures, uniting data from a broad array of studies. As emphasized, the ion signals from both dust and bioparticles are highly sensitive to ionization conditions. To understand the observed variations, we characterize the mass spectral dependence of distinct dust and bioparticle samples using total positive ion intensity (TPII) as an indicator of the laser pulse energy each particle encountered. Through this analysis, a broad range of characteristic biogenic low intensity ion peaks that may be useful to distinguish bioparticles from dust became apparent and are highlighted. Insights informed by this analysis were utilized to identify bioparticles in ambient SPMS data. Ambient particles exhibiting both dust and characteristic biogenic spectral fingerprints were excluded from the bioparticle classification. Although bioparticles only made up 0.2% of all sampled particles, their abundance was moderately correlated with INP concentrations measured at 15 °C.

54 ENVIRONMENTAL SCIENCES↗

Dataset for "Bioaerosols are the dominant source of warm-temperature immersion-mode INPs and drive uncertainties in INP predictability

Ice nucleating particles (INPs) are a rare subset of atmospheric aerosol that can initiate primary ice formation and thus trigger cloud glaciation. The re is a significant gap between our ability to measure INPs and to predict their concentrations and variability in large-scale weather and climate models. Accurate simulation of I NPs requires simulation of their major particle sources, as well as representative parameterizations of IN efficiency. Thus, there is a need for measurements of INP concentrations , delineated by particle type, to validate and improve model prediction of INP concentrations. Here we present a novel method for speciating INP concentrations into the relative c ontributions from dust, sea spray aerosol (SSA), and bioaerosol using single particle measurements. In a field campaign at Bodega Bay (coastal California), we find that bioaerosol s were the primary source of INPs between -12 and -20 ?C, while dust was a relatively minor source and SSA did not contribute significantly. We show that recent INP parameterizati ons for dust and SSA accurately predict ambient INP concentrations for these particle types. Finally, we use the speciated INP concentrations to evaluate the simulation of INPs at Bodega Bay, using a Lagrangian approach to connect the locally-observed aerosol with regionally-widespread emissions parameterizations. We find that we can skillfully simulate du st and SSA INPs, but not bioaerosol INPs. This points to a need for additional research to identify the major factors controlling the emissions and INP efficiency of bioaerosol IN Ps in order to develop improved parameterizations and enable their improved representation in models.

54 ENVIRONMENTAL SCIENCES↗

Atmospheric ice nuclei concentration measurements over a high altitude-station in the Western Ghats, India

Mixed-phase and ice clouds play a significant role in modulating the Indian summer monsoon rainfall, and modeling studies suggest that inaccurate representation of ice nucleating particles (INP) is one of the factors, which have resulted in a deficiency in the prediction of cloud properties and hydrological cycle. We do not understand the ice nucleation mechanisms to represent the ice formation in the model, and therefore more INP measurements at various supercooled temperatures are needed. This study reports for the first time real-time INP concentration at a high altitude station in the Western Ghats region of India, and these results will be used to constrain the ice nucleation parameterizations in the model. The variation of INP for any particular cloud condition can have strong microphysical responses of mixed-phase precipitation formation processes. Also, to improve the representation of heterogeneous ice nucleation, INP measurements of various types of aerosols commonly observed over the Indian region are needed. This study presents, the INP concentrations and daily concentration of non-refractory chemical composition (organics, sulfate, nitrate, ammonium, and chloride), cloud condensation nuclei (CCN), and aerosol size distribution. Spectrometer for Ice Nuclei (SPIN) was operated to measure INP concentration at the mountain site from August to December 2018. INP measurements were performed at three different temperatures (-25, -30, and - 34 °C) in the immersion freezing mode relevant for mixed-phase cloud conditions. The average INP concentrations approximately varied from 0.18 to 12.4 L-1, 0.39 to 24 L-1, 1.1 to 40.2 L-1 at -25, -30, and - 34 °C, respectively. These concentrations are within the concentrations reported in the literature from different regions across the globe. The air mass back trajectory analysis showed that continental air mass contains more INP compared to maritime air mass. The information on INP concentration and chemical characteristics of aerosol will help to improve heterogeneous ice nucleation parameterization in numerical models.

Kumar, Anil V.↗