SEARCH · Search NASA

Results for “ice nucleation processes”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

SourceResearch connectionFrom yearThrough year

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 91 records · Page 5

All sources NASA NTRS DOE OSTI

DOE OSTI2024

The impact of cloud microphysics and ice nucleation on Southern Ocean clouds assessed with single-column modeling and instrument simulators

Abstract. Supercooled liquid clouds are common at higher latitudes (especially over the Southern Ocean) and are critical for constraining climate projections. We take advantage of the Macquarie Island Cloud and Radiation Experiment (MICRE) to perform an analysis of observed and simulated cloud processes over the Southern Ocean in a region and season dominated by supercooled liquid clouds. Using a single-column version of the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecast System (IFS), we compare two different cloud microphysical schemes to ground-based observations of cloud, precipitation, and radiation over a 2.5-month period (1 January–17 March 2017). Both schemes are able to reproduce aspects of the cloud and radiation observations during MICRE to within the uncertainty of the data when the thermodynamic profile is prescribed with relaxation. There are differences in water mass and representation of reflectivity between the schemes. A sensitivity study of the cloud microphysics schemes, one a bulk one-moment scheme and the other a two-moment scheme with prediction of mass and number, indicates that several key processes create differences between the schemes. Surface radiative fluxes and total water path are highly sensitive to the formation and fall speed of precipitation. The prediction of hydrometeor number with the two-moment scheme yields a better comparison with observed reflectivity and radiative fluxes, despite predicting higher liquid water contents than observed. With the two-moment scheme, we are also able to test the sensitivity of the results to the input of liquid cloud condensation nuclei (CCN) and ice nuclei (IN). The cloud properties and resulting radiative effects are found to be sensitive to the CCN and IN concentrations. More CCN and IN increase liquid and ice water paths, respectively. Thus, both the dynamic environment and aerosols, integrated through the cloud microphysics, are important for properly representing Southern Ocean cloud radiative effects.

58 GEOSCIENCES↗

DOE OSTI2020

Pragmatic protocols for working cleanly when measuring ice nucleating particles

We report that measuring ice nucleating particles (INPs) is critical for understanding, and modeling, cloud formation, reflectivity, and precipitation patterns. However, because INPs are very rare in the atmosphere, but abundant—sometimes alarmingly so—in the dust that covers all work surfaces, contamination during processing of collected aerosol samples can be a significant hindrance to obtaining accurate measures of INPs. In preparing this technical note, we questioned the cleanliness of every collection and processing step involved in making immersion freezing measurements of INPs re-suspended from filter samples. The aim was to identify, and then minimize, all potential sources of significant contamination, including containers and tools used to store filters and prepare liquid suspensions, gloves, work surfaces, and the polymerase chain reaction (PCR) trays commonly used for sample analysis. While plasticware released few INPs, most gloves readily shed them, but this can be mitigated by using washed cleanroom vinyl or polyethylene gloves. Work surfaces, even those that had been cleaned, were prodigious reservoirs of contaminating INPs, but simply covering them with aluminum foil will provide an INP-free surface. By applying these practices, we developed a method to reduce the background level of INPs on Nuclepore™ polycarbonate filters in our tests to 0 at -25 °C and < 20 at -27 °C, making them suitable for use in all sampling environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Dependencies of Four Mechanisms of Secondary Ice Production on Cloud-Top Temperature in a Continental Convective Storm

Various mechanisms of secondary ice production (SIP) cause multiplication of numbers of ice particle, after the onset of primary ice. A measure of SIP is the ice enhancement ratio (“IE ratio”) defined here as the ratio between number concentrations of total ice (excluding homogeneously nucleated ice) and active ice-nucleating particles (INPs). A convective line observed on 11 May 2011 over the Southern Great Plains in the Mesoscale Continental Convective Cloud Experiment (MC3E) campaign was simulated with the “Aerosol–Cloud” (AC) model. AC is validated against coincident MC3E observations by aircraft, ground-based instruments, and satellite. Four SIP mechanisms are represented in AC: the Hallett–Mossop (HM) process of rime splintering, and fragmentation during ice–ice collisions, raindrop freezing, and sublimation. The vertical profile of the IE ratio, averaged over the entire simulation, is almost uniform (10 2 to 10 3 ) because fragmentation in ice–ice collisions dominates at long time scales, driving the ice concentration toward a theoretical maximum. The IE ratio increases with both the updraft (HM process, fragmentation during raindrop freezing, and ice–ice collisions) and downdraft speed (fragmentation during ice–ice collisions and sublimation). As reported historically in aircraft sampling, IE ratios were predicted to peak near 10 3 for cloud-top temperatures close to the −12°C level, mostly due to the HM process in typically young clouds with their age less than 15 min. Here, at higher altitudes with temperatures of −20° to −30°C, the predicted IE ratios were smaller, ranging from 10 to 10 2 , and mainly resulted from fragmentation in ice–ice collisions.

Aerosols↗

DOE OSTI2026

Aerosol-deep convection interaction based on joint cell-thermal tracking in Large Eddy Simulations during the TRACER campaign

In cumulus clouds, aerosol concentrations control cloud droplet concentrations, modifying cloud radiative properties, precipitation processes, and cloud electrification. However, mechanisms of aerosol-deep convection interactions are not well understood due to complex cloud dynamics and microphysics. We investigate the interaction of aerosols with isolated deep convection using Large Eddy Simulations of two cases during the TRacking Aerosol Convection interactions ExpeRiment (TRACER) near Houston, Texas, using a joint cell-thermal tracking algorithm. Cumulus thermals are droplet generators, since supersaturation and droplet nucleation coincide with thermal centers, where the strongest updrafts occur. Primary ice crystal formation does not take place inside thermals, but at layers where previous thermals detrained moisture. As subsequent thermals containing supercooled droplets penetrate these layers, hail and graupel form at or near these thermals. Higher aerosol concentrations result in higher droplet concentrations that suppress drizzle, delay warm rain processes, and transport more moisture aloft. This increases snow and ice amount, as well as graupel and hail, leading to more lightning. Polluted thermals initiate at slightly higher altitudes, and are slightly larger and faster, suggesting a weak invigoration. We also find more thermals per cell, but fewer isolated cells, since convection is more aggregated and intense, especially near the end of the 24 h simulation. Non-linear mesoscale feedback likely triggered by temperature and moisture responses to aerosol-thermal interactions causes the aggregation. Time-lagged aerosol-reinitialization experiments show that the mesoscale response is the predominant forcing for the invigoration. These changes happen within one day, on a smaller scale than previously suggested.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Observations of Clouds, Aerosols, Precipitation, and Surface Radiation over the Southern Ocean: An Overview of CAPRICORN, MARCUS, MICRE, and SOCRATES

Weather and climate models are challenged by uncertainties and biases in simulating Southern Ocean (SO) radiative fluxes that trace to a poor understanding of cloud, aerosol, precipitation, and radiative processes, and their interactions. Projects between 2016 and 2018 used in situ probes, radar, lidar, and other instruments to make comprehensive measurements of thermodynamics, surface radiation, cloud, precipitation, aerosol, cloud condensation nuclei (CCN), and ice nucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase clouds common to this pristine environment. Data including soundings were collected from the NSF–NCAR G-V aircraft flying north–south gradients south of Tasmania, at Macquarie Island, and on the R/V Investigator and RSV Aurora Australis. Synergistically these data characterize boundary layer and free troposphere environmental properties, and represent the most comprehensive data of this type available south of the oceanic polar front, in the cold sector of SO cyclones, and across seasons. Results show largely pristine environments with numerous small and few large aerosols above cloud, suggesting new particle formation and limited long-range transport from continents, high variability in CCN and cloud droplet concentrations, and ubiquitous supercooled water in thin, multilayered clouds, often with small-scale generating cells near cloud top. These observations demonstrate how cloud properties depend on aerosols while highlighting the importance of dynamics and turbulence that likely drive heterogeneity of cloud phase. Satellite retrievals confirmed low clouds were responsible for radiation biases. Furthermore, the combination of models and observations is examining how aerosols and meteorology couple to control SO water and energy budgets.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

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↗

DOE OSTI2023

Effects from Time Dependence of Ice Nucleus Activity for Contrasting Cloud Types

Abstract The role of time-dependent freezing of ice nucleating particles (INPs) is evaluated with the “Aerosol–Cloud” (AC) model in 1) deep convection observed over Oklahoma during the Midlatitude Continental Convective Cloud Experiment (MC3E), 2) orographic clouds observed over North California during the Atmospheric Radiation Measurement (ARM) Cloud Aerosol Precipitation Experiment (ACAPEX), and 3) supercooled, stratiform clouds over the United Kingdom, observed during the Aerosol Properties, Processes And Influences on the Earth’s climate (APPRAISE) campaign. AC uses the dynamical core of the WRF Model and has hybrid bin–bulk microphysics and a 3D mesoscale domain. AC is validated against coincident aircraft, ground-based, and satellite observations for all three cases. Filtered concentrations of ice (>0.1–0.2 mm) agree with those observed at all sampled levels. AC predicts the INP activity of various types of aerosol particles with an empirical parameterization (EP), which follows a singular approach (no time dependence). Here, the EP is modified to represent time-dependent INP activity by a purely empirical approach, using our published laboratory observations of time-dependent INP activity. In all simulated clouds, the inclusion of time dependence increases the predicted INP activity of mineral dust particles by 0.5–1 order of magnitude. However, there is little impact on the cloud glaciation because the total ice is mostly (80%–90%) from secondary ice production (SIP) at levels warmer than about −36°C. The Hallett–Mossop process and fragmentation in ice–ice collisions together initiate about 70% of the total ice, whereas fragmentation during both raindrop freezing and sublimation contributes <10%. Overall, total ice concentrations and SIP are unaffected by time-dependent INP activity. In the simulated APPRAISE case, the main causes of persistence of long-lived clouds and precipitation are predicted to be SIP in weak embedded convection and reactivation following recirculation of dust particles in supercooled layer cloud.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Cloud-Resolving ICON Simulations of Secondary Ice Production in Arctic Mixed-Phase Stratocumuli Observed during M-PACE

Field measurements and modeling studies suggest that secondary ice production (SIP) may close the gap between observed Arctic ice nucleating particle (INP) concentrations and ice crystal number concentrations ni. Here, we explore sensitivities with respect to the complexity of different INP parameterizations under the premise that ni is governed by SIP. Idealized, cloud-resolving simulations are performed for the marine cold air outbreak cloud deck sampled during the Mixed-Phase Arctic Cloud Experiment (M-PACE) with the Icosahedral Nonhydrostatic (ICON) model. The impact of the droplet shattering (DS) of raindrops and collisional breakup (BR) in addition to the existing Hallet–Mossop rime splintering mechanism were investigated. Overall, 12 different model experiments (12-h runs) were performed and analyzed. Despite the considerable amount of uncertainty remaining with regard to SIP mechanisms and their process representation in numerical models, we conclude from these experiments that (i) only simulations where DS dominates the SIP signal (potentially amplified by BR) capture observed ice-phase and liquid-phase cloud properties, and (ii) SIP events cluster around the convective outflow region and are structurally linked to mesoscale cloud organization. In addition, interactions with primary nucleation parameterizations of varied complexity were investigated. Here, our simulations show that (i) a stable long-lived mixed-phase cloud (MPC) can be maintained in the absence of primary nucleation once SIP is established, (ii) experiments using a computationally more efficient relaxation-based parameterization of primary nucleation are statistically invariant from simulations considering prognostic INP, and (iii) primary nucleation at cloud-top controls the areal extent of the mixed-phase cloud region, and reduces SIP efficacy via DS due to increased depletion of cloud liquid throughout the entire cloud column.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Annual cycle of aerosol properties over the central Arctic during MOSAiC 2019–2020 – light-extinction, CCN, and INP levels from the boundary layer to the tropopause

Abstract. The MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition was the largest Arctic field campaign ever conducted. MOSAiC offered the unique opportunity to monitor and characterize aerosols and clouds with high vertical resolution up to 30 km height at latitudes from 80 to 90∘ N over an entire year (October 2019 to September 2020). Without a clear knowledge of the complex aerosol layering, vertical structures, and dominant aerosol types and their impact on cloud formation, a full understanding of the meteorological processes in the Arctic, and thus advanced climate change research, is impossible. Widespread ground-based in situ observations in the Arctic are insufficient to provide these required aerosol and cloud data. In this article, a summary of our MOSAiC observations of tropospheric aerosol profiles with a state-of-the-art multiwavelength polarization Raman lidar aboard the icebreaker Polarstern is presented. Particle optical properties, i.e., light-extinction profiles and aerosol optical thickness (AOT), and estimates of cloud-relevant aerosol properties such as the number concentration of cloud condensation nuclei (CCN) and ice-nucleating particles (INPs) are discussed, separately for the lowest part of the troposphere (atmospheric boundary layer, ABL), within the lower free troposphere (around 2000 m height), and at the cirrus level close to the tropopause. In situ observations of the particle number concentration and INPs aboard Polarstern are included in the study. A strong decrease in the aerosol amount with height in winter and moderate vertical variations in summer were observed in terms of the particle extinction coefficient. The 532 nm light-extinction values dropped from >50 Mm−1 close to the surface to <5 Mm−1 at 4–6 km height in the winter months. Lofted, aged wildfire smoke layers caused a re-increase in the aerosol concentration towards the tropopause. In summer (June to August 2020), much lower particle extinction coefficients, frequently as low as 1–5 Mm−1, were observed in the ABL. Aerosol removal, controlled by in-cloud and below-cloud scavenging processes (widely suppressed in winter and very efficient in summer) in the lowermost 1–2 km of the atmosphere, seems to be the main reason for the strong differences between winter and summer aerosol conditions. A complete annual cycle of the AOT in the central Arctic could be measured. This is a valuable addition to the summertime observations with the sun photometers of the Arctic Aerosol Robotic Network (AERONET). In line with the pronounced annual cycle in the aerosol optical properties, typical CCN number concentrations (0.2 % supersaturation level) ranged from 50–500 cm−3 in winter to 10–100 cm−3 in summer in the ABL. In the lower free troposphere (at 2000 m), however, the CCN level was roughly constant throughout the year, with values mostly from 30 to 100 cm−3. A strong contrast between winter and summer was also given in terms of ABL INPs which control ice production in low-level clouds. While soil dust (from surrounding continents) is probably the main INP type during the autumn, winter, and spring months, local sea spray aerosol (with a biogenic aerosol component) seems to dominate the ice nucleation in the ABL during the summer months (June–August). The strong winter vs. summer contrast in the INP number concentration by roughly 2–3 orders of magnitude in the lower troposphere is, however, mainly caused by the strong cloud temperature contrast. A unique event of the MOSAiC expedition was the occurrence of a long-lasting wildfire smoke layer in the upper troposphere and lower stratosphere. Our observations suggest that the smoke particles frequently triggered cirrus formation close to the tropopause from October 2019 to May 2020.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Long-term variability in immersion-mode marine ice-nucleating particles from climate model simulations and observations

Abstract. Ice-nucleating particles (INPs) in the Southern Ocean (SO) atmosphere have significant impacts on cloud radiative and microphysical properties. Yet, INP prediction skill in climate models remains poorly understood, in part because of the lack of long-term measurements. Here we show, for the first time, how model-simulated INP concentrations compare with year-round INP measurements during the Macquarie Island Cloud Radiation Experiment (MICRE) campaign from 2017–2018. We simulate immersion-mode INP concentrations using the Energy Exascale Earth System Model version 1 (E3SMv1) by combining simulated aerosols with recently developed deterministic INP parameterizations and the native classical nucleation theory (CNT) for mineral dust in E3SMv1. Because MICRE did not collect aerosol measurements of super-micron particles, which are more effective ice nucleators, we evaluate the model's aerosol fields at other high-latitude sites using long-term in situ observations of dust and sea spray aerosol. We find that the model underestimates dust and overestimates sea spray aerosol concentrations by 1 to 2 orders of magnitude for most of the high-latitude sites in the Southern Hemisphere. We next compare predicted INP concentrations with concentrations of INPs collected on filter samples (typically for 2 or 3 d) and processed offline using the Colorado State University ice spectrometer (IS) in immersion freezing mode. We find that when deterministic parameterizations for both dust and sea spray INPs are used, simulated INPs are within a factor of 10 of observed INPs more than 60 % of the time during summer. Our results also indicate that the E3SM's current treatment of mineral dust immersion freezing in the SO is impacted by compensating biases – an underprediction of dust amount was compensated by an overprediction of its effectiveness as INPs. We also perform idealized droplet freezing experiments to quantify the implications of the time-dependent behavior assumed by the E3SM's CNT-parameterization and compare with the ice spectrometer observations. We find that the E3SM CNT 10 s diagnostic used in this study is a reasonable approximation of the exact formulation of CNT, when applied to ice spectrometer measurements in low-INP conditions similar to Macquarie Island. However, the linearized 10 s diagnostic underestimates the exact formula by an order of magnitude or more in places with high-INP conditions like the Sahara. Overall, our findings suggest that it is important to correct the biases in E3SM's simulated dust life cycle and update E3SM's INP parameterizations. INP prediction errors of 2 to 3 orders of magnitude can have considerable impacts on the simulated cloud and radiative properties in global climate models. On comparing INP concentrations during MICRE against ship-based campaigns, Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS) and Antarctic Circumnavigation Expedition (ACE), we find that INPs from the latter are significantly higher only in regions closer to Macquarie Island. This alludes to the fact that physical, chemical and biological processes affecting INP concentrations as stimulated by the island could be partly responsible for the high INP concentrations observed at Macquarie Island during the MICRE campaign. Therefore, improvements to both aerosol simulation and INP parameterizations are required to adequately simulate INPs and their cloud impacts in E3SM. It will be helpful to include a parallel measurement of the size-resolved aerosol composition and explore opportunities for long-term measurement platforms in future field campaigns studying INP sources in remote marine regions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Texas A&M University Mobile Facility Measurements during TRACER (Field Campaign Report)

One of the main goals of the U.S Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Tracking Aerosol Convection Interactions Experiment (TRACER) near Houston, Texas is to improve understanding of how meteorology and aerosols impact storm dynamical and microphysical processes in deep convection to better constrain and improve their model representation. The Houston area is strongly influenced by sea- and bay-breeze circulations that generate convergence and help to initiate and organize deep convection. To properly isolate and understand the roles of varied meteorological conditions and cloud condensation nuclei (CCN) and ice nucleation particles (INP) distributions in different air masses, co-located thermodynamic, kinematic, and aerosol vertical profile observations are needed. The focus of this campaign was to provide key measurements in air masses both in front of and behind sea/bay breeze fronts moving through the greater Houston area to sample the airmass heterogeneity. The overarching scientific goal of this campaign is to understand how the vertical distributions of both CCN and INP correspond to the inflow layer of deep convection in maritime, background continental, and polluted continental air masses, and how these variations influence deep convection. To fully sample the heterogeneity in both meteorological conditions and aerosols across the sea-breeze front (SBF), Texas A&M University (TAMU) deployed a InterMet 3050A 403 MHz mobile unit launching iMet-4 radiosondes and the new Rapid Onsite Atmospheric Measurement Van (ROAM-V) for aerosol sampling during the TRACER intensive operational period (IOP) from June to September 2022. The suite of instruments deployed on ROAM-V included a condensation particle counter (CPC; GRIMM Model 5.403 CPC), scanning mobility particle sizer (SMPS; TSI 3750 detector, TSI 3082 classifier, TSI 3088 neutralizer, TSI 3081A differential mobility analyzer), cloud condensation nuclei counter (Droplet Measurement Technologies CCN counter), micropulse lidar (Droplet Measurement Technologies micropulse lidar [miniMPL]), and a Davis Rotating Uniform size-cut Monitor (DRUM; DRUMAir 4-DRUM). Before sampling at each location, the latitude and longitude were recorded using the Global Positioning System (GPS) on the phone application “My Altitude”. The DRUM data were collected as part of a closely related ARM field campaign and also supported by DOE Atmospheric System Research grant DE-SC0021047. The TAMU team sampled these airmass heterogeneities by strategically choosing deployment sites in a different airmass than the ARM fixed sites in La Porte and Guy, Texas. On days when the sea/bay breeze boundary was pushing inland, the TAMU team would usually sample the airmass on the maritime side of the SBF at a coastal site in Galveston, Texas in the early afternoon (1730-1900 UTC) and then move inland ahead of the SBF to sample the airmass on the continental side during late afternoon (2030-2230). Figure 1 shows the Galveston maritime site and the array of sites for the late afternoon continental measurements.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Evidence for Secondary Ice Production in Southern Ocean Maritime Boundary Layer Clouds

Abstract Maritime boundary‐layer clouds over the Southern Ocean (SO) have a large shortwave radiative effect. Yet, climate models have difficulties in representing these clouds and, especially, their phase in this observationally sparse region. This study aims to increase the knowledge of SO cloud phase by presenting in‐situ cloud microphysical observations from the Southern Ocean Clouds, Radiation, Aerosol, Transport Experimental Study (SOCRATES). We investigate the occurrence of ice in summertime marine stratocumulus and cumulus clouds in the temperature range between 6 and −25°C. Our observations show that in ice‐containing clouds, maximum ice number concentrations of up to several hundreds per liter were found. The observed ice crystal concentrations were on average one to two orders of magnitude higher than the simultaneously measured ice nucleating particle (INP) concentrations in the temperature range below −10°C and up to five orders of magnitude higher than estimated INP concentrations in the temperature range above −10°C. These results highlight the importance of secondary ice production (SIP) in SO summertime marine boundary‐layer clouds. Evidence for rime splintering was found in the Hallett‐Mossop (HM) temperature range but the exact SIP mechanism active at lower temperatures remains unclear. Finally, instrument simulators were used to assess simulated co‐located cloud ice concentrations and the role of modeled HM rime‐splintering. We found that CAM6 is deficient in simulating number concentrations across the HM temperature range with little sensitivity to the model HM process, which is inconsistent with the aforementioned observational evidence of highly active SIP processes in SO low‐level clouds.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

CACTI ARM Mobile Facility (AMF) Measurements of Ice Nucleating Particles

The dataset comprises measures, using Colorado State University's Ice Spectrometer (IS, an immersion freezing device with a range from 0°C down to -26 to -29°C) of atmosperic ice nucleating particle (INP) concentrations taken on ARM's Mobile Facility (AMF-1) Aerosol Observing System, near Villa Yacanto in central Argentina, during the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) Experiment. A filter sampler was mounted on the AOS trailer (2 m below the AOS inlet). Single-use filter units open to the atmosphere fitted with pre-cleaned and pre-sterilized, 47-mm dia. Nuclepore polycarbonate filters were used. Filters were typically drawn for an 8-hour period, totaling 6000 liters sampled on average. After collection, filters were stored at -20°C until processed. Initial processing to obtain spectra of INP number concentration active via the immersion freezing mechanism versus temperature was conducted using CSU's IS instrument (McCluskey et al., 2018). For measurment of INPs, collected aerosol particles were re-suspended in 7-8 mL of 0.1 µm-filtered deionized (DI) water. Aliquots of each suspension, and serial dilutions, were dispensed into trays which were fit into aluminum blocks in the IS. Samples are cooled at 0.33°C min-1 and the freezing temperatures of wells recorded automatically. Cumulative INP concentrations were determined by first calculating the INPs per mL of suspension based on Vali (1971) and then converting to concentration per standard liter of air using the proportion of the total liquid sample dispensed and the air sample volumes. An aliquot of suspension fro selected samples were also heat treated (95°C for 20 min) to denature and deactivate biological INPs, and another aliquot digested in 10% H2O2 at 95°C under UV-B to remove all organic carbon INPs. McCluskey, C. S., J. Ovadnevaite, M. Rinaldi, J. Atkinson, F. Belosi, D. Ceburnis, S. Marullo, T. C. J. Hill, U. Lohmann, Z. A. Kanji, C. O’Dowd, S. M. Kreidenweis, P. J. DeMott, 2018: Marine and Terrestrial Organic Ice Nucleating Particles in Pristine Marine to Continentally-Influenced Northeast Atlantic Air Masses, Journal of Geophysical Research: Atmospheres, 123, 6196–6212, https://doi.org/10.1029/2017JD028033. Vali, G., 1971: Quantitative evaluation of experimental results on the heterogeneous freezing nucleation of supercooled liquids. J. Atmos. Sci., 28, 402–409.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

CACTI ARM Aerial Facility Measurements of Ice Nucleating Particles

The dataset comprises measures, using Colorado State University's Ice Spectrometer (IS, an immersion freezing device with a range from 0°C down to -26 to -29°C) of atmospheric ice nucleating particle (INP) concentrations taken on the Atmospheric Radiation Measurement (ARM) program Aerial Facilty (AAF) G-1 aircraft. INP measurements on the G-1 were collected from varied altitudes on different flights over the region of the Sierras de Córdoba mountain range of north-central Argentina, centred over ARM's Mobile Facility (AMF-1) near Villa Yacanto, where ground-based INP measures were being taken concurrently. Both studies took place as part of the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) Experiment. A filter sampling system was deployed on the G-1 to collect aerosol particles for post-processing of INPs collected on filters (measuring their immersion freezing ability) once returned to Colorado State University (CSU). Filter holders used were pre-cleaned aluminum in-line units loaded with pre-cleaned and pre-sterilized 47 mm dia. Nuclepore polycarbonate filters (0.2 mm pore size). Filters were drawn for varied times, resulting in varied volumes collected (51 to 1667 SL). Mass flow rate was recorded in real-time so that total sampled volume (at standard temperature and pressure) could be determined. A total of 34 sample filters were collected over the IOP, including 5 blanks. Filters were stored at -20°C freezer prior to frozen return to Colorado State University (CSU). . Processing to obtain spectra of INP number concentration active via the immersion freezing mechanism versus temperature was conducted using CSU's IS instrument (McCluskey et al., 2018). For measurment of INPs, collected aerosol particles were re-suspended in 7 mL of 0.02 µm-filtered deionized water. Aliquots of each suspension, and serial dilutions, were dispensed into trays which were fit into aluminum blocks in the IS. Samples are cooled at 0.33°C min-1 and the freezing temperatures of wells recorded automatically. Cumulative INP concentrations were determined by first calculating the INPs per mL of suspension based on Vali (1971) and then converting to concentration per standard liter of air using the proportion of the total liquid sample dispensed and the air sample volumes. Aliquots of suspensions from selected samples were also heat treated (95°C for 20 min) to denature and deactivate biological INPs, and digested in 10% H2O2 at 95°C under UV-B to remove all organic carbon INPs. McCluskey, C. S., J. Ovadnevaite, M. Rinaldi, J. Atkinson, F. Belosi, D. Ceburnis, S. Marullo, T. C. J. Hill, U. Lohmann, Z. A. Kanji, C. O’Dowd, S. M. Kreidenweis, P. J. DeMott, 2018: Marine and Terrestrial Organic Ice Nucleating Particles in Pristine Marine to Continentally-Influenced Northeast Atlantic Air Masses, Journal of Geophysical Research: Atmospheres, 123, 6196–6212, https://doi.org/10.1029/2017JD028033. Vali, G., 1971: Quantitative evaluation of experimental results on the heterogeneous freezing nucleation of supercooled liquids. J. Atmos. Sci., 28, 402–409.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Toward a Theory of the Evolution of Drop Morphology and Splintering by Freezing

Abstract The drop freezing process is described by a phase-field model. Two cases are considered: when the freezing is triggered by central nucleation and when nucleation occurs on the drop surface. Depending on the environmental temperature and drop size, different morphological structures develop. Detailed dendritic growth was simulated at the first stage of drop freezing. Independent of the nucleation location, a decrease in temperature within the range from ~−5° to −25°C led to an increase in the number of dendrites and a decrease in their width and the interdendritic space. At temperatures lower than about −25°C, a planar front developed following surface nucleation, while dendrites formed a granular-like structure with small interdendritic distances following bulk nucleation. An ice shell grew in at the same time (but slower) as dendrites following surface nucleation, while it started forming once the dendrites have reached the drop surface in the case of central nucleation. The formed ice morphology at the first freezing stage predefined the splintering probability. We assume that stresses needed to break the ice shell arose from freezing of the water in the interdendritic spaces. Under this assumption, the number of possible splinters/fragments was proportional to the number of dendrites, and the maximum rate of splintering/fragmentation occurred within a temperature range of about −10° to −20°C, is in agreement with available laboratory and in situ measurements. At temperatures < −25°C, freezing did not lead to the formation of significant stresses, making splintering unlikely. The number of dendrites increased with drop size, causing a corresponding increase in the number of splinters. Examples of morphology that favors drop cracking are presented, and the duration of the freezing stages is evaluated. Sensitivity of the freezing process to the surface fluxes is discussed.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

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↗

DOE OSTI2024

Characteristics and sources of fluorescent aerosols in the central Arctic Ocean

The Arctic is sensitive to cloud radiative forcing. Due to the limited number of aerosols present throughout much of the year, cloud formation is susceptible to the presence of cloud condensation nuclei and ice nucleating particles (INPs). Primary biological aerosol particles (PBAP) contribute to INPs and can impact cloud phase, lifetime, and radiative properties. We present yearlong observations of hyperfluorescent aerosols (HFA), tracers for PBAP, conducted with a Wideband Integrated Bioaerosol Sensor, New Electronics Option during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition (October 2019–September 2020) in the central Arctic. We investigate the influence of potential anthropogenic and natural sources on the characteristics of the HFA and relate our measurements to INP observations during MOSAiC. Anthropogenic sources influenced HFA during the Arctic haze period. But surprisingly, we also found sporadic “bursts” of HFA with the characteristics of PBAP during this time, albeit with unclear origin. The characteristics of HFA between May and August 2020 and in October 2019 indicate a strong contribution of PBAP to HFA. Notably from May to August, PBAP coincided with the presence of INPs nucleating at elevated temperatures, that is, >–9°C, suggesting that HFA contributed to the “warm INP” concentration. The air mass residence time and area between May and August and in October were dominated by the open ocean and sea ice, pointing toward PBAP sources from within the Arctic Ocean. As the central Arctic changes drastically due to climate warming with expected implications on aerosol–cloud interactions, we recommend targeted observations of PBAP that reveal their nature (e.g., bacteria, diatoms, fungal spores) in the atmosphere and in relevant surface sources, such as the sea ice, snow on sea ice, melt ponds, leads, and open water, to gain further insights into the relevant source processes and how they might change in the future.

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↗