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DOE OSTI2023

Important ice processes are missed by the Community Earth System Model (CESM) in Southern Ocean mixed–phase clouds: Bridging SOCRATES observations to model developments

Global climate models (GCMs) are challenged by difficulties in simulating cloud phase and cloud radiative effect over the Southern Ocean (SO). Some of the new generation GCMs predict too much liquid and too little ice in mixed-phase clouds. This misrepresentation of cloud phase in GCMs results in weaker negative cloud feedback over the SO and a higher climate sensitivity. Based on a model comparison with observational data obtained during the Southern Ocean Cloud Radiation and Aerosol Transport Experimental Study (SOCRATES), this study addresses a key uncertainty in the Community Earth System Model version 2 (CESM2) related to cloud phase, namely ice formation in pristine remote SO clouds. It is found that sea spray organic aerosols (SSOA) are the most important type of ice nucleating particles (INPs) over the SO with concentrations one order of magnitude higher than those of dust INPs based on measurements and CESM2 simulations. Secondary ice production (SIP) which includes riming splintering, rain droplet shattering, and ice-ice collisional fragmentation as implemented in CESM2 is the dominant ice production process in moderately cold clouds with cloud temperatures greater than –20°C. SIP enhances the in-cloud ice number concentrations (Ni) by 1-3 orders of magnitude and predicts more mixed-phase (with percentage occurrence increased from 15% to 21%), in better agreement with the observations. Finally, this study highlights the importance of accurately representing cloud phase over the pristine remote SO by considering the ice nucleation of SSOA and SIP processes, which are currently missing in most GCM cloud microphysics parameterizations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

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↗

NASA NTRS1978

Ice nucleation activity of rocket effluent

An investigation was conducted concerning the ice nucleation activity of the exhaust products of solid rockets. The Voyager I and II payloads were launched from Kennedy Space Center on September 5 and August 20, 1977, respectively. A visible stabilized ground cloud (SGC) consisting of rocket effluent and dust formed downwind. An instrumented aircraft was used to make multiple passes in the SGC. A Mylar bag was rapidly filled with SGC aerosol and then immediately sampled with an ice nucleus counter. Analyses of rocket effluent collected are discussed, taking into account the ice nucleus concentration, particle concentration and size distribution, and the elemental composition of individual particles. A description of laboratory experiments is also presented, giving attention to the elemental composition of individual particles and the ice nucleus concentration.

Parungo, F. P.↗

DOE OSTI2023

Biological particles and aerosol-cloud interactions in the Southern Great Plains

The United States Southern Great Plains (SGP) is the genesis for much of the warm season precipitation in the central and eastern United States. While atmospheric thermodynamics and large-scale dynamics play an important role in formation of precipitation, precipitation mechanisms are also sensitive to aerosols. Aerosols can suppress precipitation as cloud condensation nuclei (CCN) or act as ice nucleating particles (INP) in deep convective clouds. This project focused on understanding the role of primary biological aerosol particles (PBAP) in the region and its influence on cloud formation. Specifically, we focused on biological aerosol in the form of pollen, one type of PBAP that is emitted in large yet variable quantities from vegetation in the mid latitudes. Field observations provide evidence of pollen in the planetary boundary layer and pollen components in cloud droplets and fine particulate matter. Further, pollen grains can easily rupture when wet, forming smaller, sub pollen particles with sizes less than one micron. We evaluated the potential for PBAP events at the Department of Energy (DoE) SGP Atmospheric Radiation Measurement (ARM) research facility due to the rich dataset available. We also developed model simulations that accounted for pollen emission and the generation of sub pollen particles, which have been shown to be both cloud condensation nuclei and ice nucleating particles. The proposed work was designed to address the following questions: 1. What are the physical and chemical signatures of biological aerosol such as pollen in SGP ARM measurements? 2. What is the role of pollen-derived particles on deep convection and precipitation in the Central US? Using measurements from the DoE SGP ARM site and recent airborne campaigns, we evaluated the signatures of pollen and pollen-derived aerosols on optical properties, cloud properties and precipitation (Subba et al., 2021). We identified pollen-driven events over the data record and used the Weather Research and Forecasting Model with fully coupled chemistry (WRF-Chem) to conduct chemically realistic simulations of aerosols during and summer mesoscale convective events in the Southern Great Plains (Subba et al., in review). This work improved our understanding of the role of biological aerosol on clouds and precipitation in the Central United States and placed these results in context with anthropogenically-driven processes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Biological particles and aerosol-cloud interactions in the Southern Great Plains (Final Report)

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2021

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 co-located 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, that 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. 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.

ice formation↗

NASA NTRS1992

Deuterium in North Atlantic storm tops

During the ERICA project in 1989, ice crystals were collected from the tops of two winter storms and one broad cirrus cloud. Deuterium concentration in the storm ice samples, together with a model of isotope fractionation, are used to determine the temperature where the ice was formed. Knowledge of the ice formation temperature allows us to determine whether the ice has fallen or been lofted to the altitude of collection. In both storms, the estimated fall distance decreases upward. In the 21 January storm, the fall distance decreases to zero at the cloud top. In the 23 January storm, the fall distance decreases to zero at a point 2 km below the cloud top and appears to become negative above, indicating lofted ice. Cloud particle data from the cloud tops show an ice-to-vapor ratio greater than one and indicate the presence of particles with small terminal velocities; both observations support the idea of ice lofting. The satellite-derived cloud tops lie well below the actual cloud top (e.g., 2.5 km below on 23 January), indicating that the lofted ice in winter storms may not be detectable from space using IR radiance techniques. A comparison of deuterium in cloud-top ice and clear-air vapor suggests that even in winter, when vertical air motions are relatively weak, lofted ice crystals are the dominant source of water vapor in the upper troposphere.

Smith, Ronald B.↗

DOE OSTI2023

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↗

DOE OSTI2024

Cloud Processing of Aerosol during SAIL Field Campaign Report

Globally, on average, the release rate of aerosols from clouds is estimated to be about 6,000 Tg/yr and an aerosol particle is estimated to experience about three cloud cycles. Cloud processing of aerosol produces aerosols that have dramatically different physicochemical properties compared to their original form. Cloud processing may transform particles to efficient cloud condensation nuclei (CCN) or ice nucleating particles (INP) that can further participate in cloud formation. We investigated cloud processing of aerosol during the U.S. Department of Energy (DOE)’s Atmospheric Radiation Measurement (ARM) Surface Atmosphere Integrated Field Laboratory (SAIL) field campaign using multi-modal offline analysis techniques available at DOE’s Environmental Molecular Sciences Laboratory (EMSL). The main scientific aim of this project was to understand the processes that transform aerosols (chemically, and physically), and influence aerosol-cloud interactions. Aerosol particles undergo significant modifications due to warm (cloud droplets) and cold cloud (ice crystals) processing. Cloud processing of aerosol has important effects on the atmospheric aerosol number and mass concentration, size distribution, phase separation, and chemical composition.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Implications of Aerosol Physicochemical Properties Including Ice Nucleation at ARM Mega Sites for Improved Understanding of Microphysical Atmospheric Cloud Processes (Final Technical Report)

Continuous, long-term measurements of atmospheric ice-nucleating particles (INPs) that influence clouds and precipitation were conducted to investigate the abundance and variability of ground-level INPs across the world. Three field campaigns were organized by the DOE Atmospheric Radiation Measurement (ARM) program, including Examining INP from Southern Great Plains (ExINP-SGP, 2019), Examining INP from Eastern North Atlantic (ExINP-ENA, 2020 – 2021), and Examining INP from North Slope of Alaska (ExINP-NSA, 2021 – 2024). Additional small-scale supporting field experiments were performed in 2019 and 2021 to collect airborne particulate matter at SGP for complementary laboratory characterization of the particles’ physical and chemical properties [Aerosol-Ice Formation Closure Pilot Study (AEROICESTUDY), 2019; ExINP-SGP II, 2021]. In these studies, the PI’s team measured INP concentration with both real-time and laboratory measurements in a wide range of freezing temperatures ($T$ from 0 °C to about –30 °C). This project elucidated spatial variability and seasonality in the abundance of immersion mode active INPs across three ARM sites using a single instrument, a Portable Ice Nucleation Experiment (PINE) chamber version 03 (PINE-03 hereafter). Collocated aerosol and meteorological data were analyzed to assess the correlation between ambient INP abundance, air mass origin region, and meteorological variability. Our findings suggest very high freezing efficiency of INPs at the NSA site across the measured temperatures (ice nucleation active surface site density, $n_s(T)$, $\approx 2 \times 10^{8} - 10^{10}$ m -2 for from –16 to –31 °C), which is a factor of 10 – 1000 times greater efficiency as compared to that found in the previous mid-latitude INP measurements in autumn using the same instrument; surprisingly high INP abundance ($\ge 1 \text{ L}^{-1}$ at –25 °C) for the examined temperatures throughout the year that PINE-03 did not measure at other sites; and high INP concentration in spring, possibly related to arctic haze episodes.

58 GEOSCIENCES↗

NASA NTRS1982

Interpretation of satellite-observed thunderstorm anvil structure

The radiative characteristics of an anvil plume sensed by satellite radiometers are studied to discern the reason for an observed 'V' pattern of colder temperatures and a corresponding internal warm region. The measured black body temperature is affected by the ice water content and particle distributions in the cloud layer. Attention is given to 'V' anvil structure examined by Haynesfield et al. (1979). The GOES satellite IR data are treated with a plane parallel geometric radiative transfer model and a particle trajectory model is used to simulate ice particle concentrations downwind from a strongly divergent cloud top. Output from the two models indicate the 'V' pattern arises from divergence in the storm anvil. The particle concentration was elevated within the V-shaped region, causing lower temperatures in the V arms. The V is produced by strong upper level flow as well as strong mass and moisture divergence in the storm outflow.

Heymsfield, G. M.↗

NASA NTRS1999

Far Infrared Measurements of Cirrus

Improved techniques for remote sensing of cirrus are needed to obtain global data for assessing the effect of cirrus in climate change models. Model calculations show that the far infrared/sub-millimeter spectral region is well suited for retrieving cirrus Ice Water Path and particle size parameters. Especially useful cirrus information is obtained at frequencies below 60 cm-1 where single particle scattering dominates over thermal emission for ice particles larger than about 50 m. Earth radiance spectra have been obtained for a range of cloud conditions using an aircraft-based Fourier transform spectrometer. The Far InfraRed Sensor for Cirrus (FIRSC) is a Martin-Puplett interferometer which incorporates a polarizer for the beamsplitter and can be operated in either intensity or linear polarization measurement mode. Two detector channels span 10 to 140 cm-1 with a spectral resolution of 0.1 cm-1; achieving a Noise Equivalent Temperature of approximately 1K at 30 cm-1 in a 4 sec scan. Examples are shown of measured and modeled Earth radiance for a range of cloud conditions from 1998 and 1999 flights.

Nolt, I. G.↗

NASA NTRS2016

The Relationships Between Insoluble Precipitation Residues, Clouds, and Precipitation Over California's Southern Sierra Nevada During Winter Storms

Ice formation in orographic mixed-phase clouds can enhance precipitation and depends on the type of aerosols that serve as ice nucleating particles (INP). The resulting precipitation from these clouds is a viable source of water, especially for regions such as the California Sierra Nevada. Thus, a better understanding of the sources of INP that impact orographic clouds is important for assessing water availability in California. This study presents a multi-site, multi-year analysis of single particle insoluble residues in precipitation samples that likely influenced cloud ice and precipitation formation above Yosemite National Park. Dust and biological particles represented the dominant fraction of the residues (64% on average). Cloud glaciation, determined using GOES satellite observations, not only depended on high cloud tops (greater than 6.2 km) and low temperatures (less than -26 C), but also on the composition of the dust and biological residues. The greatest prevalence of ice-phase clouds occurred in conjunction with biologically-rich residues and mineral dust rich in calcium, followed by iron and aluminosilicates. Dust and biological particles are known to be efficient INP, thus these residues are what likely influenced ice formation in clouds above the sites and subsequent precipitation quantities reaching the surface during events with similar meteorology. The goal of this study is to use precipitation chemistry information to gain a better understanding of the potential sources of INP in the south-central Sierra Nevada, where cloud-aerosol-precipitation interactions are under-studied and where mixed-phase orographic clouds represent a key element in the generation of precipitation and thus the water supply in California.

Creamean, Jessie M.↗

NASA NTRS2018

Implementation of a Comprehensive Ice Crystal Formation Parameterization for Cirrus and Mixed-Phase Clouds in the EMAC Model (Based on MESSy 2.53)

A comprehensive ice nucleation parameterization has been implemented in the global chemistry-climate model EMAC to realistically represent ice crystal number concentrations. The parameterization of Barahona and Nenes (2009, hereafter BN09) allows the treatment of ice nucleation, taking into account the competition for water vapour between homogeneous and heterogeneous nucleation and pre-existing ice crystals in cold clouds. Furthermore, the influence of chemically-heterogeneous, polydisperse aerosols is considered via multiple ice nucleating particle spectra, which are included in the parameterization to compute the heterogeneously formed ice crystals. BN09 has been implemented to operate both in the cirrus and in the mixed-phase regimes. Compared to the standard EMAC results, BN09 produces fewer ice crystals in the upper troposphere but higher ice crystal number concentrations in the middle troposphere, especially in the Northern Hemisphere where ice nucleating mineral dust particles are relatively abundant. The comparison with a climatological data set of aircraft measurements shows that BN09 used in the cirrus regime improves the model results and, therefore, is recommended for future EMAC simulations.

EMAC↗

NASA NTRS1993

Liquid water content measurements using the Phase Doppler Particle Analyzer in the NASA Lewis Icing Research Tunnel

The performance of a Phase Doppler Particle Analyzer (PDPA) based icing probe suitable for use in icing tunnels and airborne applications is assessed. The instrument is shown to accurately and repeatably measure liquid water content (LWC) to within better than 20 percent of the nominal expected value in the NASA Lewis IRT. This was seen to be true over a wide range of tunnel operating conditions. The principles used by the PDPA for MVD and LWC determination are discussed. Calibration curves for the IRT median volume diameter are also determined and compared to the existing calibration determined via the PMS instruments. As has been shown in previous work, the PDPA is quite repeatable. The results are typically 3 to 5 microns smaller than the existing calibrations for a given run condition. Reasons for these differences are also discussed.

Rudoff, R. C.↗

DOE OSTI2021

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↗

NASA NTRS1972

Light scattering by ice clouds in the visible and infrared - A theoretical study.

Computations of the intensity and linear polarization for single scattering by ice clouds have been made based on the assumption that the particles in ice clouds can be approximated by long circular cylinders which are allowed to be polydispersive as well as arbitrarily oriented in space. The results of two models of optically thin ice clouds are presented and compared with those for polydisperse ice spheres. The two models for ice cylinders are assumed to be either uniformly or randomly oriented in a horizontal plane. Four different wavelengths, 0.7, 3, 3.5 and 6.05 microns, are employed in the light scattering computations. It is found that, compared to ice spheres, long ice cylinders scatter more light in the region with scattering angles near 90 deg, at the expense of scattering in both the forward and backward directions. The glory and cloudbows, which occur in light scattered by spherical particles, are either lost (the glory) or largely reduced and distorted (the cloudbows in the case of cylinders). It is probable that for more irregular particles the cloudbows would also disappear. These differences in scattering by spherical and non-spherical scatterers therefore provide useful information for the differentiation between the ice and liquid phase of cloud particles.

Liou, K.-N.↗

DOE OSTI2023

Agricultural Ice Nuclei at Southern Great Plains Supplemental Sampling (AGINSGP-SUPP) Field Campaign Report

The Agricultural Ice Nuclei at Southern Great Plains Supplemental Sampling (AGINSGP-SUPP) field campaign took place from April 8 to April 28, 2022. It included sample collection and analysis of filter samples for ice-nucleating particle (INP) concentrations. By enabling quantification of INPs at warmer temperatures (i.e., T > 258 K), these samples complemented the real-time observations of INPs that were performed as part of the AGINSGP campaign during the same period. In addition to collecting ground-based samples, the campaign collected vertical samples of INPs aboard the Atmospheric Radiation Measurement (ARM) tethered balloon system (TBS) as shown in Figure 1. These vertical samples complemented the vertical profiling of aerosol properties that was supported under a related Facilities Integrating Collaborations for User Science (FICUS) proposal. The overall aim of these three campaigns was to improve understanding of the sources and variability in observed INP concentrations at ARM’s SGP observatory. For example, warm-temperature INPs in this agricultural region are thought to originate in part from regional emissions of fertile, agricultural soils containing high organic content. Laboratory experiments have shown that soil particles with high organic content are more efficient INPs than inorganic soils (e.g., Tobo et al. 2014). Quantification of warm-temperature INPs under ambient conditions currently can only be achieved via offline methods such as the ARM ice-nucleation spectrometer (INS). Therefore, offline sampling for the INS was required to complement the real-time INP measurements conducted during the AGINSGP campaign.

, tethered balloon system↗