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All sourcesNASA NTRSDOE OSTI
NASA NTRS2021

Evaluation of Higher-order Quadrature Schemes in Improving Computational Efficiency for Orientation-averaged Single-Scattering Properties of Nonspherical Ice Particles

We evaluate several high-order quadrature schemes for accuracy and efficacy in obtaining orientation-averaged single-scattering properties (SSPs). We use the highly efficient MIDAS to perform electromagnetic scattering calculations to evaluate the gain in efficiency from these schemes. MIDAS is shown to be superior to DDSCAT, a popular discrete dipole approximation (DDA) method. This study is motivated by the fact that quality physical precipitation retrievals rely on using accurate orientation-averaged SSPs derived from realistic hydrometeors as input to radiative transfer Models (RTMs). The DDA has been a popular choice for single-scattering calculations, due to its versatility with respect to target geometry. However, being iterative-solver-based (ISB), the most used DDA codes, e.g. DDSCAT and ADDA, must solve the scattering problem for each orientation of the target separately. As the size parameter and geometric anisotropy of the hydrometeor increase, the number of orientations needed to obtain accurate orientation-averages can increase drastically and so does the computation cost incurred by the ISB-DDA methods. MIDAS is a Direct-Solver-Based (DSB) code, its decomposition of the original large matrix with a high rank into multiple more manageable smaller matrices of lower ranks makes it much more computationally efficient while maintaining excellent accuracy. In addition, direct solvers consider all requested orientations at once, giving MIDAS further advantage over popular ISB-DDA methods. MIDAS, when combined with high-order quadrature for orientation averaging, can be greater than three orders of magnitude more efficient in obtaining RTM-ready SSPs of complex-shaped hydrometeors than existing ISB-DDA methods, with the native quadrature schemes they offer.

Ines Fenni↗
DOE OSTI2024

The Abundance and Sources of Ice Nucleating Particles Within Alaskan Ice Fog

Abstract The Alaskan Layered Pollution and Chemical Analysis (ALPACA) field campaign included deployment of a suite of atmospheric measurements in January–February 2022 with the goal of better understanding atmospheric processes and pollution under cold and dark conditions in Fairbanks, Alaska. We report on measurements of particle composition, particle size, ice nucleating particle (INP) composition, and INP size during an ice fog period (29 January–3 February). During this period, coarse particulate matter (PM 10 ) concentrations increased by 150% in association with a decrease in air temperature, a stronger temperature inversion, and relatively stagnant conditions. Results also show a 18%–78% decrease in INPs during the ice fog period, indicating that particles had activated into the ice fog via nucleation. Peroxide and heat treatments performed on INPs indicated that, on average, the largest contributions to the INP population were heat‐labile (potentially biological, 63%), organic (31%), then inorganic (likely dust, 6%). Measurements of levoglucosan and bulk and single‐particle composition corroborate the presence of dust and aerosols from combustion sources. Heat‐labile and organic INPs decreased during the peak period of the ice fog, indicating those were preferentially activated, while inorganic INPs increased, suggesting they remained as interstitial INPs. In general, INP concentrations were unexpectedly high in Fairbanks compared to other locations in the Arctic during winter. The fact that these INPs likely facilitated ice fog formation in Fairbanks has implications for other high latitude locations subject to the hazards associated with ice fog.

Meteorology & Atmospheric Sciences↗
DOE OSTI2020

A biogenic secondary organic aerosol source of cirrus ice nucleating particles

Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at –46°C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L –1 . Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

The Portable Ice Nucleation Experiment (PINE): a new online instrument for laboratory studies and automated long-term field observations of ice-nucleating particles

Atmospheric ice-nucleating particles (INPs) play an important role in determining the phase of clouds, which affects their albedo and lifetime. A lack of data on the spatial and temporal variation of INPs around the globe limits our predictive capacity and understanding of clouds containing ice. Automated instrumentation that can robustly measure INP concentrations across the full range of tropospheric temperatures is needed in order to address this knowledge gap. In this study, we demonstrate the functionality and capacity of the new Portable Ice Nucleation Experiment (PINE) to study ice nucleation processes and to measure INP concentrations under conditions pertinent for mixed-phase clouds, with temperatures from about -10 to about -40°C. PINE is a cloud expansion chamber which avoids frost formation on the cold walls and thereby omits frost fragmentation and related background ice signals during the operation. The development, working principle and treatment of data for the PINE instrument is discussed in detail. We present laboratory-based tests where PINE measurements were compared with those from the established AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber. Within experimental uncertainties, PINE agreed with AIDA for homogeneous freezing of pure water droplets and the immersion freezing activity of mineral aerosols. Results from a first field campaign conducted at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) observatory in Oklahoma, USA, from 1 October to 14 November 2019 with the latest PINE design (a commercially available PINE chamber) are also shown, demonstrating PINE's ability to make automated field measurements of INP concentrations at a time resolution of about 8 min with continuous temperature scans for INP measurements between -10 and -30°C. During this field campaign, PINE was continuously operated for 45 d in a fully automated and semi-autonomous way, demonstrating the capability of this new instrument to also be used for longer-term field measurements and INP monitoring activities in observatories.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Unexpected Phenomenology in Particle-Based Ice Absent in Magnetic Spin Ice

While particle-based ices are often considered essentially equivalent to magnet-based spin ices, the two differ essentially in frustration and energetics. Here, we show that at equilibrium particle-based ices correspond exactly to spin ices coupled to a background field. In trivial geometries, such a field has no effect, and the two systems are indeed thermodynamically equivalent. In other cases, however, the field controls a richer phenomenology, absent in magnetic ices, and still largely unexplored: ice rule fragility, topological charge transfer, radial polarization, decimation induced disorder, and glassiness.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

On the Role of Airborne Ice Nucleating Particles in Primary and Secondary Ice Formation Processes in Convective Midlatitude Clouds

Abstract Formation of ice in mixed-phase clouds may proceed via primary nucleation and secondary ice production (SIP). Primary nucleation involves the presence of ice nucleating particles (INPs), while SIP follows primary nucleation, resulting in ice crystal number concentrations N ice exceeding the number of INPs. The ice formation pathways in young congestus clouds are not well understood nor are the environmental conditions favorable for the onset of SIP. Coincident airborne measurements of INPs and N ice collected during the Secondary Production of Ice in Cumulus Experiment (SPICULE) campaign over the U.S. central Great Plains are reported for young congestus clouds. Number concentrations of INPs and N ice at temperatures between −10° and −20°C were used to categorize whether SIP was active in each analyzed cloud pass. Observational data suggested that fragmentation of freezing droplets (FFDs) was occurring and the most likely SIP mechanism for ice enhancement during the early stages of the sampled clouds, where higher cloud-base temperatures and stronger updrafts produced conditions favorable for the onset of FFD. Simple model simulations of a congestus cloud were used to compare predictions of N ice from newly implemented SIP mechanisms (including FFD) alongside those from the existing Hallett–Mossop (HM) mechanism. Although predicted N ice , when all SIP mechanisms were active, was in good agreement with observations, the dominant SIP mechanism in the model was predicted to be HM. The rate of heterogeneous freezing in raindrops was likely inhibiting realistic FFD rates in the simulated cloud. These discrepancies between the observations and simulations underscore the need for extended laboratory studies to formulate improved model representations of SIP in convective clouds.

Patnaude, Ryan J. [Department of Atmospheric Scien↗
NASA NTRS2017

How the Emitted Size Distribution and Mixing State of Feldspar Affect Ice Nucleating Particles in a Global Model

The effect of aerosol particles on ice nucleation and, in turn, the formation of ice and mixed phase clouds is recognized as one of the largest sources of uncertainty in climate prediction. We apply an improved dust mineral specific aerosol module in the NASA GISS Earth System ModelE, which takes into account soil aggregates and their fragmentation at emission as well as the emission of large particles. We calculate ice nucleating particle concentrations from K-feldspar abundance for an active site parameterization for a range of activation temperatures and external and internal mixing assumption. We find that the globally averaged INP concentration is reduced by a factor of two to three, compared to a simple assumption on the size distribution of emitted dust minerals. The decrease can amount to a factor of five in some geographical regions. The results vary little between external and internal mixing and different activation temperatures, except for the coldest temperatures. In the sectional size distribution, the size range 24 micrometer contributes the largest INP number.

Perlwitz, Jan P.↗
DOE OSTI2017

Contribution of feldspar and marine organic aerosols to global ice nucleating particle concentrations

Ice-nucleating particles (INPs) are known to affect the amount of ice in mixed-phase clouds, thereby influencing many of their properties. The atmospheric INP concentration changes by orders of magnitude from terrestrial to marine environments, which typically contain much lower concentrations. Many modelling studies use parameterizations for heterogeneous ice nucleation and cloud ice processes that do not account for this difference because they were developed based on INP measurements made predominantly in terrestrial environments without considering the aerosol composition. Errors in the assumed INP concentration will influence the simulated amount of ice in mixed-phase clouds, leading to errors in top-of-atmosphere radiative flux and ultimately the climate sensitivity of the model. Here we develop a global model of INP concentrations relevant for mixed-phase clouds based on laboratory and field measurements of ice nucleation by K-feldspar (an ice-active component of desert dust) and marine organic aerosols (from sea spray). The simulated global distribution of INP concentrations based on these two species agrees much better with currently available ambient measurements than when INP concentrations are assumed to depend only on temperature or particle size. Underestimation of INP concentrations in some terrestrial locations may be due to the neglect of INPs from other terrestrial sources. Our model indicates that, on a monthly average basis, desert dusts dominate the contribution to the INP population over much of the world, but marine organics become increasingly important over remote oceans and they dominate over the Southern Ocean. However, day-to-day variability is important. Because desert dust aerosol tends to be sporadic, marine organic aerosols dominate the INP population on many days per month over much of the mid- and high-latitude Northern Hemisphere. This study advances our understanding of which aerosol species need to be included in order to adequately describe the global and regional distribution of INPs in models, which will guide ice nucleation researchers on where to focus future laboratory and field work.

Vergara-Temprado, Jesús (ORCID:0000000231050946)↗
NASA NTRS1984

Ice depolarization on low-angle 2 GHz satellite downlinks

The impact of ice depolarization on the statistical performance of satellite downlinks were investigated. Propagation data recorded during 1979 and 1980 to see what impact of ice depolarization on link performance were analyzed. The effects on the cross polarization discrimination (XPD) statistics amounted to at most a 2 to 4 dB reduction in the XPD values which rain would have produced for a given percentage of time. Ice depolarization had no effect on the statistics of XPD values below the 0.01% level. Most of the severe ice depolarization events were associated with drops in barometric pressure and the passage of intense cold fronts through our area. Ice contents as the product of three individually undetermined quantities were defined: ice particle density, ice cloud thickness, and the average volume of the ice crystals. It is indicated that populations of ice particle with ice contents on the order of 0.002 m4/m3 are probably responsible for the lower values of measured XPD.

Stutzman, W. L.↗
DOE OSTI2025

Long-term measurements of ice nucleating particles at Atmospheric Radiation Measurement (ARM) sites worldwide

Ice nucleating particles (INPs) play a critical role in cloud microphysics and precipitation formation, yet long-term, spatially extensive observational datasets remain limited. Here, we present one of the most comprehensive publicly available datasets of immersion-mode INP concentrations using a single analytical method, generated through the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility. INP filter samples have been collected across a broad range of environments – including agricultural plains, Arctic coastlines, high-elevation mountain sites, marine regions, and urban areas – via fixed observatories, mobile facility deployments, and vertically-resolved tethered balloon system operations. We describe the standardized processing and quality assurance pipeline, from filter collection and processing using the Ice Nucleation Spectrometer to final data products archived on the ARM Data Discovery portal. The dataset includes both total INP concentrations and selectively treated samples, allowing for classification of biological, organic, and inorganic INP types. It features a continuous 5-year record of INP measurements from a central U.S. site, with data collection still ongoing. Seasonal and site-specific differences in INP concentrations are illustrated through intercomparisons at −10 and −20 °C, revealing distinct regional sources and atmospheric drivers. We also outline mechanisms for researchers to access existing data, request additional sample analyses, and propose future field campaigns involving ARM INP measurements. This dataset supports a wide range of scientific applications, from observational and mechanistic studies to model development, and provides critical constraints on aerosol-cloud interactions across diverse atmospheric regimes (Creamean et al., 2024, 2020b; https://doi.org/10.5439/1770816).

Creamean, Jessie M. [Colorado State Univ., Fort Co↗
DOE OSTI2014

Micro-Spectroscopic Imaging and Characterization of Individually Identified Ice Nucleating Particles from a Case Field Study

The effect of anthropogenic and biogenic organic particles on atmospheric glaciation processes is poorly understood. We use an optical microscopy (OM) setup to identify the location of ice nuclei (IN) active in immersion freezing and deposition ice nucleation for temperatures of 200-273 K within a large population of particles sampled from an ambient environment. Applying multi-modal micro-spectroscopy methods we characterize the physicochemical properties of individual IN in particle populations collected in central California. Chemical composition and mixing state analysis of particle populations are performed to identify characteristic particle-type classes. All particle-types contained organic material. Particles in these samples take up water at subsaturated conditions, induce immersion freezing at subsaturated and saturated conditions above 226 K, and act as deposition IN below 226 K. The identified IN belong to the most common particle-type classes observed in the field samples: organic coated sea salt, Na-rich, and secondary and refractory carbonaceous particles. Based on these observations, we suggest that the IN are not always particles with unique chemical composition and exceptional ice nucleation propensity; rather, they are common particles in the ambient particle population. Thus, particle composition and morphology alone are insufficient to assess their potential to act as IN. The results suggest that particle-type abundance is also a crucial factor in determining the ice nucleation efficiency of specific IN types. These findings emphasize that ubiquitous organic particles can induce ice nucleation under atmospherically relevant conditions and that they may play an important role in atmospheric glaciation processes.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2018

Ice rule fragility via topological charge transfer in artificial colloidal ice

Artificial particle ices are model systems of constrained, interacting particles. They have been introduced theoretically to study ice-manifolds emergent from frustration, along with domain wall and grain boundary dynamics, doping, pinning-depinning, controlled transport of topological defects, avalanches, and memory effects. Recently such particle-based ices have been experimentally realized with vortices in nano-patterned superconductors or gravitationally trapped colloids. Here we demonstrate that, although these ices are generally considered equivalent to magnetic spin ices, they can access a novel spectrum of phenomenologies that are inaccessible to the latter. With experiments, theory and simulations we demonstrate that in mixed coordination geometries, entropy-driven negative monopoles spontaneously appear at a density determined by the vertex-mixture ratio. Unlike its spin-based analogue, the colloidal system displays a “fragile ice” manifold, where local energetics oppose the ice rule, which is instead enforced through conservation of the global topological charge. The fragile colloidal ice, stabilized by topology, can be spontaneously broken by topological charge transfer.

36 MATERIALS SCIENCE↗