Search NASA⌕ Search

SEARCH · Search NASA

Results for “Ice Nucleation”

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.

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

At least 73 records · Page 4

African Dust Aerosols as Atmospheric Ice Nuclei

Measurements of the ice nucleating ability of aerosol particles in air masses over Florida having sources from North Africa support the potential importance of dust aerosols for indirectly affecting cloud properties and climate. The concentrations of ice nuclei within dust layers at particle sizes below 1 pn exceeded 1/cu cm; the highest ever reported with our device at temperatures warmer than homogeneous freezing conditions. These measurements add to previous direct and indirect evidence of the ice nucleation efficiency of desert dust aerosols, but also confirm their contribution to ice nuclei populations at great distances from source regions.

DeMott, Paul J.↗

Surface Crystallization of Supercooled Water in Clouds

The process by which liquid cloud droplets homogeneously crystallize into ice is still not well-understood. The ice nucleation process based on the standard and classical theory of homogeneous freezing, initiates within the interior volume of a cloud droplet. Current experimental data on homogeneous freezing rates of ice in droplets of supercooled water, both in air and emulsion oil samples, show considerable scatter. For example, at -33 C, the reported volume-based freezing rates of ice in supercooled water vary by as much as 5 orders of magnitude, which is well outside the range of measurement uncertainties. Here, we show that the process of ice nucleus formation at the air (or oil)-liquid water interface may help to explain why experimental results on ice nucleation rates yield different results in different ambient phases. Our results also suggest that surface crystallization of ice in cloud droplets can explain why low amounts of supercooled water have been observed in the atmosphere near -40 C.

Tabazadeh, Azadeh↗

On the Susceptibility of Cold Tropical Cirrus to Ice Nuclei Abundance

Numerical simulations of cirrus formation in the tropical tropopause layer (TTL) are used to evaluate the impact heterogeneous ice nuclei (IN) abundance on cold cloud microphysical properties. The model includes homogeneous and heterogeneous ice nucleation, deposition growthsublimation, and sedimentation. Reanalysis temperature and wind fields are used to force the simulations, with addition of high-frequency wave temperature variability based on in situ measurements. The model results are constrained by recent in situ observations of TTL cirrus and relative humidity, as well as satellite measurements of cirrus bulk properties and occurrence frequencies. Temperature variability driven by high-frequency waves has a dominant influence on TTL cirrus microphysical properties and occurrence frequencies, and inclusion of these waves is required to produce agreement between the simulated and observed cloud properties as well as the abundance of TTL cirrus. With a composition-independent supersaturation threshold for homogeneous freezing of aqueous aerosols, the model produces excessive ice concentrations compared with in situ observations. Inclusion of relatively numerous heterogeneous nuclei ( 100L) in the simulations improves the agreement with observed ice concentrations. However, when IN contribute significantly to TTL cirrus ice nucleation, the occurrence frequency of large supersaturations with respect to ice is less than indicated by in situ measurements. The simulated TTL cirrus extinction statistics agree with observations (within uncertainties) from both in situ and remote-sensing measurements. We find that the sensitivity of TTL cirrus extinction and ice water content statistics to heterogeneous ice nuclei abundance is relatively weak. Likewise, the simulated occurrence frequencies of TTL cirrus are insensitive to ice nuclei abundance, both in terms of cloud frequency height distribution and regional distribution throughout the tropics.

occurences↗

Midlatitude Cirrus Clouds Derived from Hurricane Nora: A Case Study with Implications for Ice Crystal Nucleation and Shape

Hurricane Nora traveled up the Bala Peninsula coast in the unusually warm El Nino waters of September 1997, until rapidly decaying as it approached Southern California on 24 September. The anvil cirrus blowoff from the final surge of tropical convection became embedded in subtropical flow that advected the cirrus across the western US, where it was studied from the Facility for Atmospheric Remote Sensing (FARS) in Salt Lake City, Utah. A day later, the cirrus shield remnants were redirected southward by midlatitude circulations into the Southern Great Plains, providing a case study opportunity for the research aircraft and ground-based remote sensors assembled at the Clouds and Radiation Testbed (CART) site in northern Oklahoma. Using these comprehensive resources and new remote sensing cloud retrieval algorithms, the microphysical and radiative cloud properties of this unusual cirrus event are uniquely characterized. Importantly, at both the FARS and CART sites the cirrus generated spectacular optical displays, which acted as a tracer for the hurricane cirrus, despite the limited lifetimes of individual ice crystals. Lidar polarization data indicate widespread regions of uniform ice plate orientations, and in situ particle masticator data show a preponderance of pristine, solid hexagonal plates and columns. It is suggested that these unusual aspects are the result of the mode of cirrus particle nucleation, presumably involving the lofting of sea-salt nuclei in thunderstorm updrafts into the upper troposphere. This created a reservoir of haze particles that continued to produce halide-saltcontaminated ice crystals during the extended period of cirrus cloud maintenance. The reference that marine microliters are embedded in the replicas of ice crystals collected over the CART site points to the longevity of marine effects. Various nucleation scenarios proposed for cirrus clouds based on this and other studies, and the implications for understanding cirrus radiative properties or a global scale, are discussed.

Sassen, Kenneth↗

Influence of Nucleation Mechanisms on the Radiative Properties of Deep Convective Clouds and Subvisible Cirrus in CRYSTAL/FACE

During the past few years we have conducted work on several different topics, as reflected by our publications. As one of the Co-Project scientists for The Cirrus Regional Study of Tropical Anvils and Cirrus Layers - Florida Area Cirrus Experiment (CRYSTAL FACE) we worked to help design the mission and then conduct it in the field. Another major activity during the past two years has been to pull together various groups to formulate plans for follow on missions to CRYSTAL FACE. We organized a workshop at the University of Colorado during the summer of 2003 to assess the best locations for future missions. Working with a group of about 10 scientists from around the country we prepared a science-planning document (Tropical Composition, Cloud and Climate Coupling Experiment (TC(sup 4)) that outlined the rationale, locations, strategy to accomplish the goals, and possible payloads for a set of three tropical missions. We also prepared background materials for various NRAs being prepared at NASA Headquarters for missions in Costa Rica, Darwin and Guam. In conjunction with the group at NASA Ames we have helped build a new numerical model for deep convection and have applied that model to simulate the CRYSTAL data. Our goal in particular has been to better understand how convection distributes water vapor isotopes. CRYSTAL observations of water isotopes are very different from those suggested by previous workers who assumed the isotopes would obey Rayleigh fractionation. The water isotope study has several implications. First it is a check on the realism of the deep convection model. Second, the isotopes are a measure of the precipitation removal in the atmosphere. Hence they provide a constraint on a parameter that is difficult to otherwise measure. Finally it has been suggested that isotopes may be the key to unraveling the water transport into the stratosphere and upper troposphere. Such transport is critical both for the radiation balance and for stratospheric chemistry. Ours is the first model that is able to treat this transport. Our initial results have just been submitted to Geophys. Res. Lett (Smith et al., 2005). Essentially we are able to explain the vertical profiles of isotopes in the tropical tropopause transition layer. We are also able to account for stratospheric humidity and isotope abundances with this model. We have also been heavily involved in trying to improve our understanding of nitric acid condensation on ice. Gao et al (2004) have shown that water supersaturations above ice occur when the atmosphere is supersaturated with respect to nitric acid trihydrate. As one of the co-authors of that work, we suggested the mechanism that may explain why this is occurring. Essentially, ice does not like to grow near unit supersaturation, but does so because the water molecules can find sites on the ice surface to attach themselves to before they fly off the ice surface. This phenomena was well known in the 1960s when it was a source of debate about whether condensation and evaporation coefficients for ice would be the same. Evaporation does not require any molecular orientation, while condensation does, so it was possible that the coefficients would differ. They don't differ because the water molecules rapidly move across the surface and find places to attach. Nitric acid may be occupying these preferred sites and therefore the water molecules can't find a desirable place to attach. We anticipate that this research will be the subject of laboratory work during the coming few years. Another possibility that has been suggested is that cubic ice is forming in clouds. We have measured the vapor pressure of cubic ice, and plan to publish that result in the next few months. We have also been working on additional aspects of the condensation of nitric acid on ice. With Y. Kondo we studied the condensation of NOy on ice using the SOLVE data. Gamblin et al. have continued this work. The CRYSTAL NOy and HNO, groups have shown th their data can be fit using standard Langmuir isotherms as suggested in some, but not all, laboratory studies. We have found in the SOLVE data set that this is not the case. Moreover some laboratory studies show there are important kinetic effects that may be occurring in the atmosphere limiting the transfer of nitric acid to the ice. The SOLVE data seem consistent with these studies. We are currently re-analyzing the CRYSTAL data to look for these kinetic effects. There are a number of implications of these studies. One of the more interesting is that the nitric acid coating on ice can be used as a cloud clock to determine how long the cloud parcel has been in existence. We have also been involved with several laboratory studies. We have worked to improve the database on ice optical constants, which are critical for remote sensing. We have also studied the ways in which ice nucleates on clays. We suspect now that the standard theories used for depositional ice nucleation are completely incorrect. Further work will be needed to develop a new theory.

Toon, Owen B.↗

Saharan Dust Event Impacts on Cloud Formation and Radiation over Western Europe

We investigated the impact of mineral dust particles on clouds, radiation and atmospheric state during a strong Saharan dust event over Europe in May 2008, applying a comprehensive online-coupled regional model framework that explicitly treats particle-microphysics and chemical composition. Sophisticated parameterizations for aerosol activation and ice nucleation, together with two-moment cloud microphysics are used to calculate the interaction of the different particles with clouds depending on their physical and chemical properties. The impact of dust on cloud droplet number concentration was found to be low, with just a slight increase in cloud droplet number concentration for both uncoated and coated dust. For temperatures lower than the level of homogeneous freezing, no significant impact of dust on the number and mass concentration of ice crystals was found, though the concentration of frozen dust particles reached up to 100 l-1 during the ice nucleation events. Mineral dust particles were found to have the largest impact on clouds in a temperature range between freezing level and the level of homogeneous freezing, where they determined the number concentration of ice crystals due to efficient heterogeneous freezing of the dust particles and modified the glaciation of mixed phase clouds. Our simulations show that during the dust events, ice crystals concentrations were increased twofold in this temperature range (compared to if dust interactions are neglected). This had a significant impact on the cloud optical properties, causing a reduction in the incoming short-wave radiation at the surface up to -75Wm-2. Including the direct interaction of dust with radiation caused an additional reduction in the incoming short-wave radiation by 40 to 80Wm-2, and the incoming long-wave radiation at the surface was increased significantly in the order of +10Wm-2. The strong radiative forcings associated with dust caused a reduction in surface temperature in the order of -0.2 to -0.5K for most parts of France, Germany, and Italy during the dust event. The maximum difference in surface temperature was found in the East of France, the Benelux, and Western Germany with up to -1 K. This magnitude of temperature change was sufficient to explain a systematic bias in numerical weather forecasts during the period of the dust event.

Bangert, M.↗

Cirrus Susceptibility to Changes in Ice Nuclei: Physical Processes, Model Uncertainties, and Measurement Needs

One of the proposed concepts for mitigating the warming effect of increasing greenhouse gases is seeding cirrus cloud with ice nuclei (IN) in order to reduce the lifetime and coverage of cold cirrus that have a net warming impact on the earth's surface. Global model simulations of the net impact of changing upper tropospheric IN have given widely disparate results, partly as a result of poor understanding of ice nucleation processes in the current atmosphere, and partly as a result of poor representation of these processes in global models. Here, we present detailed process-model simulations of tropical tropopause layer (TTL) transport and cirrus formation with ice nuclei properties based on recent laboratory nucleation experiments and field measurements of aerosol composition. The model is used to assess the sensitivity of TTL cirrus occurrence frequency and microphysical properties to the abundance and efficacy of ice nuclei. The simulated cloud properties compared with recent high-altitude aircraft measurements of TTL cirrus and ice supersaturation. We find that abundant effective IN (either from glassy organic aerosols or crystalline ammonium sulfate with concentrations greater than about 100/L) prevent the occurrences of large ice concentration and large ice supersaturations, both of which are clearly indicated by the in situ observations. We find that concentrations of effective ice nuclei larger than about 50/L can drive significant changes in cirrus microphysical properties and occurrence frequency. However, the cloud occurrence frequency can either increase or decrease, depending on the efficacy and abundance of IN added to the TTL. We suggest that our lack of information about ice nuclei properties in the current atmosphere, as well as uncertainties in ice nucleation processes and their representations in global models, preclude meaningful estimates of climate impacts associated with addition of ice nuclei in the upper troposphere. We will briefly discuss the key field measurements needed to constrain ice nucleation processes.

Jensen, Eric↗

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↗

Homogeneous condensation - Freezing nucleation rate measurements for small water droplets in an expansion cloud chamber

Experimental data on ice nucleation, presented in an earlier paper, are analyzed to yield information about the homogeneous nucleation rate of ice from supercooled liquid and the heights of energy barriers to that nucleation. The experiment consisted of using an expansion cloud chamber to nucleate from the vapor a cloud of supercooled pure water drops and the observation of the fraction of drops which subsequently froze. The analysis employed standard classical homogeneous nucleation theory. The data are used to extract the first experimental measurement (albeit indirect) of the activation energy for the transfer of a water molecule across the liquid-ice interface at temperatures near -40 C. The results provide further evidence that the local liquid structure becomes more icelike as the temperature is lowered.

Hagen, D. E.↗

Formation of Large (Approximately 100 micrometers) Ice Crystals Near the Tropical Tropopause

Recent high-altitude aircraft measurements with in situ imaging instruments indicated the presence of relatively large (approx.100 microns length), thin (aspect ratios of approx.6:1 or larger) hexagonal plate ice crystals near the tropical tropopause in very low concentrations (<0.01/L). These crystals were not produced by deep convection or aggregation. We use simple growth-sedimentation calculations as well as detailed cloud simulations to evaluate the conditions required to grow the large crystals. Uncertainties in crystal aspect ratio leave a range of possibilities, which could be constrained by knowledge of the water vapor concentration in the air where the crystal growth occurred. Unfortunately, water vapor measurements made in the cloud formation region near the tropopause with different instruments ranged from <2 ppmv to approx.3.5 ppmv. The higher water vapor concentrations correspond to very large ice supersaturations (relative humidities with respect to ice of about 200%). If the aspect ratios of the hexagonal plate crystals are as small as the image analysis suggests (6:1, see companion paper (Lawson et al., 2008)) then growth of the large crystals before they sediment out of the supersaturated layer would only be possible if the water vapor concentration were on the high end of the range indicated by the different measurements (>3 ppmv). On the other hand, if the crystal aspect ratios are quite a bit larger (approx.10:1), then H2O concentrations toward the low end of the measurement range (approx.2-2.5 ppmv) would suffice to grow the large crystals. Gravity-wave driven temperature and vertical wind perturbations only slightly modify the H2O concentrations needed to grow the crystals. We find that it would not be possible to grow the large crystals with water concentrations less than 2 ppmv, even with assumptions of a very high aspect ratio of 15 and steady upward motion of 2 cm/s to loft the crystals in the tropopause region. These calculations would seem to imply that the measurements indicating water vapor concentrations less than 2ppmv are implausible, but we cannot rule out the possibility that higher humidity prevailed upstream of the aircraft measurements and the air was dehydrated by the cloud formation. Simulations of the cloud formation with a detailed model indicate that homogeneous freezing should generate ice concentrations larger than the observed concentrations (20/L), and even concentrations as low as 20/L should have depleted the vapor in excess of saturation and prevented growth of large crystals. It seems likely that the large crystals resulted from ice nucleation on effective heterogeneous nuclei at low ice supersaturations. Improvements in our understanding of detailed cloud microphysical processes require resolution of the water vapor measurement discrepancies in these very cold, dry regions of the atmosphere.

Jensen, E. J.↗

Effect of volcanic emissions on clouds during the 2008 and 2018 Kilauea degassing events

Volcanic eruptions in otherwise clean environments are “natural experiments” wherein the effects of aerosol emissions on clouds and climate can be partitioned from meteorological variability and anthropogenic activities. In this work, we combined satellite retrievals, reanalysis products, and atmospheric modeling to analyze the mechanisms of aerosol–cloud interactions during two degassing events at the Kilauea volcano in 2008 and 2018. The eruptive nature of the 2008 and 2018 degassing events was distinct from long-term volcanic activity for Kilauea. Although previous studies assessed the modulation of cloud properties from the 2008 event, this is the first time such an analysis has been reported for the 2018 event and that multiple degassing events have been analyzed and compared at this location. Both events resulted in significant changes in cloud effective radius and cloud droplet number concentration that were decoupled from local meteorology and in line with an enhanced cloud albedo. However, it is likely that the effects of volcanic emissions on liquid water path and cloud fraction were largely offset by meteorological variability. Comparison of cloud anomalies between the two events suggested a threshold response of aerosol–cloud interactions to overcome meteorological effects, largely controlled by aerosol loading. In both events, the ingestion of aerosols within convective parcels enhanced the detrainment of condensate in the upper troposphere, resulting in deeper clouds than observed under pristine conditions. Accounting for ice nucleation on ash particles led to enhanced ice crystal concentrations at cirrus levels and a slight decrease in ice water content, improving the correlation of the model results with the satellite retrievals. Overall, aerosol loading, plume characteristics, and meteorology contributed to changes in cloud properties during the Kilauea degassing events.

Katherine H. Breen↗

GCSS Cirrus Parcel Model Comparison Project

The Cirrus Parcel Model Comparison Project, a project of GCSS Working Group on Cirrus Cloud Systems (WG2), involves the systematic comparison of current models of ice crystal nucleation and growth for specified, typical, cirrus cloud environments. The goal of this project is to document and understand the factors resulting in significant inter-model differences. The intent is to foment research leading to model improvement and validation. In Phase 1 of the project reported here, simulated cirrus cloud microphysical properties are compared for situations of "warm" (-40 C) and "cold" (-60 C) cirrus subject to updrafts of 4, 20 and 100 cm/s, respectively. Five models participated. These models employ explicit microphysical schemes wherein the size distribution of each class of particles (aerosols and ice crystals) is resolved into bins. Simulations are made including both homogeneous and heterogeneous ice nucleation mechanisms. A single initial aerosol population of sulfuric acid particles is prescribed for all simulations. To isolate the treatment of the homogeneous freezing (of haze drops) nucleation process, the heterogeneous nucleation mechanism is disabled for a second parallel set of simulations. Qualitative agreement is found for the homogeneous-nucleation-only simulations, e.g., the number density of nucleated ice crystals increases with the strength of the prescribed updraft. However, non-negligible quantitative differences are found. Detailed analysis reveals that the homogeneous nucleation formulation, aerosol size, ice crystal growth rate (particularly the deposition coefficient), and water vapor uptake rate are critical components that lead to differences in predicted microphysics. Systematic bias exists between results based on a modified classical theory approach and models using an effective freezing temperature approach to the treatment of nucleation. Each approach is constrained by critical freezing data from laboratory studies, but each includes assumptions that can only be justified by further laboratory data. Consequently, it is not yet clear if the two approaches can be made consistent. Large haze particles may deviate considerably from equilibrium size in moderate to strong updrafts (20-100 cm/s) at -60 C when the commonly invoked equilibrium assumption is lifted. The resulting difference in particle-size-dependent solution concentration of haze particles may significantly affect the ice nucleation rate during the initial nucleation interval. The uptake rate for water vapor excess by ice crystals is another key component regulating the total number of nucleated ice crystals. This rate, the product of ice number concentration and ice crystal diffusional growth rate, which is sensitive to the deposition coefficient when ice particles are small, partially controls the peak nucleation rate achieved in an air parcel and the duration of the active nucleation time period. The effects of heterogeneous nucleation are most pronounced in weak updraft situations. Vapor competition by the nucleated (heterogeneous) ice crystals limits the achieved ice supersaturation and thus suppresses the contribution of homogeneous nucleation. Correspondingly, ice crystal number density is markedly reduced. Definitive laboratory and atmospheric benchmark data are needed for the heterogeneous nucleation process. Inter-model differences are correspondingly greater than in the case of the homogeneous nucleation process acting alone.

Lin, Ruei-Fong↗

The Cirrus Parcel Model Comparison Project

The cirrus Parcel Model Comparison Project involves the systematic comparison of current models of ice crystal nucleation and growth for specified, typical, cirrus cloud environments. In Phase 1 of the project reported here, simulated cirrus cloud microphysical properties are compared for situations of "warm" (-40 C) and "cold" (-60 C) cirrus subject to updrafts of 4, 20 and 100 centimeters per second, respectively. Five models are participating in the project. These models employ explicit microphysical schemes wherein the size distribution of each class of particles (aerosols and ice crystals) is resolved into bins. Simulations are made including both homogeneous and heterogeneous ice nucleation mechanisms. A single initial aerosol population of sulfuric acid particles is prescribed for all simulations. To isolate the treatment of the homogeneous freezing (of haze drops) nucleation process, the heterogeneous nucleation mechanism is disabled for a second parallel set of simulations. Qualitative agreement is found amongst the models for the homogeneous-nucleation-only simulations, e.g., the number density of nucleated ice crystals increases with the strength of the prescribed updraft. However, non-negligible quantitative differences are found. Systematic bias exists between results of a model based on a modified classical theory approach and models using an effective freezing temperature approach to the treatment of nucleation. Each approach is constrained by critical freezing data from laboratory studies. This information is necessary, but not sufficient, to construct consistent formulae for the two approaches. Large haze particles may deviate considerably from equilibrium size in moderate to strong updrafts (20-100 centimeters per second) at -60 C when the commonly invoked equilibrium assumption is lifted. The resulting difference in particle-size-dependent solution concentration of haze particles may significantly affect the ice nucleation rate during the initial nucleation interval. The uptake rate for water vapor excess by ice crystals is another key component regulating the total number of nucleated ice crystals. This rate, the product of ice number concentration and ice crystal diffusional growth rate, partially controls the peak nucleation rate achieved in an air parcel and the duration of the active nucleation time period.

Lin, Ruei-Fong↗

Aerosol-Ice Formation Closure Pilot Study (AEROICSTUDY) Field Campaign Report

The aerosol-ice formation closure pilot study (AEROICESTUDY) was a field campaign conducted at the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility at the Southern Great Plains (SGP) observatory from October 7 to 28, 2019. The purpose of this campaign was to test a field observational approach for conducting an aerosol-ice formation closure study. In other words, the goal was to predict the number of ice nucleating particles (INPs) from the measurements of physical and chemical aerosol properties and compare those to measured INP number concentrations. This project was motivated by the fact that the aerosol community has widely conducted aerosol radiative closure, aerosol-cloud condensation nuclei (CCN), and CCN-droplet closure studies to test the physical models and parameterizations that cloud-resolving and climate models rely on to perform reliable simulations of the Earth system and energy budget. However, very few closure studies related to INPs have been conducted, and to our knowledge, none using robust, size-resolved, ambient aerosol composition measurements as model inputs.

aerosol-ice formation↗

Aerosol-Ice Formation Closure Pilot Study (AEROICESTUDY) Field Campaign Report

The aerosol-ice formation closure pilot study (AEROICESTUDY) was a field campaign conducted at the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility at the Southern Great Plains (SGP) observatory from October 7 to 28, 2019. The purpose of this campaign was to test a field observational approach for conducting an aerosol-ice formation closure study. In other words, the goal was to predict the number of ice nucleating particles (INPs) from the measurements of physical and chemical aerosol properties and compare those to measured INP number concentrations. This project was motivated by the fact that the aerosol community has widely conducted aerosol radiative closure, aerosol-cloud condensation nuclei (CCN), and CCN-droplet closure studies to test the physical models and parameterizations that cloud-resolving and climate models rely on to perform reliable simulations of the Earth system and energy budget. However, very few closure studies related to INPs have been conducted, and to our knowledge, none using robust, size-resolved, ambient aerosol composition measurements as model inputs

AEROICESTUDY↗

Ice Cloud Formation and Dehydration in the Tropical Tropopause Layer

Stratospheric water vapor is important not only for its greenhouse forcing, but also because it plays a significant role in stratospheric chemistry. several recent studies have focused on the potential for dehydration due to ice cloud formation in air rising slowly through the tropical tropopause layer. Holton and Gettelman showed that temperature variations associated with horizontal transport of air in the tropopause layer can drive ice cloud formation and dehydration, and Gettelman et al. recently examined the cloud formation and dehydration along kinematic trajectories using simple assumptions about the cloud properties. In this study, we use a Lagrangian, one-dimensional cloud model to further investigate cloud formation and dehydration as air is transported horizontally and vertically through the tropical tropopause layer. Time-height curtains of temperature are extracted from meteorological analyses. The model tracks the growth and sedimentation of individual cloud particles. The regional distribution of clouds simulated in the model is comparable to the subvisible cirrus distribution indicated by SAGE II. The simulated cloud properties depend strongly on the assumed ice supersaturation threshold for ice nucleation. with effective nuclei present (low supersaturation threshold), ice number densities are high (0.1--10 cm(circumflex)-3), and ice crystals do not grow large enough to fall very far, resulting in limited dehydration. With higher supersaturation thresholds, ice number densities are much lower (less than 0.01 cm(circumflex)-3), and ice crystals grow large enough to fall substantially; however, supersaturated air often crosses the tropopause without cloud formation. The clouds typically do not dehydrate the air along trajectories down to the temperature minimum saturation mixing ratio. Rather the water vapor mixing ratio crossing the tropopause along trajectories is typically 10-50% larger than the saturation mixing ratio.

Jensen, Eric↗

Preconditioning of overcast-to-broken cloud transitions by riming in marine cold air outbreaks

Marine cold air outbreaks (CAOs) commonly form overcast cloud decks that transition into broken cloud fields downwind, dramatically altering the local radiation budget. In this study, we investigate the impact of frozen hydrometeors on these transitions. We focus on a CAO case in the NW Atlantic, the location of the multi-year flight campaign ACTIVATE (Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment). We use MERRA-2 (Modern-Era Retrospective analysis for Research and Applications, version 2) reanalysis fields to drive large eddy simulations with mixed-phase two-moment microphysics in a Lagrangian framework. We find that transitions are triggered by substantial rain (rainwater paths >25 g m−2), and only simulations that allow for aerosol depletion result in sustained breakups, as observed. Using a range of diagnostic ice nucleating particle concentrations, Ninp, we find that increasing ice progressively accelerates transitions, thus abbreviating the overcast state. Ice particles affect the cloud-topped boundary layer evolution, primarily through riming-related processes prior to substantial rain, leading to (1) a reduction in cloud liquid water, (2) early consumption of cloud condensation nuclei, and (3) early and light precipitation cooling and moistening below cloud. We refer to these three effects collectively as “preconditioning by riming”. Greater boundary layer aerosol concentrations available as cloud condensation nuclei (CCN) delay the onset of substantial rain. However, cloud breakup and low CCN concentration final stages are found to be inevitable in this case, due, primarily, to liquid water path buildup. An ice-modulated cloud transition speed suggests the possibility of a negative cloud–climate feedback. To address prevailing uncertainties in the model representation of mixed-phase processes, the magnitude of ice formation and riming impacts and, thereby, the strength of an associated negative cloud–climate feedback process, requires further observational evaluation by targeting riming hot spots with in situ imaging probes that allow for both the characterization of ice particles and abundance of supercooled droplets.

Marine cold air outbreaks↗