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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 OSTI2022

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

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

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Ice Nucleating Particles, Aerosols and Clouds over the Higher Latitude Southern Ocean

Improved understanding of aerosol-cloud-precipitation interactions is a key goal of the DOE-ASR program. Ice Nucleating Particles (INPs) are rare aerosol particles that trigger ice formation in clouds. By doing so they may initiate precipitation in clouds, and this impacts cloud lifetime. Nowhere may the role of INPs be manifested so dramatically as in the Southern Ocean (SO). This vast region was the focus of the DOE-ARM MARCUS (Measurement of Aerosols, Radiation and CloUds over the Southern Oceans) and MICRE (Macquarie Island Cloud and Radiation Experiment) campaigns. In the SO, a deficit of INPs has been a leading hypothesis for why liquid clouds persist, which underlays the bias of global climate models in predicting excess shortwave radiation reaching the ocean surface between 55°S and Antarctica. In this study, we used the 6-month acquisition of INP data on four MARCUS cruises from Hobart, Tasmania, to Antarctica, and the single-location full annual INP cycle observed in MICRE, to gain a holistic, quantitative picture of the INP number concentrations as a function of temperature and their variability over SO latitudes from 43°S to Antarctica. Augmenting initial processing of filter collections of aerosol particles during MARCUS and MICRE, additional freezing studies following thermal treatment (to removes INPs associated with microbes) and peroxide treatment (to remove all organics), as well as ionic chemistry and total organic carbon analysis, were applied to samples to improve time and space resolution, and differentiate marine from terrestrial contributions. We also performed Next Generation Sequencing to determine that bacterial composition can tag periods of enhanced and degraded marine organic INPs and the relative lack of occurrence of land-sourced bio-particles. Through these and other analyses, INP data were categorized into representative source types (e.g., marine versus terrestrially-influenced). The products of our analyses are being used to parameterize ice formation for use in numerical modeling studies to determine if, and when, ocean-derived INPs control the microphysical composition and radiative balance of SO clouds in a manner not presently captured by global models. The specific objectives and approaches proposed were largely accomplished, including: 1) Additional and value-added chemical and biological analyses of archived samples of aerosols were completed to categorize and quantify INP types and concentrations over the SO. 2) Analyses were completed to place INP data in meteorological and aerosol context. 3) Sea spray aerosol INPs were demonstrated to dominate the SO region in all but episodic events. 4) New parameterizations for INP sources relevant to the SO were constructed. 5) Collaborative modeling studies demonstrating the crucial role of INPs in determining cloud radiative and precipitation properties were conducted with MARCUS and MICRE partners. Collaborative publication submissions in this regard ensued within the two year study. This work will advance the science of interactions of aerosols, clouds and precipitation, to improve their representation in regional and global climate models. Results have informed representation of primary ice crystal nucleation, give inference to the role of secondary processes, and improve investigations of aerosol influences on clouds via ice nucleation over SO high latitudes and similar vast ocean regions. Application will improve representation of such interactions for clouds in both regional and global climate models. The data base and analyses methods applied will continue to serve research studies in the future.

58 GEOSCIENCES↗
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 OSTI2025

Advancing the Understanding of Cloud Microphysical Processes and Aerosol Indirect Effects in High-Latitude Mixed-Phase Clouds by Linking ARM Measurements with Climate Model Simulations (Final Report)

The key objectives of this project were to advance our understanding of cloud microphysical characteristics and aerosol indirect effects on mixed-phase clouds in high latitudes. To improve the representation of ice and mixed-phase clouds in Earth System Models (ESMs), we propose an integrated observation and modeling study of cloud macro- and microphysical properties, including spatial heterogeneities, mass partitioning between ice crystals and supercooled liquid water, effects of ice nucleating particles (INPs), and efficiency of secondary ice production (SIP), etc. Specifically, we took four main approaches in this project: (1) examining macro- and microphysical properties of ice and mixed-phase clouds based on in-situ and ground-based observations from multiple field campaigns funded by the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program, including the Mixed-Phase Arctic Cloud Experiment (M-PACE), Indirect and Semi-Direct Aerosol Campaign (ISDAC), Ice Nucleating Particle Sources at Oliktok Point (INPOP), ARM West Antarctic Radiation Experiment (AWARE), Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS), and Macquarie Island Cloud and Radiation Experiment (MICRE); (2) evaluating the DOE Energy Exascale Earth System Model (E3SM) simulations based on observations, particularly for ice and mixed-phase cloud microphysical properties; (3) examining the impacts of INPs on ice and mixed-phase clouds. Specifically, a series of comparisons were conducted using observations over the Arctic, Southern Ocean, and Antarctica, including comparisons between the lower and higher southern latitudes as well as comparisons between the northern and southern hemispheres. In addition, aerosol indirect effects from distinct sources of dust particles were examined; and (4) investigating the impacts of SIP. Ultimately, these results helped to improve cloud microphysics and aerosol-cloud interaction parameterizations in the E3SM model. Overall, the project provided improved understanding regarding various factors, including thermodynamic, dynamic, and aerosol conditions, on the micro- and macrophysical properties of ice and mixed-phase clouds in the high latitudes. Resulting analysis helped to provide an improved physical basis for refining the current cloud microphysics parameterizations related to ice and mixed-phase clouds in E3SM.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Use of Remote Sensing and In-Situ Observations to Develop and Evaluate Improved Representations of Convection and Clouds for the ACME Model

The overachieving goal of the whole CMDV-MCS project is to improve understanding of warm season continental convection and to develop treatments of convection and microphysics capable of representing mesoscale convective systems (MCSs) features in large-scale models. Our tasks for this project contributing to the overachieving goal include: (1) Improve the ice nucleation formulation for MG2 and P3 cloud microphysics schemes; (2) Improve the treatment of subgrid dynamics and thermodynamics driving the ice nucleation in E3SM; and (3) Test the performance of improved ice microphysics in E3SM with observation data. In this project, we have (1) Improved the ice nucleation parameterization for MG2 and P3 in E3SM by implementing two advanced empirical parameterizations with connection to aerosols. The two deterministic heterogeneous ice nucleation parameterizations (i.e., DeMott et al., 2015; Niemand et al., 2012) were merged with the MG2 and P3 cloud microphysics schemes in E3SM. Long-term simulations were conducted to examine the impacts of these new parameterizations on simulated cloud properties; (2) Improved the treatment of subgrid dynamics and thermodynamics driving the ice nucleation in E3SM. We evaluated the double Gaussian PDF of vertical velocity simulated by the Cloud Layers Unified By Binormals (CLUBB) and the sub-column vertical velocity sampled from the Subgrid Importance Latin Hypercube Sampler (SILHS) in E3SM. We introduced the vertical velocity variance induced by topographic gravity waves for ice nucleation and droplet activation; and (3) Tested the performance of improved ice microphysics in E3SM with observation data. We tested the new treatments of ice nucleation in the single column model (SCM) mode for the stratiform mixed-phase clouds observed during 9-10 October 2004 in the DOE ARM Mixed-Phase Arctic Cloud Experiment (M-PACE) and for the convective clouds observed on 20 May 2011 in the Midlatitude Continental Convective Clouds Experiment (MC3E). Modeled ice nucleating particles (INPs) concentrations were compared against observations collected around the globe.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Assessing Secondary Ice Production in Continental Clouds Based on AMF Synergistic Remote Sensing Observations

Ice crystals play an important role in radiation and precipitation formation. However, the prediction of ice number concentration has proven to be problematic, because the predicted concentration of ice nucleating particles is often smaller than the observed by several orders of magnitude. This difference between the observed and the predicted number concentration has been explained by so-called secondary ice production (SIP), which includes hypothesized mechanisms like rime splintering, shattering of large frozen drops, and ice-ice collision breakup. To better observe SIP and understand its frequency, production rate, and impact on cloud evolution, we developed a new method for retrieving microphysical properties of concurrent pristine ice and snow aggregates from X-band polarimetric radar observations. Compared to aircraft cloud probe measurements, our retrieved total number concentration and ice water content are overestimated by 98% and 44%, respectively, which outperforms other empirical relationships. The capability of quantifying pristine ice number concentration, which is the most essential observable in SIP studies, opens a new opportunity to build a long-term record of SIP from surface-based radar measurements. We have also conducted simulations using a cloud-resolving model to evaluate the representativeness of the parameterizations of three SIP mechanisms and for studying the impact of SIP on a frontal system. We found a surprisingly good agreement between the observed and retrieved pristine ice number concentrations. The good performance is attributed to the rime splintering process in the temperature zone between–3° and –8°C, and to the ice-ice collision breakup process at higher altitudes. The impact of the shattering of large frozen drops appears minimal. Apart from the enhancement of ice number concentration and increased horizontal coverage of pristine ice, the addition of three SIP processes does not change cloud evolutions dramatically in our simulations.

58 GEOSCIENCES↗
DOE OSTI2020

Improving GCM Predictability of Mixed-Phase Clouds and Aerosol Interactions at High Latitudes with ARM Observations

The overachieving goal of this project is to improve the predictability of mixed-phase clouds and aerosol interactions in the Community Atmosphere Model version 6 (CAM6) through comparison with the ARM observations. There are three main objectives of the proposed study: (1) Improve the representation of ice microphysical processes in mixed-phase clouds; (2) Test the performance of ice microphysics in CESM-CAM6 with the ARM observations in northern and southern high latitudes; and (3) Examine mixed-phase cloud microphysics-aerosol-turbulence-radiation interactions in CESM-CAM6. In this project, we have (1) Improved the representation of ice microphysical processes in mixed-phase clouds in CESM-CAM6 by implementing the marine organic aerosol (MOA) and treating the ice nucleating particles (INPs) from MOA and its impacts on mixed-phase clouds. We improved the treatment of ice depositional growth through the Wegener–Bergeron–Findeisen (WBF) process by considering the subgrid heterogeneous distributions between liquid droplets and ice crystals in mixed-phase clouds; (2) Tested the performance of ice microphysics in CESM-CAM6 with the ARM observations at high latitudes. We compared the simulated INP concentrations with the ARM observations, e.g., from M-PACE, ISDAC, INPOP, and other data (Mace Head, Zeppelin, CAPRICORN). We examined the impact of improved WBF treatment on model simulated Arctic mixed-phase clouds observed in the M-PACE field campaign. Seasonal variations of modeled mixed-phase cloud properties (LWO, IWP) are compared with the ground-based remote sensing retrievals at the ARM’s NSA $Utqia\dot{g}vik$ site; and (3) Examined mixed-phase cloud microphysics-aerosol-dynamics-radiation interactions in CESM-CAM6 that include the impacts of MOA INPs, and impacts of different model parameterizations (CLUBB versus UW turbulence & shallow convection schemes, MG2 versus MG1) on high-latitude mixed-phase cloud properties. Aerosol indirect effects of MOA through the liquid phase (droplet activation) and ice phase processes (e.g., the glaciation indirect effect) were investigated.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Simulated Dust Transport in the Convective Boundary Layer

Soil dusts are an important source of aerosol in agricultural regions and can affect the Earth's radiation budget through the modification of cloud properties, and in particular, through their ability to act as ice nucleating particles. In order to impact cloud properties, agricultural soil dusts need to be transported from the point of emission to cloud–relevant altitudes. Vertical transport within the planetary boundary layer is strongly controlled by turbulence and is challenging to represent accurately in regional and global models. Large–eddy simulations (LES) are run at resolutions capable of resolving most of the turbulent energy directly and can thus better simulate vertical transport. In this study, we leverage the LES ARM Symbiotic Simulation and Observation (LASSO) large–eddy simulations to simulate vertical transport of agricultural dust within the turbulent boundary layer using a modified version of the stochastic dispersion model FLEXPART–WRF. We find that the modified model is better capable of simulating particle transport due to turbulence, and that particle size was the greatest factor in determining particle lifetime. Individual meteorology and particle density had intermediate effects upon particle transport, while release height had little effect upon simulation results. Finally, we utilize a quasi–single column model (QSCM) approach to determine how our results compare to a parameterized treatment of turbulence. The QSCM simulations led to greater tracer transport out of the boundary layer, with ramifications for any studies utilizing a Lagrangian stochastic model to understand tracer dispersion. Furthermore, these results highlight the importance of accurately simulating turbulence for understanding particle transport.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Dataset for "FLEXPART-WRF simulations to assess dust transport in the convective boundary layer at the Southern Great Plains site"

Soil dusts are an important source of aerosol in agricultural regions and can affect the Earth’s radiation budget through the modification of cloud properties, and in particular, through their ability to act as ice nucleating particles. In order to impact cloud properties, agricultural soil dusts need to be transported from the point of emission to cloud-relevant altitudes. Vertical transport within the planetary boundary layer is strongly controlled by turbulence and is challenging to represent accurately in regional and global models. Large-eddy simulations (LES) are run at resolutions capable of resolving most of the turbulent energy directly and can thus better simulate vertical transport. In this study, we leverage the LES ARM Symbiotic Simulation and Observation (LASSO) large-eddy simulations to simulate vertical transport of agricultural dust within the turbulent boundary layer using a modified version of the stochastic dispersion model FLEXPART-WRF. We find that the modified model is better capable of simulating particle transport due to turbulence, and that particle size was the greatest factor in determining particle lifetime. Individual meteorology and particle density had intermediate effects upon particle transport, while release height had little effect upon simulation results. Finally, we utilize a quasi-single column model (QSCM) approach to determine how our results compare to a parameterized treatment of turbulence. The QSCM simulations led to greater tracer transport out of the boundary layer, with ramifications for any studies utilizing a Lagrangian stochastic model to understand tracer dispersion. These results highlight the importance of accurately simulating turbulence for understanding particle transport.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Vertical Structure and Ice Production Processes of Shallow Convective Postfrontal Clouds over the Southern Ocean in MARCUS. Part II: Modeling Study

Abstract Part I of this series presented a detailed overview of postfrontal mixed-phase clouds observed during the Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS) field campaign. In Part II, we focus on a multiday (23–26 February 2018) case with the aim of understanding ice production as well as model sensitivity to ice process parameterizations using the Weather Research and Forecasting (WRF) Model. The control simulation with the Predicted Particle Properties (P3) microphysics scheme underestimates the ice content and overestimates the supercooled liquid water content, contrary to the bias common in global climate models. The simulations targeted at ice production processes show negligible sensitivity to cloud droplet number concentrations. Further, neither increasing ice nuclei particle (INP) concentrations to an unrealistic level nor adjusting it to MARCUS field estimations alone guarantees more ice production in the model. However, the simulated clouds are found to be highly sensitive to the implementation of immersion freezing, the thresholding of condensation/deposition freezing initiation, and the rime splintering process. By increasing immersion freezing of cloud droplets, relaxing thresholds for condensation/deposition freezing, or removing rime splintering thresholds, the model significantly improves its performance in producing ice. The relaxation of the immersion freezing temperature threshold to the observed cloud-top temperature suggests an in-cloud seeder–feeder mechanism. The results of this work call for an increase in observations of INP, especially over the remote Southern Ocean and at relatively high temperatures, and measurements of ice particle size distributions to better constrain ice nucleating processes in models.

Meteorology & Atmospheric Sciences↗
DOE OSTI2025

Multi-seasonal measurements of the ground-level atmospheric ice-nucleating particle abundance on the North Slope of Alaska

Atmospheric ice-nucleating particles (INPs) are an important subset of aerosol particles that are responsible for the heterogeneous formation of ice crystals. INPs modulate the arctic cloud phase (liquid vs. ice), resulting in implications for radiative feedbacks. The number of arctic INP studies investigating specific INP episodes or sources increased recently. However, existing studies are based on short-duration field data, and long-term datasets are lacking. Continuous, long-term measurements are key to determining the abundance and variability of ambient arctic INPs and constraining aerosol–cloud interactions, e.g., to verify and/or improve simulations of mixed-phase clouds. Here, we present a new long-duration INP dataset from the Arctic: 2 years of predominantly immersion-mode INP concentrations (n INP ) measured continuously at the National Oceanic and Atmospheric Administration's Barrow Atmospheric Baseline Observatory (BRW) on the North Slope of Alaska. A portable ice nucleation experiment chamber (PINE-03), which simulates adiabatic expansion cooling, was used to directly measure the ground-level INP abundance with an approximately 12 min time resolution from October 2021 to December 2023. We document PINE-03 n INP measurements as well as estimated ice nucleation active surface site density (n s ) over a wide range of heterogeneous freezing temperatures from −16 to −31 °C from which we introduce new season-specific parameterizations suitable for modeling mixed-phase clouds. Collocated aerosol and meteorological data were analyzed to assess the correlation between ambient n INP , air mass origin region, and meteorological variability. Our findings suggest (1) very high freezing efficiency of INPs across the measured temperatures (n s ≈ 2×10 8 –10 10 m −2 for −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 fall using the same instrument; (2) surprisingly high n INP (≥ 1 L −1 at −25 °C) for the examined temperatures throughout the year that were not measured by PINE-03 at other sites; and (3) high n INP in spring, possibly related to arctic haze episodes. Relatively low concentrations of aerosol surface area and contrasting high-INP concentrations at BRW relative to mid-latitude sites are the possible reasons for the observed high freezing efficiency.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Model Intercomparison of the Impacts of Varying Cloud Droplet–Nucleating Aerosols on the Life Cycle and Microphysics of Isolated Deep Convection

The microphysical impacts of aerosol particles on scattered isolated deep convective cells near Houston, Texas, on 19 June 2013, are examined using multiple cloud-resolving model (CRM) simulations initialized with vertical profiles of low and high concentrations of cloud droplet–nucleating aerosols. These simulations formed part of the Model Intercomparison Project (MIP) conducted by the Deep Convective Working Group of the Aerosol, Cloud, Precipitation and Climate (ACPC) initiative. Each CRM generated a field of convective cells representing those observed during the case study with varying degrees of accuracy. The Tracking and Object-Based Analysis of Clouds (tobac) cell-tracking algorithm was applied to each MIP CRM simulation to track relatively long-lived convective cells (20–60 min). Most of the CRMs produced similar aerosol loading impacts on the warm phase of tracked cell properties with reduced autoconversion and accretion growth of rain, increased cloud water, reduced rainfall, and reduced near-surface evaporation of rain. The sign of aerosol impacts on the warm-phase properties of the convective cells was also quite consistent over cell lifetimes with the greatest magnitude of influence in the first half of the life cycle in most CRMs. In contrast, the ice-phase response to aerosol loading was highly variable among CRMs and included increases or decreases in ice amounts at inconsistent stages of the cell life cycle and midlevel versus upper-level changes in ice. This intermodel variability in ice is indicative both of the complex indirect interactions between aerosols and ice-phase processes in deep convection and their associated parameterizations.

Aerosol-cloud interaction↗
DOE OSTI2025

Field intercomparison of ice nucleation measurements: the Fifth International Workshop on Ice Nucleation Phase 3 (FIN-03)

Abstract. The third phase of the Fifth International Ice Nucleation Workshop (FIN-03) was conducted at the Storm Peak Laboratory in Steamboat Springs, Colorado, in September 2015 to facilitate the intercomparison of instruments measuring ice-nucleating particles (INPs) in the field. Instruments included two online and four offline measurement systems for INPs, which are a subset of those utilized in the laboratory study that comprised the second phase of FIN (FIN-02). The composition of the total aerosols was characterized using the Particle Analysis by Laser Mass Spectrometry (PALMS) and Wideband Integrated Bioaerosol Sensor (WIBS) instruments, and aerosol size distributions were measured by a laser aerosol spectrometer (LAS). The dominant total particle compositions present during FIN-03 were composed of sulfates, organic compounds, and nitrates, as well as particles derived from biomass burning. Mineral-dust-containing particles were ubiquitous throughout and represented 67 % of supermicron particles. Total WIBS fluorescing particle concentrations for particles with diameters of > 0.5 µm were 0.04 ± 0.02 cm−3 (0.1 cm−3 highest; 0.02 cm−3 lowest), typical of the warm season in this region and representing ≈ 9 % of all particles in this size range as a campaign average. The primary focus of FIN-03 was the measurement of INP concentrations via immersion freezing at temperatures > −33 °C. Additionally, some measurements were made in the deposition nucleation regime at these same temperatures, representing one of the first efforts to include both mechanisms within a field campaign. INP concentrations via immersion freezing agreed within factors ranging from nearly 1 to 5 times on average between matched (time and temperature) measurements, and disagreements only rarely exceeded 1 order of magnitude for sampling times coordinated to within 3 h. Comparisons were restricted to temperatures lower than −15 °C due to the limits of detection related to sample volumes and very low INP concentrations. Outliers of up to 2 orders of magnitude occurred between −25 and −18 °C; a better agreement was seen at higher and lower temperatures. Although the 5–10 factor agreement of INP measurements found in FIN-03 aligned with the results of the FIN-02 laboratory comparison phase, giving confidence in progress of this measurement field, this level of agreement still equates to temperature uncertainties of 3.5 to 5 °C that may not be sufficient for numerical cloud modeling applications that utilize INP information. INP activity in the immersion-freezing mode was generally found to be an order of magnitude or more, making it more efficient than in the deposition regime at 95 %–99 % water relative humidity, although this limited data set should be augmented in future efforts. To contextualize the study results, an assessment was made of the composition of INPs during the late-summer to early-fall period of this study inferred through comparison to existing ice nucleation parameterizations and through measurement of the influence of thermal and organic carbon digestion treatments on immersion-freezing ice nucleation activity. Consistent with other studies in continental regions, biological INPs dominated at temperatures of > −20 °C and sometimes colder, while arable dust-like or other organic-influenced INPs were inferred to dominate below −20 °C.

54 ENVIRONMENTAL SCIENCES↗