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Hill, Thomas C. J.

Publications and source records attributed to Hill, Thomas C. J..

16 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

62°S Witnesses the Transition of Boundary Layer Marine Aerosol Pattern Over the Southern Ocean (50°S–68°S, 63°E– 150°E) During the Spring and Summer: Results From MARCUS (I)

The Atmospheric Radiation Measurement Mobile Facility-2 was installed onboard the research vessel Aurora Australis to measure aerosol properties during the 2017-2018 Measurement of Aerosols, Radiation, and CloUds over the pristine Southern ocean (MARCUS) Experiment, providing unique data on aerosols latitudinal and seasonal variation, including south of 60 degrees S where previous observations are scarce. Data from a Cloud Condensation Nuclei (CCN) counter and Ultra-High-Sensitivity Aerosol Spectrometer show that both the number concentration (N-CCN) and size distribution of CCN-active aerosols, with diameters (D) between 60 nm < D < 1,000 nm are different over the North Southern Ocean (NSO) (50 degrees S-60 degrees S) and the South Southern Ocean (SSO) (62 degrees S-68 degrees S). The average NSO N-CCN at 0.2% and 0.5% supersaturation were 28% and 49% less than that over the SSO. This increase of CCN over the SSO is caused by the increase of aerosols with 60 nm < D < 200 nm, consistent with calculations of Aerosol Scattering Angstrom Exponents derived from a nephelometer. Aerosol hygroscopicity growth factor measured by the Hygroscopic Tandem Differential Mobility Analyzer stayed close to 1.41 for aerosols with 50 nm < D < 250 nm over the SSO, but increased from 1.30 to 1.67 over the NSO, indicating different chemical compositions. Both CCN and Ice Nucleating Particles (INPs) showed a stronger variation with season than with latitude. The variation of heat-labile and presumably proteinacous INPs suggests an increase of ice nucleating-active microbes in summer.

Niu, Qing↗
DOE OSTI2024

Ice Nucleation Spectrometer (INS) Instrument Handbook

The Ice Nucleation Spectrometer (INS) is an offline analytical measurement system used to process filter samples for freezing temperature spectra of immersion-mode ice nucleating particle (INP) number concentrations. It is almost identical to the CSU Ice Spectrometer (IS) design. While basic immersion freezing methods have been applied for decades, recent intercomparison studies (DeMott et al. 2017, 2018b) with other methods for sampling ambient INPs support the method’s utility. Use of the INS with filters produces spectra spanning wide dynamic ranges of temperature and, hence, INP concentration (e.g., six orders of magnitude). The INS is supported with well-established experimental protocols and has been applied in many diverse scenarios.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Characterizing Ice Nucleating Particles Over the Southern Ocean Using Simultaneous Aircraft and Ship Observations

Abstract Supercooled liquid clouds are ubiquitous over the Southern Ocean (SO), even to temperatures below −20°C, and comprise a large fraction of the marine boundary layer (MBL) clouds. Earth system models and reanalysis products have struggled to reproduce the observed cloud phase distribution and occurrence of cloud ice in the region. Recent simulations found the microphysical representation of ice nucleation and growth has a large impact on these properties, however, measurements of SO ice nucleating particles (INPs) to validate simulations are sparse. This study presents measurements of INPs from simultaneous aircraft and ship campaigns conducted over the SO in austral summer 2018, which include the first in situ observations in and above cloud in the region. Our results confirm recent observations that INP concentrations are uniformly lower than measurements made in the late 1960s. While INP concentrations below and above cloud are similar, higher ice nucleation efficiency above cloud supports model simulations that the dominant INP composition varies with height. Model parameterizations based solely on aerosol properties capture the mean relationship between INP concentration and temperature but not the observed variability, which is likely related to the only modest correlations observed between INPs and environmental or aerosol metrics. Including wind speed in addition to activation temperature in a marine INP parameterization reduces bias but does not explain the large range of observed INP concentrations. Direct and indirect inference of marine INP size suggests MBL INPs, at least during Austral summer, are dominated by particles with diameters smaller than 500 nm.

Meteorology & Atmospheric Sciences↗
DOE OSTI2023

Bioaerosols are the dominant source of warm-temperature immersion-mode INPs and drive uncertainties in INP predictability

Ice-nucleating particles (INPs) are rare atmospheric aerosols that initiate primary ice formation, but accurately simulating their concentrations and variability in large-scale climate models remains a challenge. Doing so requires both simulating major particle sources and parameterizing their ice nucleation (IN) efficiency. Validating and improving model predictions of INP concentrations requires measuring their concentrations delineated by particle type. We present a method to speciate INP concentrations into contributions from dust, sea spray aerosol (SSA), and bioaerosol. Field campaign data from Bodega Bay, California, showed that bioaerosols were the primary source of INPs between –12° and –20°C, while dust was a minor source and SSA had little impact. We found that recent parameterizations for dust and SSA accurately predicted ambient INP concentrations. However, the model did not skillfully simulate bioaerosol INPs, suggesting a need for further research to identify major factors controlling their emissions and INP efficiency for improved representation in models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Simulating Southern Ocean Aerosol and Ice Nucleating Particles in the Community Earth System Model Version 2

Southern Ocean (SO) low-level mixed phase clouds have been a long-standing challenge for Earth system models to accurately represent. While improvements to the Community Earth System Model version 2 (CESM2) resulted in increased supercooled liquid in SO clouds and improved model radiative biases, simulated SO clouds in CESM2 now contain too little ice. Previous observational studies have indicated that marine particles are major contributor to SO low-level cloud heterogeneous ice nucleation, a process that initiates a number of cloud processes that govern cloud radiative properties. In this study, we utilize detailed aerosol and ice nucleating particle (INP) measurements from two recent measurement campaigns to assess simulated aerosol abundance, number size distributions, and composition and INP parameterizations for use in CESM2. Our results indicate that CESM2 has a positive bias in simulated surface-level total aerosol surface area at latitudes north of 58°S. Measured INP populations were dominated by marine INPs and we present evidence of refractory INPs present over the SO assumed here to be mineral dust INPs. Results highlight a critical need to assess simulated mineral dust number and size distributions in CESM2 in order to adequately represent SO INP populations and their response to long-term changes in atmospheric transport patterns and land use change. Furthermore, we also discuss important cautions and limitations in applying a commonly used mineral dust INP parameterization to remote regions like the pristine SO.

58 GEOSCIENCES↗
DOE OSTI2022

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

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

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Ice Nucleating Particle Connections to Regional Argentinian Land Surface Emissions and Weather During the Cloud, Aerosol, and Complex Terrain Interactions Experiment

Abstract Here, we present a multi‐season study of ice‐nucleating particles (INPs) active via the immersion freezing mechanism, which took place in north‐central Argentina, a worldwide hotspot for mesoscale convective storms. INPs were measured untreated, after heating to 95°C, and after hydrogen peroxide digestion. No seasonal cycle of INP concentrations was observed. Heat labile INPs, which we define as “biological” herein, dominated the population active at −5 to −20°C, while non‐heat‐labile organic INPs (decomposed by peroxide) dominated at lower temperatures, from −20 to −28°C. Inorganic INPs (remaining after peroxide digestion), were minor contributors to the overall INP activity. Biological INP concentration active around −12°C peaked during rain events and under high relative humidity, reflecting emission mechanisms independent of the background aerosol concentration. The ratio of non‐heat‐labile organic and inorganic INPs was generally constant, suggesting they originated from the same source, presumably from regional arable topsoil based on air mass histories. Single particle mass spectrometry showed that soil particles aerosolized from a regionally common agricultural topsoil contained known mineral INP sources (K‐feldspar and illite) as well as a significant organic component. The INP activity observed in this study correlates well with agricultural soil INP activities from this and other regions of the world, suggesting that the observed INP spectra might be typical of many arable landscapes. These results demonstrate the strong influence of regional continental landscapes, emitting INPs of types that are not yet well represented in global models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

COMBLE ARM Mobile Facility (AMF) Measurements of Ice Nucleating Particles Field Campaign Report

During the Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE), a project with the overarching goal to shed light on the dynamics and microphysical properties of clouds and precipitation in the high-latitude marine boundary layer during cold-air outbreaks (CAOs), we were tasked with providing and assisting the collection of aerosol filter samples for measuring ice nucleating particle (INP) concentrations. Little is known about the properties of CAO cloud systems, how they vary with surface, environmental, and aerosol conditions, the role of cold-air outbreaks in the global atmospheric and ocean circulation, and the accuracy of the treatment of this atmospheric regime in climate models. Uncertainties in climate projections for the arctic and sub-arctic region are large, in part due to the lack of observational guidance to constrain the treatment of aerosol-cloud-precipitation linkages in climate models.

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↗