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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.
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A numerical framework for simulating the atmospheric variability of supermicron marine biogenic ice nucleating particles
Abstract. We present a framework for estimating concentrations of episodicallyelevated high-temperature marine ice nucleating particles (INPs) in the seasurface microlayer and their subsequent emission into the atmosphericboundary layer. These episodic INPs have been observed in multipleship-based and coastal field campaigns, but the processes controlling theirocean concentrations and transfer to the atmosphere are not yet fullyunderstood. We use a combination of empirical constraints and simulationoutputs from an Earth system model to explore different hypotheses forexplaining the variability of INP concentrations, and the occurrence ofepisodic INPs, in the marine atmosphere. In our calculations, we examine the following two proposed oceanic sources of high-temperature INPs: heterotrophic bacteria and marine biopolymer aggregates (MBPAs). Furthermore, we assume that the emission of these INPs is determined by the production of supermicron sea spray aerosol formed from jet drops, with an entrainment probability that is described by Poisson statistics. The concentration of jet drops is derived from the number concentration of supermicron sea spray aerosol calculated from model runs. We then derive the resulting number concentrations of marine high-temperature INPs (at 253 K) in the atmospheric boundary layer and compare their variability to atmospheric observations of INP variability. Specifically, we compare against concentrations of episodically occurring high-temperature INPs observed during field campaigns in the Southern Ocean, the Equatorial Pacific, and the North Atlantic. In this case study, we evaluate our framework at 253 K because reliable observational data at this temperature are available across three different ocean regions, but suitable data are sparse at higher temperatures. We find that heterotrophic bacteria and MBPAs acting as INPs provide only apartial explanation for the observed high INP concentrations. We note,however, that there are still substantial knowledge gaps, particularlyconcerning the identity of the oceanic INPs contributing most frequently toepisodic high-temperature INPs, their specific ice nucleation activity, andthe enrichment of their concentrations during the sea–air transfer process. Therefore, targeted measurements investigating the composition of these marine INPs and drivers for their emissions are needed, ideally incombination with modeling studies focused on the potential cloud impacts ofthese high-temperature INPs.
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- Award ID(s):
- 1801971
- PAR ID:
- 10329713
- Date Published:
- Journal Name:
- Atmospheric Chemistry and Physics
- Volume:
- 22
- Issue:
- 2
- ISSN:
- 1680-7324
- Page Range / eLocation ID:
- 847 to 859
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Oceans are, generally, relatively weak sources of ice nucleating particles (INPs). Thus, dust transported from terrestrial regions can dominate atmospheric INP concentrations even in remote marine regions. Studies of ocean‐emitted INPs have focused upon sea spray aerosols containing biogenic species. Even though large concentrations of dust are transported over marine regions, resuspended dust has never been explicitly considered as another possible source of ocean‐emitted INPs. Current models assume that deposited dust is not re‐emitted from surface waters. Our laboratory studies of aerosol particles produced from coastal seawater and synthetic seawater doped with dust show that dust can indeed be ejected from water during bubble bursting. INP concentration measurements show these ejected dust particles retain ice nucleating activity. Doping synthetic seawater to simulate a strong dust deposition event produced INPs active at temperatures colder than −13°C and INP concentrations 1 to 2 orders of magnitude greater than either lab sea spray or marine boundary layer measurements. The relevance of these laboratory findings is highlighted by single‐particle composition measurements along the Californian coast where at least 9% of dust particles were mixed with sea salt. Additionally, global modeling studies show that resuspension of dust from the ocean could exert the most impact over the Southern Ocean, where ocean‐emitted INPs are thought to dominate atmospheric INP populations. More work characterizing the factors governing the resuspension of dust particles is required to understand the potential impact upon clouds.more » « less
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Abstract Ice‐nucleating particles (INPs) play a key role in ice formation and cloud microphysics and thus significantly impact the water cycle and the climate. However, our understanding of atmospheric INPs, particularly their sources, emissions, and spatiotemporal variability, is incomplete. While the enhancement of atmospheric INP concentrations with rainfall has been previously shown, a mechanistic understanding of the process is lacking. Here, we link detailed precipitation observations with near‐surface atmospheric INP concentrations at a semiarid grassland site in Colorado. Considering the during‐precipitation air samples, INP concentrations positively correlate with cumulative rainfall kinetic energy and amount, suggesting that INP aerosolization is induced by raindrop and hailstone impact. By additionally analyzing the INP content of precipitation water, terrestrial source samples, and heat‐treated samples, we demonstrate that local plants are the most plausible source of rain‐induced INPs during a precipitation event. Should INPs aerosolized by precipitation rise to cloud height, they could influence cloud ice fraction and initiate precipitation resulting in an aerosol‐cloud‐precipitation feedback.more » « less
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.5194/acp-22-847-2022
