Abstract The formation of ice in clouds can strongly impact cloud properties and precipitation processes during storms, including atmospheric rivers. Sea spray aerosol (SSA) particles are relatively inefficient as ice nucleating particles (INPs) compared to mineral dust. However, due to the vast coverage of the Earth's surface by the oceans, a number of recent studies have focused on identifying sources of marine INPs, particularly in regions lacking a strong influence from dust. This study describes the integration, validation, and application of a system coupling a continuous flow diffusion chamber with a single particle mass spectrometer using a pumped counterflow virtual impactor to remove nonnucleated particles and selectively measure the composition of INPs with a detection efficiency of 3.10×10−4. In situ measurements of immersion freezing INP composition were made at a coastal site in California using the integrated system. Mineral dust particles were the most abundant ice crystal residual type during the sampling period and found to be ice active despite having undergone atmospheric processing. SSA were more abundant in ambient measurements but represented only a minor fraction of the ice crystal residual population at −31 °C. Notably, the SSA particles that activated were enriched with organic nitrogen species that were likely transferred from the ocean. Calculations of ice nucleation active site densities were within good agreement with previous studies of mineral dust and SSA.
more »
« less
The Abundance and Sources of Ice Nucleating Particles Within Alaskan Ice Fog
Abstract The Alaskan Layered Pollution and Chemical Analysis (ALPACA) field campaign included deployment of a suite of atmospheric measurements in January–February 2022 with the goal of better understanding atmospheric processes and pollution under cold and dark conditions in Fairbanks, Alaska. We report on measurements of particle composition, particle size, ice nucleating particle (INP) composition, and INP size during an ice fog period (29 January–3 February). During this period, coarse particulate matter (PM10) concentrations increased by 150% in association with a decrease in air temperature, a stronger temperature inversion, and relatively stagnant conditions. Results also show a 18%–78% decrease in INPs during the ice fog period, indicating that particles had activated into the ice fog via nucleation. Peroxide and heat treatments performed on INPs indicated that, on average, the largest contributions to the INP population were heat‐labile (potentially biological, 63%), organic (31%), then inorganic (likely dust, 6%). Measurements of levoglucosan and bulk and single‐particle composition corroborate the presence of dust and aerosols from combustion sources. Heat‐labile and organic INPs decreased during the peak period of the ice fog, indicating those were preferentially activated, while inorganic INPs increased, suggesting they remained as interstitial INPs. In general, INP concentrations were unexpectedly high in Fairbanks compared to other locations in the Arctic during winter. The fact that these INPs likely facilitated ice fog formation in Fairbanks has implications for other high latitude locations subject to the hazards associated with ice fog.
more »
« less
- PAR ID:
- 10535522
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Publisher / Repository:
- DOI PREFIX: 10.1029
- Date Published:
- Journal Name:
- Journal of Geophysical Research: Atmospheres
- Volume:
- 129
- Issue:
- 16
- ISSN:
- 2169-897X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
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
-
Abstract. Ice-nucleating particles (INPs) initiate primary ice formation in Arctic mixed-phase clouds (MPCs), altering cloud radiative properties and modulating precipitation. For atmospheric INPs, the complexity of their spatiotemporal variations, heterogeneous sources, and evolution via intricate atmospheric interactions challenge the understanding of their impact on microphysical processes in Arctic MPCs and induce an uncertain representation in climate models. In this work, we performed a comprehensive analysis of atmospheric aerosols at the Arctic coastal site in Ny-Ålesund (Svalbard, Norway) from October to November 2019, including their ice nucleation ability, physicochemical properties, and potential sources. Overall, INP concentrations (NINP) during the observation season were approximately up to 3 orders of magnitude lower compared to the global average, with several samples showing degradation of NINP after heat treatment, implying the presence of proteinaceous INPs. Particle fluorescence was substantially associated with INP concentrations at warmer ice nucleation temperatures, indicating that in the far-reaching Arctic, aerosols of biogenic origin throughout the snow- and ice-free season may serve as important INP sources. In addition, case studies revealed the links between elevated NINP and heat lability, fluorescence, high wind speeds originating from the ocean, augmented concentration of coarse-mode particles, and abundant organics. Backward trajectory analysis demonstrated a potential connection between high-latitude dust sources and high INP concentrations, while prolonged air mass history over the ice pack was identified for most scant INP cases. The combination of the above analyses demonstrates that the abundance, physicochemical properties, and potential sources of INPs in the Arctic are highly variable despite its remote location.more » « less
-
Abstract. Rapid Arctic climate warming, amplified relative to lower-latitude regions, has led to permafrost thaw and associated thermokarst processes. Recent work has shown permafrost is a rich source of ice-nucleating particles (INPs) that can initiate ice formation in supercooled liquid clouds. Since the phase of Arctic clouds strongly affects the surface energy budget, especially over ice-laden surfaces, characterizing INP sources in this region is critical. For the first time, we provide a large-scale survey of potential INP sources in tundra terrain where thermokarst processes are active and relate to INPs in the air. Permafrost, seasonally thawed active layer, ice wedge, vegetation, water, and aerosol samples were collected near Utqiaġvik, Alaska, in late summer and analyzed for their INP contents. Permafrost was confirmed as a rich source of INPs that was enhanced near the coast. Sensitivity to heating revealed differences in INPs from similar sources, such as the permafrost and active layer. Water, vegetation, and ice wedge INPs had the highest heat-labile percentage. The aerosol likely contained a mixture of known and unsurveyed INP types that were inferred as biological. Arctic water bodies were shown to be potential important links of sources to the atmosphere in thermokarst regions. Therefore, a positive relationship found with total organic carbon considering all water bodies gives a mechanism for future parameterization as permafrost continues to thaw and drive regional landscape shifts.more » « less
-
null (Ed.)Abstract. Ice-nucleating particles (INPs) are efficiently removed fromclouds through precipitation, a convenience of nature for the study of thesevery rare particles that influence multiple climate-relevant cloudproperties including ice crystal concentrations, size distributions andphase-partitioning processes. INPs suspended in precipitation can be used toestimate in-cloud INP concentrations and to infer their originalcomposition. Offline droplet assays are commonly used to measure INPconcentrations in precipitation samples. Heat and filtration treatmentsare also used to probe INP composition and size ranges. Many previousstudies report storing samples prior to INP analyses, but little is knownabout the effects of storage on INP concentration or their sensitivity totreatments. Here, through a study of 15 precipitation samples collected at acoastal location in La Jolla, CA, USA, we found INP concentration changes upto > 1 order of magnitude caused by storage to concentrations ofINPs with warm to moderate freezing temperatures (−7 to−19 ∘C). We compared four conditions: (1) storage at roomtemperature (+21–23 ∘C), (2) storage at +4 ∘C, (3) storage at −20 ∘C and (4) flash-freezing samples with liquid nitrogen prior to storage at −20 ∘C. Results demonstrate that storage can lead to bothenhancements and losses of greater than 1 order of magnitude, withnon-heat-labile INPs being generally less sensitive to storage regime, butsignificant losses of INPs smaller than 0.45 µm in all tested storageprotocols. Correlations between total storage time (1–166 d) and changesin INP concentrations were weak across sampling protocols, with theexception of INPs with freezing temperatures ≥ −9 ∘C in samples stored at room temperature. We provide thefollowing recommendations for preservation of precipitation samples fromcoastal or marine environments intended for INP analysis: that samples bestored at −20 ∘C to minimize storage artifacts, thatchanges due to storage are likely an additional uncertainty in INPconcentrations, and that filtration treatments be applied only to freshsamples. At the freezing temperature −11 ∘C, average INPconcentration losses of 51 %, 74 %, 16 % and 41 % were observed foruntreated samples stored using the room temperature, +4, −20 ∘C, and flash-frozen protocols, respectively.Finally, the estimated uncertainties associated with the four storage protocolsare provided for untreated, heat-treated and filtered samples for INPsbetween −9 and −17 ∘C.more » « less
An official website of the United States government
