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Ice-nucleating particles (INPs) are crucial for cloud freezing processes in the atmosphere. Given the limited knowledge about the vertical distribution of INPs and its relation to aerosols in China, we present two aircraft observations of INPs over the North China Plain on 23 October 2019 and 25 October 2019, before and after a cold front passage. We used a well-established method to identify the INPs on a silicon wafer and then performed single-particle chemical composition analysis using an environmental scanning electron microscope-energy dispersive spectrometer (ESEM-EDS). The INP concentrations range from 0.1 to 9.2 L−1 within activation temperatures from −20 to −29 °C. INPs are mostly concentrated within the boundary layer, and their concentration shows a decreasing trend with height (0.5~6 km) before the cold front passage. However, the highest INP concentration always appears at higher altitudes (4~5 km) after the cold front passage. The cold front passage also significantly weakens the correlations between the concentrations of INPs and aerosol particles at different sizes. The activated fraction (AF) of total aerosols increases from 10−6 to 10−4 with height from near ground to 6 km, reflecting a better nucleating capacity of the aerosols at higher altitudes. There is no obvious variation in AF after the cold front passage. Chemical analysis reveals that the INPs containing mineral dust components comprise the majority of total INPs during both flights. The proportion of pure mineral dust declines from 52.2% to 43.5% after the cold front passage while the proportion of mixed mineral dust increases from 23.9% to 45.7%, suggesting that an increased probability of aging or coating of INPs is introduced by the cold front during their long-distance transport. In addition, 88% of INPs have a diameter larger than 1 μm. This indicates that larger aerosols (>1 μm) are the major contributors to INPs at high altitudes despite their relatively low abundance. Our results demonstrate a significant impact of transport events on the sources and vertical distribution of INPs in the atmosphere. [ABSTRACT FROM AUTHOR]

Ice-nucleating particles (INPs) are crucial for cloud freezing processes in the atmosphere. Given the limited knowledge about the vertical distribution of INPs and its relation to aerosols in China, we present two aircraft observations of INPs over the North China Plain on 23 October 2019 and 25 October 2019, before and after a cold front passage. We used a well-established method to identify the INPs on a silicon wafer and then performed single-particle chemical composition analysis using an environmental scanning electron microscope-energy dispersive spectrometer (ESEM-EDS). The INP concentrations range from 0.1 to 9.2 L−1 within activation temperatures from −20 to −29 °C. INPs are mostly concentrated within the boundary layer, and their concentration shows a decreasing trend with height (0.5~6 km) before the cold front passage. However, the highest INP concentration always appears at higher altitudes (4~5 km) after the cold front passage. The cold front passage also significantly weakens the correlations between the concentrations of INPs and aerosol particles at different sizes. The activated fraction (AF) of total aerosols increases from 10−6 to 10−4 with height from near ground to 6 km, reflecting a better nucleating capacity of the aerosols at higher altitudes. There is no obvious variation in AF after the cold front passage. Chemical analysis reveals that the INPs containing mineral dust components comprise the majority of total INPs during both flights. The proportion of pure mineral dust declines from 52.2% to 43.5% after the cold front passage while the proportion of mixed mineral dust increases from 23.9% to 45.7%, suggesting that an increased probability of aging or coating of INPs is introduced by the cold front during their long-distance transport. In addition, 88% of INPs have a diameter larger than 1 μm. This indicates that larger aerosols (>1 μm) are the major contributors to INPs at high altitudes despite their relatively low abundance. Our results demonstrate a significant impact of transport events on the sources and vertical distribution of INPs in the atmosphere.

We examined ice-nucleating particles (INPs) in the plumes of the Tocantins and Amazon rivers, which drain watersheds with different proportions of degraded land. The concentration of INPs active at −15°C (INP−15) was an order of magnitude lower in the Tocantins (mean = 13.2 ml−1; s.d. = 7.8 ml−1), draining the more degraded watershed, compared with the Amazon (mean = 175.8 ml−1; s.d. = 11.2 ml−1), where the concentration was also significantly higher than in Atlantic surface waters (mean = 3.2 ml−1; s.d. = 2.3 ml−1). Differences in heat tolerance suggest that INPs emitted by the Amazon rainforest to the atmosphere or washed into the river might originate from contrasting sources on top of and below the rainforest canopy, respectively. For the Amazon River, we estimate a daily discharge of 1018 INP−15 to Atlantic waters. Rivers in cooler climate zones tend to have much higher concentrations of INPs and could, despite a smaller water volume discharged, transfer even larger absolute numbers of INP−15 to shelf waters than does the Amazon. To what extent these terrestrial INPs become aerosolized by breaking waves and bubble-bursting remains an open question.

Mixed‐phase clouds (MPCs), which consist of both supercooled cloud droplets and ice crystals, play an important role in the Earth's radiative energy budget and hydrological cycle. In particular, the fraction of ice crystals in MPCs determines their radiative effects, precipitation formation and lifetime. In order for ice crystals to form in MPCs, ice‐nucleating particles (INPs) are required. However, a large‐scale relationship between INPs and ice initiation in clouds has yet to be observed. By analyzing satellite observations of the typical transition temperature (T*) where MPCs become more frequent than liquid clouds, we constrain the importance of INPs in MPC formation. We find that over the Arctic and Southern Ocean, snow and sea ice cover significantly reduces T*. This indicates that the availability of INPs is essential in controlling cloud phase evolution and that local sources of INPs in the high‐latitudes play a key role in the formation of MPCs. Plain Language Summary: Mixed‐phase clouds (MPCs), which consist of both liquid droplets and ice crystals, play an important role for the Earth's climate system. For example, the number of ice crystals in MPCs determines how much sunlight is reflected by the cloud and how efficiently the cloud can form precipitation. The formation of ice crystals in MPCs requires a special subset of aerosol particles called ice‐nucleating particles (INPs). INPs are required for liquid cloud droplets to freeze at temperatures warmer than −36°C. However, a large‐scale relationship between INPs and ice formation in clouds has yet to be observed. Using satellite observations, we determine the transition temperature (T*) where MPCs become more frequent than liquid clouds and find that T* is strongly dependent on snow and sea ice cover over the Arctic and Southern Ocean. This indicates that sea ice and snow cover act as a lid that inhibits the emission of INPs from the ocean. In a warming world with retreating sea ice and snow cover, our results suggest that clouds in these regions will contain ice crystals at warmer temperatures than previously estimated and, thus, have potential implications for future warming predictions. Key Points: Ice‐nucleating particles (INPs) control ice formation in high‐latitude cloudsSea ice and snow cover inhibit the local emission of INPs, which directly influences cloud phase in the Arctic and Southern OceanThis has implications for the predicted negative cloud phase feedback with future warming and the associated sea ice and snow cover loss [ABSTRACT FROM AUTHOR]

The amount of ice versus supercooled water in clouds is important for their radiative properties and role in climate feedbacks. Hence, knowledge of the concentration of ice‐nucleating particles (INPs) is needed. Generally, the concentrations of INPs are found to be very low in remote marine locations allowing cloud water to persist in a supercooled state. We had expected the concentrations of INPs at the North Pole to be very low given the distance from open ocean and terrestrial sources coupled with effective wet scavenging processes. Here we show that during summer 2018 (August and September) high concentrations of biological INPs (active at >−20°C) were sporadically present at the North Pole. In fact, INP concentrations were sometimes as high as those recorded at mid‐latitude locations strongly impacted by highly active biological INPs, in strong contrast to the Southern Ocean. Furthermore, using a balloon borne sampler we demonstrated that INP concentrations were often different at the surface versus higher in the boundary layer where clouds form. Back trajectory analysis suggests strong sources of INPs near the Russian coast, possibly associated with wind‐driven sea spray production, whereas the pack ice, open leads, and the marginal ice zone were not sources of highly active INPs. These findings suggest that primary ice production, and therefore Arctic climate, is sensitive to transport from locations such as the Russian coast that are already experiencing marked climate change. Plain Language Summary: Clouds play a critical role in Earth's climate, both reflecting incoming sunlight and trapping outgoing infrared radiation. Hence, even small errors in the representation of clouds in climate models can lead to uncertainty in predictions of, for example, sea ice extent. In the Arctic, liquid clouds often exist below 0°C and cloud water droplets can exist in a supercooled liquid state. In the absence of special particles that can trigger ice formation in droplets, ice‐nucleating particles (INPs), supercooled water droplets can cool well below −35°C before spontaneously freezing. The presence of INPs can reduce the lifetime of a cloud and the amount of supercooled water in clouds, making them less reflective. Based on our knowledge of INPs in other remote oceans, we expected very low INP concentrations in the central Arctic. However, we found very high concentrations of biological INPs in the summertime North Pole. Furthermore, these INPs come from the seas off the coast of Russia, a region already experiencing strong climate change. It is possible that these sources may become even more important as the Arctic becomes increasingly ice‐free, causing changes in Arctic clouds and further changes in climate. Key Points: The concentration of ice‐nucleating particles at the North Pole in summer 2018 was amongst the highest anywhere in the worldBiological ice‐nucleating particles were derived from the Russian seas and perhaps associated with wind‐driven sea sprayThe concentration of ice‐nucleating particles at the surface was often different to that higher in the boundary layer where clouds form [ABSTRACT FROM AUTHOR]

Arctic amplification (AA) is simulated by all global climate models, however the spread in the degree of projected warming is large and the underlying mechanisms driving it are poorly understood. The impact of the temperature dependence of immersion freezing on cloud feedbacks and AA is studied using NASA's GEOS‐5 model. Parameterizations that exhibit low ice‐nucleating particle (INP) concentrations in the high Arctic during summer are found to weaken the cloud‐phase feedback. This allows sunlight to readily melt sea‐ice in the summer, which decreases the stability of the lower troposphere, causing a decrease in wintertime cloud fraction over open ocean. Arctic amplification was found to span from ∼1.4 to >2.6, which spans 30% of the spread in AA in the coupled model intercomparison project models, depending on the temperature dependence of immersion freezing. These results suggest that summertime INP concentrations may provide an observational constraint on AA. Plain Language Summary: The Arctic is warming at more than twice the pace as the rest of the globe. Global climate models also exhibit the largest spread in surface warming in the Arctic region, where low‐level stratiform clouds are poorly represented. These clouds frequently consist of mixtures of liquid droplets and ice crystals, the latter which form with the aid of ice‐nucleating particles (INPs). Here, we show that the sensitivity of the activation of INPs in stratiform clouds to temperature results in a difference in Arctic amplification (AA) that spans over 30% of the spread in the latest generation of global climate models. The apparent warming mechanism is triggered by the extent of thermodynamic phase changes in Arctic mixed‐phase clouds during the summer and their subsequent influence of sea‐ice melt. Accurate measurements of collocated in‐cloud INP concentrations and temperature are critical for improved constraints on AA. Key Points: Ice‐nucleating particles (INPs) may trigger summertime cloud‐phase feedback interactions with sea ice that strongly impact Arctic amplification (AA)AA is highly sensitive to temperature‐dependent ice nucleation schemesSummertime measurements of (INPs) are lacking but important for constraining Arctic cloud feedbacks [ABSTRACT FROM AUTHOR]

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. Key Points: The most abundant immersion freezing ice nucleating particle type (T = −30 °C) was mineral dust during a week‐long study at a coastal siteNitrate content made little difference to the ice nucleation activity of dustSea spray aerosol that formed ice crystals were enriched in organic nitrogen species [ABSTRACT FROM AUTHOR]

The abundance and sources of ice‐nucleating particles, particles required for heterogeneous ice nucleation, are long‐standing sources of uncertainty in quantifying aerosol‐cloud interactions. In this study, we demonstrate near closure between immersion freezing ice‐nucleating particle number concentration (nINPs) observations and nINPs calculated from simulated sea spray aerosol and dust. The Community Atmospheric Model with constrained meteorology was used to simulate aerosol concentrations at the Mace Head Research Station (North Atlantic) and over the Southern Ocean to the south of Tasmania (Clouds, Aerosols, Precipitation, Radiation, and atmospherIc Composition Over the southeRN ocean campaign). Model‐predicted nINPs were within a factor of 10 of nINPs observed with an off‐line ice spectrometer at Mace Head Research Station and Clouds, Aerosols, Precipitation, Radiation, and atmospherIc Composition Over the southeRN ocean campaign, for 93% and 69% of observations, respectively. Simulated vertical profiles of nINPs reveal that transported dust may be critical to nINPs in remote regions and that sea spray aerosol may be the dominate contributor to primary ice nucleation in Southern Ocean low‐level mixed‐phase clouds. Plain Language Summary: The clouds over remote oceans are often comprised of supercooled liquid droplets, but global models struggle to represent the complex processes that control ice formation in these clouds. One poorly understood, but critical, aspect controlling the liquid‐ice partitioning in these clouds is the abundance of particles that catalyze ice crystal formation, or ice‐nucleating particles (INPs). Observations show that INPs are extremely rare in remote marine environments and are dominated by an oceanic source. However, current global models do not account for these uniquely low INP concentrations and their marine source. We used observations of INPs from two previous field campaigns to evaluate INP concentrations estimated from a global climate model that incorporates particles from sea salt, marine organic matter, and mineral dust. Our results constitute an early evaluation of the potential of present‐day global atmospheric models to successfully predict INP concentrations in the lowest atmospheric level that feeds clouds over the ocean. Extrapolating our approach to higher altitudes, the model suggests mineral/soil dust particles from long‐range transport may also be a critical INP source for marine clouds. Key Points: Observed marine boundary layer ice‐nucleating particle concentrations were successfully predicted using marine and dust parameterizationsSea spray aerosol was the dominant source of simulated ice‐nucleating particle populations up to 3–5 km over the Southern OceanMineral dust aerosol was a critical component of model‐predicted ice‐nucleating particle populations present above 5 km [ABSTRACT FROM AUTHOR]

Secondary ice production via rime-splintering is considered to be an important process for rapid glaciation and high ice crystal numbers observed in mixed-phase convective clouds. An open question is how rime-splintering is triggered in the relatively short time between cloud formation and observations of high ice crystal numbers. We use idealised simulations of a deep convective cloud system to investigate the thermodynamic and cloud microphysical evolution of air parcels, in which the model predicts secondary ice formation. The Lagrangian analysis suggests that the “in-situ” formation of rimers either by growth of primary ice or rain freezing does not play a major role in triggering secondary ice formation. Instead, rimers are predominantly imported into air parcels through sedimentation form higher altitudes. While ice nucleating particles (INPs) initiating heterogeneous freezing of cloud droplets at temperatures warmer than −10 °C have no discernible impact of the occurrence of secondary ice formation, in a scenario with rain freezing secondary ice production is initiated slightly earlier in the cloud evolution and at slightly different places, although with no major impact on the abundance or spatial distribution of secondary ice in the cloud as a whole. These results suggest that for interpreting and analysing observational data and model experiments regarding cloud glaciation and ice formation it is vital to consider the complex vertical coupling of cloud microphysical processes in deep convective clouds via three-dimensional transport and sedimentation.

A series of measurements of ice-nucleating particles (INPs) were performed at two sites in Beijing. At the Beijing Meteorological Service (BMS) site, which was an urban site, no INPs were found to be active above-15°C. However, at the Yanjiaping (YJP) site, which was a rural site, the concentration of INPs active at temperatures above-15°C was found to be as high as 1.73 g-1. Two parameterizations were constructed by respectively fitting the data obtained at BMS site and YJP site. The two parameterizations, as well as another parameterization from the literature, were implemented into a parcel model to investigate the effect of INPs active above-15°C on phase partitioning in mixed-phase clouds. At a vertical velocity of 0.01 m s-1, which is typical for stratiform clouds associated with frontal systems, the INPs active above-15°C nucleate ice crystals at low levels. The growth of these ice crystals remarkably reduces both the maximum liquid water mixing ratio and the altitude where the maximum liquid water mixing ratio is reached. When the vertical velocity of the parcel is increased to 0.1 m s-1 or an even higher value, the evolution of liquid water mixing ratio is not controlled by the INPs active above-15°C but those active below-15°C. [ABSTRACT FROM AUTHOR]

Abstract: Sea spray aerosol (SSA) generated by bubble bursting at the ocean surface is an important component of aerosol‐cloud interactions over remote oceans, providing the atmosphere with ice‐nucleating particles (INPs) or particles required for heterogeneous ice nucleation. Studies have shown that organic INPs are emitted during phytoplankton blooms, but changes in INP number concentrations (nINPs) due to ocean biological activity have not been directly demonstrated in natural SSA. In this study, a clean sector sampler was used to differentiate ice nucleation and composition of pristine SSA from terrestrial aerosol at the Mace Head Research Station in August 2015. Average nINPs active at −15 °C (nINPs,−15 °C) were 0.0011 L−1, and large variability (up to a factor of 200) was observed for INPs active warmer than −22 °C. Highest nINPs in the clean sector occurred during a period of elevated marine organic aerosol from offshore biological activity (M1, nINPs,−15 °C = 0.0077 L−1). A peak in nINPs was also observed in terrestrial organic aerosol (T1, nINPs,−15 °C = 0.0076 L−1). The impacts of heating and hydrogen peroxide digestion on nINPs indicate that INPs at Mace Head Research Station were largely organic and that INPs observed during M1 and T1 were biological (i.e., protein containing). Complexities of predicting increases in nINPs due to offshore biological activity are explored. A parameterization for pristine SSA INPs over the North Atlantic Ocean was developed, illustrating that SSA is associated with a factor of 1,000 fewer ice‐nucleating sites per surface area of aerosol compared to mineral dust. [ABSTRACT FROM AUTHOR]

Heterogeneous ice nucleation in the atmosphere is not fully understood. In particular, our knowledge of biological materials and their atmospheric ice nucleation properties remains scarce. Here, we present the results from systematic investigations of the ice nucleation activity of plant materials using cryo-microscopy. We examined berry juices, frozen berries, as well as extracts of leaves and dried berries of plants native to boreal regions. All of our samples possess reasonable ice nucleation activity. Their ice nucleating particle concentrations per unit of water volume vary between 9.7 × 105 and 9.2 × 109 cm−3 when examined within temperatures of −12 to −34 °C. Mean freezing temperatures ranged from −18.5 to −45.6 °C. We show that all samples contained ice nuclei in a size range below 0.2 µm and remain active if separated from coarse plant tissue. The results of examining ice nucleation properties of leaves and dry berry extracts suggests that their ice-nucleating components can be easily suspended in water. Sea buckthorn and black currant were analyzed using subtilisin (a protease) and urea. Results suggest proteinaceous compounds to play an important role in their ice nucleation activity. These results show that separation between ice nucleation particles stemming from microorganisms and those stemming from plants cannot be differentiated solely on proteinaceous features. Further oxidation experiments with ozone showed that black currant is highly stable towards ozone oxidation, indicating a long atmospheric life time.

Secondary ice production via rime-splintering is considered to be an important process for rapid glaciation and high ice crystal numbers observed in mixed-phase convective clouds. An open question is how rime-splintering is triggered in the relatively short time between cloud formation and observations of high ice crystal numbers. We use idealised simulations of a deep convective cloud system to investigate the thermodynamic and cloud microphysical evolution of air parcels, in which the model predicts secondary ice formation. The Lagrangian analysis suggests that the "in-situ" formation of rimers either by growth of primary ice or rain freezing does not play a major role in triggering secondary ice formation. Instead, rimers are predominantly imported into air parcels through sedimentation form higher altitudes. While ice nucleating particles (INPs) initiating heterogeneous freezing of cloud droplets at temperatures warmer than −10 °C have no discernible impact of the occurrence of secondary ice formation, in a scenario with rain freezing secondary ice production is initiated slightly earlier in the cloud evolution and at slightly different places, although with no major impact on the abundance or spatial distribution of secondary ice in the cloud as a whole. These results suggest that for interpreting and analysing observational data and model experiments regarding cloud glaciation and ice formation it is vital to consider the complex vertical coupling of cloud microphysical processes in deep convective clouds via three-dimensional transport and sedimentation. [ABSTRACT FROM AUTHOR]

Heterogeneous ice nucleation in the atmosphere is not fully understood. In particular, our knowledge of biological materials and their atmospheric ice nucleation properties remains scarce. Here, we present the results from systematic investigations of the ice nucleation activity of plant materials using cryo-microscopy. We examined berry juices, frozen berries, as well as extracts of leaves and dried berries of plants native to boreal regions. All of our samples possess reasonable ice nucleation activity. Their ice nucleating particle concentrations per unit of water volume vary between 9.7 × 105 and 9.2 × 109 cm−3 when examined within temperatures of −12 to −34 °C. Mean freezing temperatures ranged from −18.5 to −45.6 °C. We show that all samples contained ice nuclei in a size range below 0.2 µm and remain active if separated from coarse plant tissue. The results of examining ice nucleation properties of leaves and dry berry extracts suggests that their ice-nucleating components can be easily suspended in water. Sea buckthorn and black currant were analyzed using subtilisin (a protease) and urea. Results suggest proteinaceous compounds to play an important role in their ice nucleation activity. These results show that separation between ice nucleation particles stemming from microorganisms and those stemming from plants cannot be differentiated solely on proteinaceous features. Further oxidation experiments with ozone showed that black currant is highly stable towards ozone oxidation, indicating a long atmospheric life time. [ABSTRACT FROM AUTHOR]