ALBERT

Description: Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at –46 °C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L–1. Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties.

Description: In situ cloud observations at mountain-top research stations regularly measure ice crystal number concentrations (ICNCs) orders of magnitudes higher than expected from measurements of ice nucleating particle (INP) concentrations. Thus, several studies suggest that mountain-top in situ cloud microphysical measurements are influenced by surface processes, e.g., blowing snow, hoar frost or riming on snow-covered trees, rocks and the snow surface. This limits the relevance of such measurements for the study of microphysical properties and processes in free-floating clouds. This study assesses the impact of surface processes on in situ cloud observations at the Sonnblick Observatory in the Hohen Tauern region, Austria. Vertical profiles of ICNCs above a snow-covered surface were observed up to a height of 10 m. The ICNC decreases at least by a factor of 2 at 10 m if the ICNC at the surface is larger than 100 L−1. This decrease can be up to 1 order of magnitude during in-cloud conditions and reached its maximum of more than 2 orders of magnitudes when the station was not in cloud. For one case study, the ICNC for regular and irregular ice crystals showed a similar relative decrease with height. This suggests that either surface processes produce both irregular and regular ice crystals or other effects modify the ICNCs near the surface. Therefore, two near-surface processes are proposed to enrich ICNCs near the surface. Either sedimenting ice crystals are captured in a turbulent layer above the surface or the ICNC is enhanced in a convergence zone because the cloud is forced over a mountain. These two processes would also have an impact on ICNCs measured at mountain-top stations if the surrounding surface is not snow covered. Conclusively, this study strongly suggests that ICNCs measured at mountain-top stations are not representative of the properties of a cloud further away from the surface.

Description: In this work we describe the Horizontal Ice Nucleation Chamber (HINC) as a new instrument to measure ambient ice-nucleating particle (INP) concentrations for conditions relevant to mixed-phase clouds. Laboratory verification and validation experiments confirm the accuracy of the thermodynamic conditions of temperature (T) and relative humidity (RH) in HINC with uncertainties in T of ±0.4 K and in RH with respect to water (RHw) of ±1.5 %, which translates into an uncertainty in RH with respect to ice (RHi) of ±3.0 % at T 〉 235 K. For further validation of HINC as a field instrument, two measurement campaigns were conducted in winters 2015 and 2016 at the High Altitude Research Station Jungfraujoch (JFJ; Switzerland, 3580 m a. s. l. ) to sample ambient INPs. During winters 2015 and 2016 the site encountered free-tropospheric conditions 92 and 79 % of the time, respectively. We measured INP concentrations at 242 K at water-subsaturated conditions (RHw = 94 %), relevant for the formation of ice clouds, and in the water-supersaturated regime (RHw = 104 %) to represent ice formation occurring under mixed-phase cloud conditions. In winters 2015 and 2016 the median INP concentrations at RHw = 94 % was below the minimum detectable concentration. At RHw = 104 %, INP concentrations were an order of magnitude higher, with median concentrations in winter 2015 of 2.8 per standard liter (std L−1; normalized to standard T of 273 K and pressure, p, of 1013 hPa) and 4.7 std L−1 in winter 2016. The measurements are in agreement with previous winter measurements obtained with the Portable Ice Nucleation Chamber (PINC) of 2.2 std L−1 at the same location. During winter 2015, two events caused the INP concentrations at RHw = 104 % to significantly increase above the campaign average. First, an increase to 72.1 std L−1 was measured during an event influenced by marine air, arriving at the JFJ from the North Sea and the Norwegian Sea. The contribution from anthropogenic or other sources can thereby not be ruled out. Second, INP concentrations up to 146.2 std L−1 were observed during a Saharan dust event. To our knowledge this is the first time that a clear enrichment in ambient INP concentration in remote regions of the atmosphere is observed during a time of marine air mass influence, suggesting the importance of marine particles on ice nucleation in the free troposphere.

Description: Ice nucleation is the source of primary ice crystals in mixed-phase clouds. Only a small fraction of aerosols called ice nucleating particles (INPs) catalyze ice formation, with their nature and origin remaining unclear. In this study, we investigate potential predictor parameters of meteorological conditions and aerosol properties for INP concentrations at mixed-phase cloud condition at 242 K. Measurements were conducted at the High Altitude Research Station Jungfraujoch (Switzerland, 3580 m a.s.l.), which is located predominantly in the free troposphere (FT) but can occasionally receive injections from the boundary layer (BLI). Measurements are taken during a long-term study of eight field campaigns, allowing for the first time an interannual (2014–2017) and seasonal (spring, summer, and winter) distinction of high-time-resolution INP measurements. We investigate ranked correlation coefficients between INP concentrations and meteorological parameters and aerosol properties. While a commonly used parameterization lacks in predicting the observed INP concentrations, the best INP predictor is the total available surface area of the aerosol particles, with no obvious seasonal trend in the relationship. Nevertheless, the predicting capability is less pronounced in the FT, which might be caused by ageing effects. Furthermore, there is some evidence of anthropogenic influence on INP concentrations during BLI. Our study contributes to an improved understanding of ice nucleation in the free troposphere, however, it also underlines that a knowledge gap of ice nucleation in such an environment exists.

Description: Clouds containing ice are vital for precipitation formation and are important in determining the Earth's radiative budget. However, primary formation of ice in clouds is not fully understood. In the presence of ice nucleating particles (INPs), the phase change to ice is promoted, but identification and quantification of INPs in a natural environment remains challenging because of their low numbers. In this paper, we quantify INP number concentrations in the free troposphere (FT) as measured at the High Altitude Research Station Jungfraujoch (JFJ), during the winter, spring, and summer of the years 2014–2017. INPs were measured at conditions relevant for mixed-phase cloud formation at T = 241/242 K. To date, this is the longest timeline of semiregular measurements akin to online INP monitoring at this site and sampling conditions. We find that INP concentrations in the background FT are on average capped at 10/stdL (liter of air at standard conditions [T = 273 K and p = 1013 hPa]) with an interquartile range of 0.4–9.6/stdL, as compared to measurements during times when other air mass origins (e.g., Sahara or marine boundary layer) prevailed. Elevated concentrations were measured in the field campaigns of 2016, which might be due to enhanced influence from Saharan dust and marine boundary layer air arriving at the JFJ. The upper limit of INP concentrations in the background FT is supported by measurements performed at similar conditions, but at different locations in the FT, where we find INP concentrations to be below 13/stdL most of the time. ©2018. The Authors.

Description: In-situ cloud observations at mountain-top research stations regularly measure ice crystal number concentrations (ICNCs) orders of magnitudes higher than expected from measurements of ice nucleating particle (INP) concentrations. Thus, several studies suggest that mountain-top in-situ measurements are influenced by surface processes, e.g. blowing snow, hoar frost or riming on snow covered trees, rocks and the snow surface. A strong impact on the observed ICNCs on mountain-top stations by surface processes may limit the relevance of such measurements and possibly affects the development of orographic clouds. This study assesses the impact of surface processes on in-situ cloud observations at the Sonnblick Observatory in the Hohen Tauern Region, Austria. Vertical profiles of ICNCs above a snow covered surface were observed up to a height of 10 m. The ICNC decreases at least by a factor of two at 10 m, if the ICNC at the surface is larger than 100 L−1. This decrease can be up to one order of magnitude during in-cloud conditions and reached its maximum of more than two orders of magnitudes when the station was not in cloud. For one case study, the ICNC for regular and irregular ice crystals showed a similar relative decrease with height, which cannot be explained by the above mentioned surface processes. Therefore, two near-surface processes are proposed to enrich ICNCs and explain these finding. Either sedimenting ice crystals are captured in a turbulent layer above the surface or the ICNC is enhanced in a convergence zone, because the cloud is forced over a mountain. These two processes would also have an impact on ICNCs measured at mountain-top stations if the surrounding surface is not snow covered. Conclusively, this study strongly suggests that ICNCs measured at mountain-top stations are not representative for the properties of a cloud further away from the surface.

Description: In this work we describe the Horizontal Ice Nucleation Chamber, HINC as a new instrument to measure ambient ice nucleating particle (INP) concentrations for conditions relevant to mixed-phase clouds. Laboratory verification and validation experiments confirm accuracy of the thermodynamic conditions of temperature (T) and relative humidity (RH) in HINC with uncertainties in temperature of ±0.4 K and in RH with respect to water (RHw) of ±1.5 %, which translates to an uncertainty in RH with respect to ice (RHi) of ±3.0 % at T 〉 235 K. For further validation of HINC as a field instrument, two measurement campaigns were conducted in winters 2015 and 2016 at the High Altitude Research Station Jungfraujoch (JFJ; Switzerland, 3580 m a.s.l.) to sample ambient INPs. During winters 2015 and 2016 the site encountered free tropospheric conditions 92 % and 79 % of the time respectively. We measured INP concentrations at 242 K at water sub-saturated conditions (RHw = 94 %), relevant for the formation of ice clouds, and in the water supersaturated regime (RHw = 103–104 %) to represent ice formation occurring under mixed-phase cloud conditions. In winter 2015 and 2016 the median INP concentrations at RHw = 94 % was below the minimum detectable concentration. At RHw = 104 %, INP concentrations were an order of magnitude higher, with median concentrations in winter 2015 of 2.8 per standard liter (stdL−1; normalized to standard temperature T = 273 K and pressure p = 1013 hPa) and 4.7 stdL−1 in winter 2016. The measurements are in agreement with previous winter measurements obtained with the Portable Ice Nucleation Chamber, PINC, of 2.2 stdL−1 at the same location. During winter 2015, two events caused the INP concentrations at RHw = 103–104 % to significantly increase above the campaign average. First, an increase to 72.1 stdL−1 was measured during an event influenced by marine air, coming from the Northern Sea and the Norwegian Sea. Second, INP concentrations up to 146.2 stdL−1 were observed during a Saharan dust event. To our knowledge this is the first time that a clear enrichment in ambient INP concentration is observed during a time of marine air mass influence, indicating the importance of marine particles on ice nucleation in the free troposphere.

Description: Atmospheric ice-nucleating particles (INPs) play an important role in determining the phase of clouds, which affects their albedo and lifetime. A lack of data on the spatial and temporal variation of INPs around the globe limits our predictive capacity and understanding of clouds containing ice. Automated instrumentation that can robustly measure INP concentrations across the full range of tropospheric temperatures is needed in order to address this knowledge gap. In this study, we demonstrate the functionality and capacity of the new Portable Ice Nucleation Experiment (PINE) to study ice nucleation processes and to measure INP concentrations under conditions pertinent for mixed-phase clouds, with temperatures from about −10 to about −40 ∘C. PINE is a cloud expansion chamber which avoids frost formation on the cold walls and thereby omits frost fragmentation and related background ice signals during the operation. The development, working principle and treatment of data for the PINE instrument is discussed in detail. We present laboratory-based tests where PINE measurements were compared with those from the established AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber. Within experimental uncertainties, PINE agreed with AIDA for homogeneous freezing of pure water droplets and the immersion freezing activity of mineral aerosols. Results from a first field campaign conducted at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) observatory in Oklahoma, USA, from 1 October to 14 November 2019 with the latest PINE design (a commercially available PINE chamber) are also shown, demonstrating PINE's ability to make automated field measurements of INP concentrations at a time resolution of about 8 min with continuous temperature scans for INP measurements between −10 and −30 ∘C. During this field campaign, PINE was continuously operated for 45 d in a fully automated and semi-autonomous way, demonstrating the capability of this new instrument to also be used for longer-term field measurements and INP monitoring activities in observatories.

Description: We present our field results of ice-nucleating particle (INP) measurements from the commercialized version of the Portable Ice Nucleation Experiment (PINE) chamber from two different campaigns. Our first field campaign, TxTEST, was conducted at West Texas A&M University (July–August 2019), and the other campaign, ExINP-SGP, was held at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site (October–November 2019). In both campaigns, the PINE made semi-autonomous INP measurements at a high-time-resolution of 8 min for individual expansions with continuous temperature scans from −5 to −35 °C in 90 min. The PINE instrument was set to have a minimum detection capability of ~0.3 INPs per liter of air. To complement our online PINE measurements, polycarbonate filter impactor and liquid impinger samples were also collected next to the PINE. Offline droplet-freezing assays were later conducted from the filter and impinger samples for the immersion freezing mode. Our preliminary results suggested that the immersion freezing mode was the dominant ice-nucleation mechanism at the SGP site compared to the deposition mode. We did not find any statistical correlation between cloud condensation nuclei (CCN) and INP concentration during our ExINP-SGP period, suggesting that CCN activation is not a significant prerequisite for ice nucleation at the SGP site. In addition, we analyzed the relationship between various aerosol particle size ranges and INP abundance. At SGP, we found an increase in INPs with the super-micron particles, especially for diameters 〉2 μm across the entire heterogeneous freezing temperature range examined by PINE. Lastly, we computed a variety of INP parameters, such as, ice nucleation active surface site density, water activity-based freezing, and cumulative INP per liter of air, representing the ambient INPs in the SGP. Our field campaign results demonstrated the PINE’s ability to make remote INP measurements, promising future long-term operations including at isolated locations.

Description: In this work, an abundance of ice-nucleating particles (INPs) from livestock facilities was studied through laboratory measurements from cloud-simulation chamber experiments and field investigation in the Texas Panhandle. Surface materials from two livestock facilities, one in the Texas Panhandle and another from McGregor, Texas, were selected as dust proxies for laboratory analyses. These two samples possessed different chemical and biological properties. A combination of aerosol interaction and dynamics in the atmosphere (AIDA) measurements and offline ice spectrometry was used to assess the immersion freezing mode ice nucleation ability and efficiency of these proxy samples at temperatures above −29 ∘C. A dynamic filter processing chamber was also used to complement the freezing efficiencies of submicron and supermicron particles collected from the AIDA chamber. For the field survey, periodic ambient particle sampling took place at four commercial livestock facilities from July 2017 to July 2019. INP concentrations of collected particles were measured using an offline freezing test system, and the data were acquired for temperatures between −5 and −25 ∘C. Our AIDA laboratory results showed that the freezing spectra of two livestock dust proxies exhibited higher freezing efficiency than previously studied soil dust samples at temperatures below −25 ∘C. Despite their differences in composition, the freezing efficiencies of both proxy livestock dust samples were comparable to each other. Our dynamic filter processing chamber results showed on average approximately 50 % supermicron size dominance in the INPs of both dust proxies. Thus, our laboratory findings suggest the importance of particle size in immersion freezing for these samples and that the size might be a more important factor for immersion freezing of livestock dust than the composition. From a 3-year field survey, we measured a high concentration of ambient INPs of 1171.6 ± 691.6 L−1 (average ± standard error) at −25 ∘C for aerosol particles collected at the downwind edges of livestock facilities. An obvious seasonal variation in INP concentration, peaking in summer, was observed, with the maximum at the same temperature exceeding 10 000 L−1 on 23 July 2018. The observed high INP concentrations suggest that a livestock facility is a substantial source of INPs. The INP concentration values from our field survey showed a strong correlation with measured particulate matter mass concentration, which supports the importance of size in ice nucleation of particles from livestock facilities.