Abstract. 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 (RH w ) of ±1.5 %, which translates into an uncertainty in RH with respect to ice (RH i ) 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 (RH w = 94 %), relevant for the formation of ice clouds, and in the watersupersaturated regime (RH w = 104 %) to represent ice formation occurring under mixed-phase cloud conditions. In winters 2015 and 2016 the median INP concentrations at RH w = 94 % was below the minimum detectable concentration. At RH w = 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 RH w = 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.

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.

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.

Abstract. 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.

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.

<p><strong>Abstract.</strong> 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 (RH<sub>w</sub>) of ±1.5 %, which translates to an uncertainty in RH with respect to ice (RH<sub>i</sub>) 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 (RH<sub>w</sub> = 94 %), relevant for the formation of ice clouds, and in the water supersaturated regime (RH<sub>w</sub> = 103–104 %) to represent ice formation occurring under mixed-phase cloud conditions. In winter 2015 and 2016 the median INP concentrations at RH<sub>w</sub> = 94 % was below the minimum detectable concentration. At RH<sub>w</sub> = 104 %, INP concentrations were an order of magnitude higher, with median concentrations in winter 2015 of 2.8 per standard liter (stdL<sup>−1</sup>; normalized to standard temperature T = 273 K and pressure p = 1013 hPa) and 4.7 stdL<sup>−1</sup> in winter 2016. The measurements are in agreement with previous winter measurements obtained with the Portable Ice Nucleation Chamber, PINC, of 2.2 stdL<sup>−1</sup> at the same location. During winter 2015, two events caused the INP concentrations at RH<sub>w</sub> = 103–104 % to significantly increase above the campaign average. First, an increase to 72.1 stdL<sup>−1</sup> 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<sup>−1</sup> 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.</p>

The custom-built Portable Fine Particle Concentrator (PFPC) is evaluated for the measurement of ice nucleating particles (INPs) in the atmosphere. The concentrations of INPs in remote regions of the atmosphere are very low, often close to instrumental detection limits. The PFPC is a dual slit-nozzle virtual impactor where particles are concentrated from an input flow of 250 LPM (litres per minute) into an output flow of 10 LPM. The enrichment factors for ambient particles with diameters between 0.4 and 2.5 µm were found to be 21 ± 5 at sea level and 18 ± 2 at a field station 3580 meters above sea level for the PFPC operated in horizontal configuration. Similar enhancement factors (16 ± 5) in the concentrations of INPs measured by the Horizontal Ice Nucleation Chamber at the high altitude station were observed when the air mass was characterized by high numbers of particles larger than 0.5 µm. When the number size distribution was dominated by particles smaller than 0.5 µm, the INP enrichment factor was considerably lower. Corroborating short-term measurements were provided by additional INP-measuring instruments, the Fast Ice Nucleus CHamber and the Frankfurt Ice Deposition Freezing Experiment. Results from two aerosol mass spectrometers also indicate significant particle enhancement using the PFPC. These results indicate that the PFPC can be usefully deployed to improve the detection efficiency of ambient INP measurements.

Abstract. 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.