Portable Ice Nucleation Chamber Research Articles

Development and characterization of the Portable Ice Nucleation Chamber 2 (PINCii)

Abstract. The Portable Ice Nucleation Chamber 2 (PINCii) is a newly developed continuous flow diffusion chamber (CFDC) for measuring ice nucleating particles (INPs). PINCii is a vertically oriented parallel-plate CFDC that has been engineered to improve upon the limitations of previous generations of CFDCs. This work presents a detailed description of the PINCii instrument and the upgrades that make it unique compared with other operational CFDCs. The PINCii design offers several possibilities for improved INP measurements. Notably, a specific icing procedure results in low background particle counts, which demonstrates the potential for PINCii to measure INPs at low concentrations (<10 L−1). High-spatial-resolution wall-temperature mapping enables the identification of temperature inhomogeneities on the chamber walls. This feature is used to introduce and discuss a new method for analyzing CFDC data based on the most extreme lamina conditions present within the chamber, which represent conditions most likely to trigger ice nucleation. A temperature gradient can be maintained throughout the evaporation section in addition to the main chamber, which enables PINCii to be used to study droplet activation processes or to extend ice crystal growth. A series of both liquid droplet activation and ice nucleation experiments were conducted at temperature and saturation conditions that span the spectrum of PINCii's operational conditions (-50≤ temperature ≤-15 ∘C and 100 ≤ relative humidity with respect to ice ≤160 %) to demonstrate the instrument's capabilities. In addition, typical sources of uncertainty in CFDCs, including particle background, particle loss, and variations in aerosol lamina temperature and relative humidity, are quantified and discussed for PINCii.

Measurement report: Introduction to the HyICE-2018 campaign for measurements of ice-nucleating particles and instrument inter-comparison in the Hyytiälä boreal forest

Abstract. The formation of ice particles in Earth's atmosphere strongly influences the dynamics and optical properties of clouds and their impacts on the climate system. Ice formation in clouds is often triggered heterogeneously by ice-nucleating particles (INPs) that represent a very low number of particles in the atmosphere. To date, many sources of INPs, such as mineral and soil dust, have been investigated and identified in the low and mid latitudes. Although less is known about the sources of ice nucleation at high latitudes, efforts have been made to identify the sources of INPs in the Arctic and boreal environments. In this study, we investigate the INP emission potential from high-latitude boreal forests in the mixed-phase cloud regime. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiälä, Finland, between February and June 2018. The campaign utilized the infrastructure of the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR) II, with additional INP instruments, including the Portable Ice Nucleation Chamber I and II (PINC and PINCii), the SPectrometer for Ice Nuclei (SPIN), the Portable Ice Nucleation Experiment (PINE), the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT) and the Microlitre Nucleation by Immersed Particle Instrument (µL-NIPI), used to quantify the INP concentrations and sources in the boreal environment. In this contribution, we describe the measurement infrastructure and operating procedures during HyICE-2018, and we report results from specific time periods where INP instruments were run in parallel for inter-comparison purposes. Our results show that the suite of instruments deployed during HyICE-2018 reports consistent results and therefore lays the foundation for forthcoming results to be considered holistically. In addition, we compare measured INP concentrations to INP parameterizations, and we observe good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA.

Condensation/immersion mode ice-nucleating particles in a boreal environment

Abstract. Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland at the Station for Measuring Ecosystem–Atmosphere Relations (SMEAR II) in the winter–spring of 2018. Measurements with the Portable Ice Nucleation Chamber (PINC) were conducted at 242 K and 105 % relative humidity with respect to water. The median INP number concentration [INP] during a 6-week measurement period was 13 L−1. The [INP] spanned 3 orders of magnitude and showed a general increase from mid-February until early April. No single dominant local or regional sources of INPs in the boreal environment of southern Finland could be identified. Rather, it is hypothesised that the INPs detected at SMEAR II are a result of long-range transport and dilution of INPs sourced far from the measurement site. Despite high variability, the measured [INP] values fall within the range expected for the [INP] measured elsewhere under similar thermodynamic conditions. The [INP] did not correlate with any of the examined parameters during the entire field campaign, indicating that no one single parameter can be used to predict the [INP] at the measurement location during the examined time period. The absence of a correlation across the entire field campaign also suggests that a variety of particles act as INPs at different times, although it was indirectly determined that ambient INPs are most likely within the size range of 0.1–0.5 µm in diameter on average. On shorter timescales, several particle species correlated well with the [INP]. Depending on the meteorological conditions, black carbon (BC), supermicron biological particles and sub-0.1 µm particles, most likely nanoscale biological fragments such as ice-nucleating macromolecules (INMs), correlated with the INP signal. However, an increase in the concentration of any of these particle species may not necessarily lead to the increase in the [INP]; the reasons for this remain unknown. Limitations of the instrumental set-up and the necessity for future field INP studies are addressed.

Heterogeneous ice nucleation properties of natural desert dust particles coated with a surrogate of secondary organic aerosol

Abstract. Ice nucleation abilities of surface collected mineral dust particles from the Sahara (SD) and Asia (AD) are investigated for the temperature (T) range 253–233 K and for supersaturated relative humidity (RH) conditions in the immersion freezing regime. The dust particles were also coated with a proxy of secondary organic aerosol (SOA) from the dark ozonolysis of α-pinene to better understand the influence of atmospheric coatings on the immersion freezing ability of mineral dust particles. The measurements are conducted on polydisperse particles in the size range 0.01–3 µm with three different ice nucleation chambers. Two of the chambers follow the continuous flow diffusion chamber (CFDC) principle (Portable Ice Nucleation Chamber, PINC) and the Colorado State University CFDC (CSU-CFDC), whereas the third was the Aerosol Interactions and Dynamics in the Atmosphere (AIDA) cloud expansion chamber. From observed activated fractions (AFs) and ice nucleation active site (INAS) densities, it is concluded within experimental uncertainties that there is no significant difference between the ice nucleation ability of the particular SD and AD samples examined. A small bias towards higher INAS densities for uncoated versus SOA-coated dusts is found but this is well within the 1σ (66 % prediction bands) region of the average fit to the data, which captures 75 % of the INAS densities observed in this study. Furthermore, no systematic differences are observed between SOA-coated and uncoated dusts in both SD and AD cases, regardless of coating thickness (3–60 nm). The results suggest that any differences observed are within the uncertainty of the measurements or differences in cloud chamber parameters such as size fraction of particles sampled, and residence time, as well as assumptions in using INAS densities to compare polydisperse aerosol measurements which may show variable composition with particle size. Coatings with similar properties to that of the SOA in this work and with coating thickness up to 60 nm are not expected to impede or enhance the immersion mode ice nucleation ability of mineral dust particles.

A laboratory investigation of the ice nucleation efficiency of three types of mineral and soil dust

Abstract. Surface-collected dust from three different locations around the world was examined with respect to its ice nucleation activity (INA) with the ETH Portable Ice Nucleation Chamber (PINC). Ice nucleation experiments were conducted with particles of 200 and 400 nm in diameter in the temperature range of 233–243 K in both the deposition nucleation and condensation freezing regimes. Several treatments were performed in order to investigate the effect of mineralogical composition, as well as the presence of biological and proteinaceous, organic and soluble compounds on the INA of mineral and soil dust. The INA of untreated dust particles correlated well with the total feldspar and K-feldspar content, corroborating previously published results. The removal of heat-sensitive proteinaceous and organic components from the particle surface with heat decreased the INA of dusts. However, the decrease in the INA was not proportional to the amount of these organic components, indicating that different proteinaceous and organic species have different ice nucleation activities, and the exact speciation is required in order to determine why dusts respond differently to the heating process. The INA of certain dusts increased after the removal of soluble material from the particle surface, demonstrating the low INA of the soluble compounds and/or the exposition of the underlying active sites. Similar to the proteinaceous organic compounds, soluble compounds seem to have different effects on the INA of surface-collected dusts, and a general conclusion about how the presence of soluble material on the particle surface affects its INA is not possible. The investigation of the heated and washed dusts revealed that mineralogy alone is not able to fully explain the observed INA of surface-collected dusts at the examined temperature and relative humidity conditions. The results showed that it is not possible to predict the INA of surface-collected soil dust based on the presence and amount of certain minerals or any particular class of compounds, such as soluble or proteinaceous/organic compounds. Instead, at temperatures of 238–243 K the INA of the untreated, surface-collected soil dust in the condensation freezing mode can be roughly approximated by one of the existing surrogates for atmospheric mineral dust, such as illite NX. Uncertainties associated with mechanical damage and possible changes to the mineralogy during treatments, as well as with the BET surface area and its immediate impact on the number of active sites (ns,BET), are addressed.

The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): laboratory intercomparison of ice nucleation measurements

The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): laboratory intercomparison of ice nucleation measurements

The Horizontal Ice Nucleation Chamber (HINC): INP measurements at conditions relevant for mixed-phase clouds at the High Altitude Research Station Jungfraujoch

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 (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.

Leipzig Ice Nucleation chamber Comparison (LINC): intercomparison of four online ice nucleation counters

Abstract. Ice crystal formation in atmospheric clouds has a strong effect on precipitation, cloud lifetime, cloud radiative properties, and thus the global energy budget. Primary ice formation above 235 K is initiated by nucleation on seed aerosol particles called ice-nucleating particles (INPs). Instruments that measure the ice-nucleating potential of aerosol particles in the atmosphere need to be able to accurately quantify ambient INP concentrations. In the last decade several instruments have been developed to investigate the ice-nucleating properties of aerosol particles and to measure ambient INP concentrations. Therefore, there is a need for intercomparisons to ensure instrument differences are not interpreted as scientific findings.In this study, we intercompare the results from parallel measurements using four online ice nucleation chambers. Seven different aerosol types are tested including untreated and acid-treated mineral dusts (microcline, which is a K-feldspar, and kaolinite), as well as birch pollen washing waters. Experiments exploring heterogeneous ice nucleation above and below water saturation are performed to cover the whole range of atmospherically relevant thermodynamic conditions that can be investigated with the intercompared chambers. The Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the Portable Immersion Mode Cooling chAmber coupled to the Portable Ice Nucleation Chamber (PIMCA-PINC) performed measurements in the immersion freezing mode. Additionally, two continuous-flow diffusion chambers (CFDCs) PINC and the Spectrometer for Ice Nuclei (SPIN) are used to perform measurements below and just above water saturation, nominally presenting deposition nucleation and condensation freezing.The results of LACIS and PIMCA-PINC agree well over the whole range of measured frozen fractions (FFs) and temperature. In general PINC and SPIN compare well and the observed differences are explained by the ice crystal growth and different residence times in the chamber. To study the mechanisms responsible for the ice nucleation in the four instruments, the FF (from LACIS and PIMCA-PINC) and the activated fraction, AF (from PINC and SPIN), are compared. Measured FFs are on the order of a factor of 3 higher than AFs, but are not consistent for all aerosol types and temperatures investigated. It is shown that measurements from CFDCs cannot be assumed to produce the same results as those instruments exclusively measuring immersion freezing. Instead, the need to apply a scaling factor to CFDCs operating above water saturation has to be considered to allow comparison with immersion freezing devices. Our results provide further awareness of factors such as the importance of dispersion methods and the quality of particle size selection for intercomparing online INP counters.

Ice nucleating particles in the Saharan Air Layer

Abstract. This study aims at quantifying the ice nucleation properties of desert dust in the Saharan Air Layer (SAL), the warm, dry and dust-laden layer that expands from North Africa to the Americas. By measuring close to the dust's emission source, before aging processes during the transatlantic advection potentially modify the dust properties, the study fills a gap between in situ measurements of dust ice nucleating particles (INPs) far away from the Sahara and laboratory studies of ground-collected soil. Two months of online INP concentration measurements are presented, which were part of the two CALIMA campaigns at the Izaña observatory in Tenerife, Spain (2373 m a.s.l.), in the summers of 2013 and 2014. INP concentrations were measured in the deposition and condensation mode at temperatures between 233 and 253 K with the Portable Ice Nucleation Chamber (PINC). Additional aerosol information such as bulk chemical composition, concentration of fluorescent biological particles as well as the particle size distribution was used to investigate observed variations in the INP concentration. The concentration of INPs was found to range between 0.2 std L−1 in the deposition mode and up to 2500 std L−1 in the condensation mode at 240 K. It correlates well with the abundance of aluminum, iron, magnesium and manganese (R: 0.43–0.67) and less with that of calcium, sodium or carbonate. These observations are consistent with earlier results from laboratory studies which showed a higher ice nucleation efficiency of certain feldspar and clay minerals compared to other types of mineral dust. We find that an increase of ammonium sulfate, linked to anthropogenic emissions in upwind distant anthropogenic sources, mixed with the desert dust has a small positive effect on the condensation mode INP per dust mass ratio but no effect on the deposition mode INP. Furthermore, the relative abundance of biological particles was found to be significantly higher in INPs compared to the ambient aerosol. Overall, this suggests that atmospheric aging processes in the SAL can lead to an increase in ice nucleation ability of mineral dust from the Sahara. INP concentrations predicted with two common parameterization schemes, which were derived mostly from atmospheric measurements far away from the Sahara but influenced by Asian and Saharan dust, were found to be higher based on the aerosol load than we observed in the SAL, further suggesting aging effects of INPs in the SAL.

The SPectrometer for Ice Nuclei (SPIN): an instrument to investigate ice nucleation

Abstract. The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nucleating particle (INP) counter manufactured by Droplet Measurement Technologies in Boulder, CO. The SPIN is a continuous flow diffusion chamber with parallel plate geometry based on the Zurich Ice Nucleation Chamber and the Portable Ice Nucleation Chamber. This study presents a standard description for using the SPIN instrument and also highlights methods to analyze measurements in more advanced ways. It characterizes and describes the behavior of the SPIN chamber, reports data from laboratory measurements, and quantifies uncertainties associated with the measurements. Experiments with ammonium sulfate are used to investigate homogeneous freezing of deliquesced haze droplets and droplet breakthrough. Experiments with kaolinite, NX illite, and silver iodide are used to investigate heterogeneous ice nucleation. SPIN nucleation results are compared to those from the literature. A machine learning approach for analyzing depolarization data from the SPIN optical particle counter is also presented (as an advanced use). Overall, we report that the SPIN is able to reproduce previous INP counter measurements.

Immersion mode ice nucleation measurements with the new Portable Immersion Mode Cooling chAmber (PIMCA)

AbstractThe new Portable Immersion Mode Cooling chAmber (PIMCA) has been developed for online immersion freezing of single‐immersed aerosol particles. PIMCA is a vertical extension of the established Portable Ice Nucleation Chamber (PINC). PIMCA immerses aerosol particles into cloud droplets before they enter PINC. Immersion freezing experiments on cloud droplets with a radius of 5–7 μm at a prescribed supercooled temperature (T) and water saturation can be conducted, while other ice nucleation mechanisms (deposition, condensation, and contact mode) are excluded. Validation experiments on reference aerosol (kaolinite, ammonium sulfate, and ammonium nitrate) showed good agreement with theory and literature. The PIMCA‐PINC setup was tested in the field during the Zurich AMBient Immersion freezing Study (ZAMBIS) in spring 2014 in Zurich, Switzerland. Significant concentrations of submicron ambient aerosol triggering immersion freezing at T > 236 K were rare. The mean frozen cloud droplet number concentration was estimated to be 7.22·105 L−1 for T < 238 K and determined from the measured frozen fraction and cloud condensation nuclei (CCN) concentrations predicted for the site at a typical supersaturation of SS = 0.3%. This value should be considered as an upper limit of cloud droplet freezing via immersion and homogeneous freezing processes. The predicted ice nucleating particle (INP) concentration based on measured total aerosol larger than 0.5 μm and the parameterization by DeMott et al. (2010) at T = 238 K is INPD10=54 ± 39 L−1. This is a lower limit as supermicron particles were not sampled with PIMCA‐PINC during ZAMBIS.

Ice Nucleating Particle Measurements at 241 K during Winter Months at 3580 m MSL in the Swiss Alps

Abstract Ice nucleating particle (INP) concentrations were measured at the High Altitude Research Station Jungfraujoch, Switzerland, 3580 m above mean sea level during the winter months of 2012, 2013, and 2014 with the Portable Ice Nucleation Chamber (PINC). During the measurement periods, the research station was mostly located in the free troposphere, and particle concentrations were low. At temperature T = 241 K, INP concentrations in the deposition regime [relative humidity with respect to water (RHw) = 93%] were, on average, below 1.09 per standard liter of air (stdL−1; normalized to 1013 hPa and 273 K) and 4.7 ± 8.3 stdL−1 in the condensation regime (RHw = 103%) in winter 2014. The deployment of a particle concentrator upstream of PINC decreased the limit of detection (LOD) by a factor of 3 compared to earlier measurements. The authors discuss a potential bias of INP measurements toward higher concentrations if data below the LOD are disregarded and thus recommend reporting subLOD data in future publications. Saharan dust and more local, basaltic dust mixed with marine aerosol were found to constitute the dominant INP type. Bioaerosols were not observed to play a role in ice nucleation during winter because of their low concentration during this period. The INP concentrations at Jungfraujoch are low in comparison to other studies of INP at this temperature. This represents the first study addressing interannual variations of INP concentrations during winter at one location.

Effect of photochemical ageing on the ice nucleation properties of diesel and wood burning particles

Abstract. A measurement campaign (IMBALANCE) conducted in 2009 was aimed at characterizing the physical and chemical properties of freshly emitted and photochemically aged combustion particles emitted from a log wood burner and diesel vehicles: a EURO3 Opel Astra with a diesel oxidation catalyst (DOC) but no particle filter and a EURO2 Volkswagen Transporter TDI Syncro without emission aftertreatment. Ice nucleation experiments in the deposition and condensation freezing modes were conducted with the Portable Ice Nucleation Chamber (PINC) at three nominal temperatures, −30 °C, −35 °C and −40 °C. Freshly emitted diesel particles showed ice formation only at −40 °C in the deposition mode at 137% relative humidity with respect to ice (RHi) and 92% relative humidity with respect to water (RHw), and photochemical ageing did not play a role in modifying their ice nucleation behaviour. Only one diesel experiment where α-pinene was added for the ageing process, showed an ice nucleation enhancement at −35 °C. Wood burning particles also act as ice nuclei (IN) at −40 °C in the deposition mode at the same conditions as for diesel particles and photochemical ageing also did not alter the ice formation properties of the wood burning particles. Unlike diesel particles, wood burning particles form ice via condensation freezing at −35 °C whereas no ice nucleation was observed at −30 °C. Photochemical ageing did not affect the ice nucleation ability of the diesel and wood burning particles at the three different temperatures investigated but a broader range of temperatures below −40 °C need to be investigated in order to draw an overall conclusion on the effect of photochemical ageing on deposition/condensation ice nucleation across the entire temperature range relevant to cold clouds.

Ice nuclei properties within a Saharan dust event at the Jungfraujoch in the Swiss Alps

Abstract. The new portable ice nucleation chamber (PINC) developed by the Institute for Atmospheric and Climate Sciences of ETH Zurich was operated during two measurement campaigns at the high alpine research station Jungfraujoch situated at 3580 m a.s.l, in March and June 2009. During this time of the year, a high probability of Saharan dust events (SDE) at the Jungfraujoch has been observed. We used an impactor with a cutoff size of 1 μm aerodynamic diameter and operated the system at −31 °C and relative humidities of 127 % and 91 % with respect to ice and water, respectively. Investigation of the ambient number concentration of ice nuclei (IN) in the deposition nucleation mode and during a SDE in the free troposphere is reported. The results discussed in this paper are the first continuous IN measurements over a period of several days at the Jungfraujoch. The average IN concentration found during the campaign in March was 8 particles per liter whereas during the campaign in June, the average number concentration was higher up to 14 particles per liter. Two SDEs were detected on 15 and 16 June 2009. Our measurements show that the SDEs had IN number concentration up to several hundreds per liter. We found the best correlation between the number concentration of the larger particle fraction measured by an optical particle counter and the IN number concentration during a Saharan dust event. This correlation factor is higher for particles larger than 0.5 μm meaning that a higher concentration of larger particles induced higher IN number concentration. No correlation could be found between the black carbon mass concentration and the variations in IN number concentration.