Ice Nucleating Particles Number Concentrations Research Articles

Measurement report: Atmospheric ice nuclei in the Changbai Mountains (2623 m a.s.l.) in northeastern Asia

Abstract. Atmospheric ice nucleation plays an important role in modulating the global hydrological cycle and atmospheric radiation balance. To date, few comprehensive field observations of ice nuclei have been carried out at high-altitude sites, which are close to the height of mixed-phase cloud formation. In this study, we measured the concentration of ice-nucleating particles (INPs) in the immersion freezing mode at the summit of the Changbai Mountains (2623 m above sea level), northeast Asia, in summer 2021. The cumulative number concentration of INPs varied from 1.6 × 10−3 to 78.3 L−1 over the temperature range of −5.5 to −29.0 °C. Proteinaceous-based biological materials accounted for the majority of INPs, with the proportion of biological INPs (bio-INPs) exceeding 67 % across the entire freezing-temperature range, with this proportion even exceeding 90 % above −13.0 °C. At freezing temperatures ranging from −11.0 to −8.0 °C, bio-INPs were found to significantly correlate with wind speed (r = 0.5–0.8, p < 0.05) and Ca2+ (r = 0.6–0.9), and good but not significant correlation was found with isoprene (r = 0.6–0.7) and its oxidation products (isoprene × O3) (r = 0.7), suggesting that biological aerosols may attach to or mix with soil dust and contribute to INPs. During the daytime, bio-INPs showed a positive correlation with the planetary boundary layer (PBL) height at freezing temperatures ranging from −22.0 to −19.5 °C (r > 0.7, p < 0.05), with the valley breezes from southern mountainous regions also influencing the concentration of INPs. Moreover, the long-distance transport of air mass from the Japan Sea and South Korea significantly contributed to the high concentrations of bio-INPs. Our study emphasizes the important role of biological sources of INPs in the high-altitude atmosphere of northeastern Asia and the significant contribution of long-range transport to the INP concentrations in this region.

Dominant Role of Arctic Dust With High Ice Nucleating Ability in the Arctic Lower Troposphere

AbstractRecent observations show that dust emitted within the Arctic (Arctic dust) has a remarkably high ice nucleating ability, especially between −20°C and −5°C, but its impacts on the number concentrations of ice nucleating particles (INPs) and radiative balance in the Arctic are not well understood. Here we incorporate an observation‐based ice‐nucleation parameterization indicating the high ice nucleating ability of Arctic dust into a global aerosol‐climate model. A simulation using this parameterization better reproduces INP observations in the Arctic and estimates >100 times higher dust INP number concentrations with ∼100% contribution from Arctic dust in the Arctic lower troposphere (>60°N and >700 hPa) during summer and fall (June–November) than a simulation applying a standard ice‐nucleation parameterization suitable for desert dust to Arctic dust. Our results demonstrate the importance of considering an ice‐nucleation parameterization suitable for Arctic dust when simulating INPs and their effects on aerosol‐cloud interactions in the Arctic.

The Role of Mineral Dust Aerosol Particles in Aviation Soot‐Cirrus Interactions

AbstractPredicting cirrus cloud properties with confidence requires a sound understanding of the relative roles of homogeneous and heterogeneous ice formation. This study explores the effect of mineral dust and contrail‐processed aviation soot particles as ice‐nucleating particles (INPs) competing with liquid solution droplets in cirrus formation. We study aerosol‐cirrus interactions by accounting for atmospheric variability in updraft speeds and INP number concentrations. Our results confirm the dominant role of mineral dust in ice nucleation events in cirrus clouds. In addition, we show that pre‐existing thin cirrus may suppress ice formation when updraft speeds are low. We find that homogeneous freezing of liquid solution droplets dominates clear‐sky aerosol‐cirrus interaction above a threshold updraft speed determined by total number concentrations and ice nucleation abilities of INPs. When mineral dust particles exceed number concentrations of 10 L−1, they reduce homogeneously nucleated ice crystal numbers significantly and even prevent homogeneous freezing for frequently observed local updraft speeds between 10 and 20 cm s−1. When both mineral dust and aviation soot particles coexist with solution droplets, dust typically prevents ice nucleation by aviation soot. Aviation soot exerts a notable impact on cirrus ice numbers only if updrafts are weak, large soot particles are present in number concentrations that are considerably higher than typically observed in emission measurements, and/or number concentrations of mineral dust and other INPs are low. Overall, our results elucidate the role of aviation soot‐cirrus interactions in the presence of other INP types.

Predicting atmospheric background number concentration of ice-nucleating particles in the Arctic

Abstract. Mixed-phase clouds (MPCs) can have a net warming or cooling radiative effect on Earth's climate influenced by the phase and concentration of cloud particles. They have received considerable attention due to high spatial coverage and occurrence frequency in the Arctic. To initiate ice formation in MPCs at temperatures above −38 ∘C, ice-nucleating particles (INPs) are required, which therefore have important implications on the radiative properties of MPCs by altering the ice-to-liquid ratio of hydrometeors. As a result, constraining ambient INP concentrations could promote accurate representation of cloud microphysical processes and reduce the uncertainties in estimating the cloud-phase-related climate feedback in climate models. Currently, INP parameterizations are lacking for remote Arctic environments. Here we present INP number concentrations and their variability measured in Ny-Ålesund (Svalbard) at temperatures between 0 and −30 ∘C. No distinguishable seasonal difference was observed from 12 weeks of field measurements during October and November 2019 and March and April 2020. Compared to existing studies, the absence of a seasonal difference is not surprising, as most seasonal differences are reported for summer versus winter time INP concentrations. In addition, correlating INP concentrations to aerosol physical properties was not successful. Therefore, we propose a lognormal-distribution-based parameterization to predict Arctic INP concentration solely as a function of temperature, specifically for the transition seasons autumn and spring to fill in the data gap in the literature pertaining to these seasons. In practice, the parameterized variables allow for (i) the prediction of the most likely INP concentrations and (ii) the retrieval of the governing distribution of INP concentrations at given temperatures in the Arctic.

Circum-Antarctic abundance and properties of CCN and INPs

Abstract. Aerosol particles acting as cloud condensation nuclei (CCN) or ice-nucleating particles (INPs) play a major role in the formation and glaciation of clouds. Thereby they exert a strong impact on the radiation budget of the Earth. Data on abundance and properties of both types of particles are sparse, especially for remote areas of the world, such as the Southern Ocean (SO). In this work, we present unique results from ship-borne aerosol-particle-related in situ measurements and filter sampling in the SO region, carried out during the Antarctic Circumnavigation Expedition (ACE) in the austral summer of 2016–2017. An overview of CCN and INP concentrations over the Southern Ocean is provided and, using additional quantities, insights regarding possible CCN and INP sources and origins are presented. CCN number concentrations spanned 2 orders of magnitude, e.g. for a supersaturation of 0.3 % values ranged roughly from 3 to 590 cm−3. CCN showed variable contributions of organic and inorganic material (inter-quartile range of hygroscopicity parameter κ from 0.2 to 0.9). No distinct size dependence of κ was apparent, indicating homogeneous composition across sizes (critical dry diameter on average between 30 and 110 nm). The contribution of sea spray aerosol (SSA) to the CCN number concentration was on average small. Ambient INP number concentrations were measured in the temperature range from −5 to −27 ∘C using an immersion freezing method. Concentrations spanned up to 3 orders of magnitude, e.g. at −16 ∘C from 0.2 to 100 m−3. Elevated values (above 10 m−3 at −16 ∘C) were measured when the research vessel was in the vicinity of land (excluding Antarctica), with lower and more constant concentrations when at sea. This, along with results of backward-trajectory analyses, hints towards terrestrial and/or coastal INP sources being dominant close to ice-free (non-Antarctic) land. In pristine marine areas INPs may originate from both oceanic sources and/or long-range transport. Sampled aerosol particles (PM10) were analysed for sodium and methanesulfonic acid (MSA). Resulting mass concentrations were used as tracers for primary marine and secondary aerosol particles, respectively. Sodium, with an average mass concentration around 2.8 µg m−3, was found to dominate the sampled, identified particle mass. MSA was highly variable over the SO, with mass concentrations up to 0.5 µg m−3 near the sea ice edge. A correlation analysis yielded strong correlations between sodium mass concentration and particle number concentration in the coarse mode, unsurprisingly indicating a significant contribution of SSA to that mode. CCN number concentration was highly correlated with the number concentration of Aitken and accumulation mode particles. This, together with a lack of correlation between sodium mass and Aitken and accumulation mode number concentrations, underlines the important contribution of non-SSA, probably secondarily formed particles, to the CCN population. INP number concentrations did not significantly correlate with any other measured aerosol physico-chemical parameter.

Studies on the Competition Between Homogeneous and Heterogeneous Ice Nucleation in Cirrus Formation

AbstractCirrus ice crystals are produced heterogeneously on ice‐nucleating particles (INPs) and homogeneously in supercooled liquid solution droplets. They grow by uptake of water molecules from the ice‐supersaturated vapor. The precursor particles, characterized by disparate ice nucleation abilities and number concentrations, compete for available vapor during ice formation events. We investigate cirrus formation events systematically in different temperature and updraft regimes, and for different INP number concentrations and time‐independent nucleation efficiencies. We consider vertical air motion variability due to mesoscale gravity waves and effects of supersaturation‐dependent deposition coefficients for water molecules on ice surfaces. We analyze ice crystal properties to better understand the dynamics of competing nucleation processes. We study the reduction of ice crystal numbers produced by homogeneous freezing due to INPs in both, individual simulations assuming constant updraft speeds and in ensemble simulations based on a stochastic representation of vertical wind speed fluctuations. We simulate and interpret probability distributions of total nucleated ice crystal number concentrations, showing signatures of homogeneous and heterogeneous nucleation. At typically observed, mean updraft speeds (≈15 cm s−1) competing nucleation should occur frequently, even at rather low INP number concentrations (<10 L−1). INPs increase cirrus occurrence and may alter cirrus microphysical properties without entirely suppressing homogeneous freezing events. We suggest to improve ice growth models, especially for low cirrus temperatures (<220 K) and low ice supersaturation (<0.3).

The contribution of Saharan dust to the ice-nucleating particle concentrations at the High Altitude Station Jungfraujoch (3580 m a.s.l.), Switzerland

Abstract. The ice phase in mixed-phase clouds has a pivotal role in global precipitation formation as well as for Earth's radiative budget. Above 235 K, sparse particles with the special ability to initiate ice formation, ice-nucleating particles (INPs), are responsible for primary ice formation within these clouds. Mineral dust has been found to be one of the most abundant INPs in the atmosphere at temperatures colder than 258 K. However, the extent of the abundance and distribution of INPs remains largely unknown. To better constrain and quantify the impact of mineral dust on ice nucleation, we investigate the frequency of Saharan dust events (SDEs) and their contribution to the INP number concentration at 243 K and at a saturation ratio with respect to liquid water (Sw) of 1.04 at the High Altitude Research Station Jungfraujoch (JFJ; 3580 m a.s.l.) from February to December 2020. Using the single-scattering albedo Ångström exponent retrieved from a nephelometer and an Aethalometer, satellite-retrieved dust mass concentrations, simulated tropospheric residence times, and the attenuated backscatter signal from a ceilometer as proxies, we detected 26 SDEs, which in total contributed to 17 % of the time span analyzed. We found every SDE to show an increase in median INP concentrations compared to those of all non-SDE periods; however, they were not always statistically significant. Median INP concentrations of individual SDEs spread between 1.7 and 161 INP std L−1 and thus 2 orders of magnitude. In the entire period analyzed, 74.7 ± 0.2 % of all INPs were measured during SDEs. Based on satellite-retrieved dust mass concentrations, we argue that mineral dust is also present at JFJ outside of SDEs but at much lower concentrations, thus still contributing to the INP population. We estimate that 97 % of all INPs active in the immersion mode at 243 K and Sw=1.04 at JFJ are dust particles. Overall, we found INP number concentrations to follow a leptokurtic lognormal frequency distribution. We found the INP number concentrations during SDEs to correlate with the ceilometer backscatter signals from a ceilometer located 4.5 km north of JFJ and 1510 m lower in altitude, thus scanning the air masses at the same altitude as JFJ. Using the European ceilometer network allows us to study the atmospheric pathway of mineral dust plumes over a large domain, which we demonstrate in two case studies. These studies showed that mineral dust plumes form ice crystals at cirrus altitudes, which then sediment to lower altitudes. Upon sublimation in dryer air layers, the residual particles are left potentially pre-activated. Future improvements to the sampling lines of INP counters are required to study whether these particles are indeed pre-activated, leading to larger INP number concentrations than reported here.

Model emulation to understand the joint effects of ice-nucleating particles and secondary ice production on deep convective anvil cirrus

Abstract. Ice crystal formation in the mixed-phase region of deep convective clouds can affect the properties of climatically important convectively generated anvil clouds. Small ice crystals in the mixed-phase cloud region can be formed by heterogeneous ice nucleation by ice-nucleating particles (INPs) and secondary ice production (SIP) by, for example, the Hallett–Mossop process. We quantify the effects of INP number concentration, the temperature dependence of the INP number concentration at mixed-phase temperatures, and the Hallett–Mossop splinter production efficiency on the anvil of an idealised deep convective cloud using a Latin hypercube sampling method, which allows optimal coverage of a multidimensional parameter space, and statistical emulation, which allows us to identify interdependencies between the three uncertain inputs. Our results show that anvil ice crystal number concentration (ICNC) is determined predominately by INP number concentration, with the temperature dependence of ice-nucleating aerosol activity having a secondary role. Conversely, anvil ice crystal size is determined predominately by the temperature dependence of ice-nucleating aerosol activity, with INP number concentration having a secondary role. This is because in our simulations ICNC is predominately controlled by the number concentration of cloud droplets reaching the homogeneous freezing level which is in turn determined by INP number concentrations at low temperatures. Ice crystal size, however, is more strongly affected by the amount of liquid available for riming and the time available for deposition growth which is determined by INP number concentrations at higher temperatures. This work indicates that the amount of ice particle production by the Hallett–Mossop process is determined jointly by the prescribed Hallett–Mossop splinter production efficiency and the temperature dependence of ice-nucleating aerosol activity. In particular, our sampling of the joint parameter space shows that high rates of SIP do not occur unless the INP parameterisation slope (the temperature dependence of the number concentration of particles which nucleate ice) is shallow, regardless of the prescribed Hallett–Mossop splinter production efficiency. A shallow INP parameterisation slope and consequently high ice particle production by the Hallett–Mossop process in our simulations leads to a sharp transition to a cloud with extensive glaciation at warm temperatures, higher cloud updraughts, enhanced vertical mass flux, and condensate divergence at the outflow level, all of which leads to a larger convectively generated anvil comprised of larger ice crystals. This work highlights the importance of quantifying the full spectrum of INP number concentrations across all mixed-phase altitudes and the ways in which INP and SIP interact to control anvil properties.

Two-year statistics of columnar-ice production in stratiform clouds over Hyytiälä, Finland: environmental conditions and the relevance to secondary ice production

Abstract. Formation of ice particles in clouds at temperatures of −10 ∘C or warmer was documented by using ground-based radar observations. At these temperatures, the number concentration of ice-nucleating particles (INPs) is not only expected to be small, but this number is also highly uncertain. In addition, there are a number of studies reporting that the observed number concentration of ice particles exceeds expected INP concentrations, indicating that other ice generation mechanisms, such as secondary ice production (SIP), may play an important role in such clouds. To identify formation of ice crystals and report conditions in which they are generated, W-band cloud radar Doppler spectra observations collected at the Hyytiälä station for more than 2 years were used. Given that at these temperatures ice crystals grow mainly as columns, which have distinct linear depolarization ratio (LDR) values, the spectral LDR was utilized to identify newly formed ice particles. It is found that in 5 %–13 % of clouds, where cloud top temperatures are −12 ∘C or warmer, production of columnar ice is detected. For colder clouds, this percentage can be as high as 33 %; 40 %–50 % of columnar-ice-producing events last less than 1 h, while 5 %–15 % can persist for more than 6 h. By comparing clouds where columnar crystals are produced and to the ones where these crystals are absent, the columnar-ice-producing clouds tend to have larger values of liquid water path and precipitation intensity. The columnar-ice-producing clouds were subdivided into three categories, using the temperature difference, ΔT, between the altitudes where columns are first detected and cloud top. The cases where ΔT is less than 2 K are typically single-layer shallow clouds where needles are produced at the cloud top. In multilayered clouds where 2 K < ΔT, columns are produced in a layer that is seeded by ice particles falling from above. This classification allows us to study potential impacts of various SIP mechanisms, such as the Hallet–Mossop process or freezing breakup, on columnar-ice production. To answer the question whether the observed ice particles are generated by SIP in the observed single-layer shallow clouds, ice particle number concentrations were retrieved and compared to several INP parameterizations. It was found that the ice number concentrations tend to be 1–3 orders of magnitude higher than the expected INP concentrations.

Aerosol–Ice Formation Closure: A Southern Great Plains Field Campaign

AbstractPrediction of ice formation in clouds presents one of the grand challenges in the atmospheric sciences. Immersion freezing initiated by ice-nucleating particles (INPs) is the dominant pathway of primary ice crystal formation in mixed-phase clouds, where supercooled water droplets and ice crystals coexist, with important implications for the hydrological cycle and climate. However, derivation of INP number concentrations from an ambient aerosol population in cloud-resolving and climate models remains highly uncertain. We conducted an aerosol–ice formation closure pilot study using a field-observational approach to evaluate the predictive capability of immersion freezing INPs. The closure study relies on collocated measurements of the ambient size-resolved and single-particle composition and INP number concentrations. The acquired particle data serve as input in several immersion freezing parameterizations, which are employed in cloud-resolving and climate models, for prediction of INP number concentrations. We discuss in detail one closure case study in which a front passed through the measurement site, resulting in a change of ambient particle and INP populations. We achieved closure in some circumstances within uncertainties, but we emphasize the need for freezing parameterization of potentially missing INP types and evaluation of the choice of parameterization to be employed. Overall, this closure pilot study aims to assess the level of parameter details and measurement strategies needed to achieve aerosol–ice formation closure. The closure approach is designed to accurately guide immersion freezing schemes in models, and ultimately identify the leading causes for climate model bias in INP predictions.

High Potential of Asian Dust to Act as Ice Nucleating Particles in Mixed‐Phase Clouds Simulated With a Global Aerosol‐Climate Model

AbstractMineral dust affects the microphysical and radiative properties of mixed‐phase clouds and hence the radiative balance of the Earth by acting as ice nucleating particles (INPs). However, the importance of Asian dust as INPs is not well understood. In this study, we examined the contribution of Asian dust to global dust INPs and its effect on cloud radiative forcing (CRF) using a global aerosol‐climate model with an ice nucleation parameterization that links INP number concentrations to ambient temperature and dust number concentrations. Our model well reproduces INP number concentrations measured over the Tokyo Metropolitan area in Japan during May 2017, when Asian dust was transported to Japan. Our simulation for the years 2013–2017 shows that Asian dust extends from its source regions (e.g., the Gobi and Taklimakan Deserts) to the North Pacific, North America, and the Arctic. Notably, Asian dust is transported to higher altitudes (i.e., to temperature regimes relevant for the formation of mixed‐phase clouds) more efficiently than dust from other regions. The annual‐mean simulated contribution of Asian dust to global dust INPs is 15%, which is 4.4 times higher than its contribution to global atmospheric dust loading (3.4%). These characteristics of Asian dust show its high potential to act as INPs in mixed‐phase clouds. Sensitivity simulations show that Asian dust INPs have a positive net CRF of 0.054–0.19 W m−2 in East Asia and the North Pacific during 2013–2017 (cf. 0.092–1.0 W m−2 for dust from other regions).

Characterization of aerosol particles at Cabo Verde close to sea level and at the cloud level – Part 2: Ice-nucleating particles in air, cloud and seawater

Abstract. Ice-nucleating particles (INPs) in the troposphere can form ice in clouds via heterogeneous ice nucleation. Yet, atmospheric number concentrations of INPs (NINP) are not well characterized, and, although there is some understanding of their sources, it is still unclear to what extend different sources contribute or if all sources are known. In this work, we examined properties of INPs at Cabo Verde (a.k.a. Cape Verde) from different environmental compartments: the oceanic sea surface microlayer (SML), underlying water (ULW), cloud water and the atmosphere close to both sea level and cloud level. Both enrichment and depletion of NINP in SML compared to ULW were observed. The enrichment factor (EF) varied from roughly 0.4 to 11, and there was no clear trend in EF with ice-nucleation temperature. NINP values in PM10 sampled at Cape Verde Atmospheric Observatory (CVAO) at any particular ice-nucleation temperature spanned around 1 order of magnitude below −15 ∘C, and about 2 orders of magnitude at warmer temperatures (>-12 ∘C). Among the 17 PM10 samples at CVAO, three PM10 filters showed elevated NINP at warm temperatures, e.g., above 0.01 L−1 at −10 ∘C. After heating samples at 95 ∘C for 1 h, the elevated NINP at the warm temperatures disappeared, indicating that these highly ice active INPs were most likely biological particles. INP number concentrations in PM1 were generally lower than those in PM10 at CVAO. About 83±22 %, 67±18 % and 77±14 % (median±standard deviation) of INPs had a diameter >1 µm at ice-nucleation temperatures of −12, −15 and −18 ∘C, respectively. PM1 at CVAO did not show such elevated NINP at warm temperatures. Consequently, the difference in NINP between PM1 and PM10 at CVAO suggests that biological ice-active particles were present in the supermicron size range. NINP in PM10 at CVAO was found to be similar to that on Monte Verde (MV, at 744 m a.s.l.) during noncloud events. During cloud events, most INPs on MV were activated to cloud droplets. When highly ice active particles were present in PM10 filters at CVAO, they were not observed in PM10 filters on MV but in cloud water samples instead. This is direct evidence that these INPs, which are likely biological, are activated to cloud droplets during cloud events. For the observed air masses, atmospheric NINP values in air fit well to the concentrations observed in cloud water. When comparing concentrations of both sea salt and INPs in both seawater and PM10 filters, it can be concluded that sea spray aerosol (SSA) only contributed a minor fraction to the atmospheric NINP. This latter conclusion still holds when accounting for an enrichment of organic carbon in supermicron particles during sea spray generation as reported in literature.

Observations of Ice Nucleating Particles Over Southern Ocean Waters

AbstractA likely important feature of the poorly understood aerosol‐cloud interactions over the Southern Ocean (SO) is the dominant role of sea spray aerosol, versus terrestrial aerosol. Ice nucleating particles (INPs), or particles required for heterogeneous ice nucleation, present over the SO have not been studied in several decades. In this study, boundary layer aerosol properties and immersion freezing INP number concentrations (nINPs) were measured during a ship campaign that occurred south of Australia (down to 53°S) in March–April 2016. Ocean surface chlorophyll a concentrations ranged from 0.11 to 1.77 mg/m3, and nINPs were a factor of 100 lower than historical surveys, ranging from 0.38 to 4.6 m−3 at −20 °C. The INP population included organic heat‐stable material, with contributions from heat‐labile material. Lower INP source potentials of SO seawater samples compared to Arctic seawater were consistent with lower ice nucleating site densities in this study compared to north Atlantic air masses.

Background Free‐Tropospheric Ice Nucleating Particle Concentrations at Mixed‐Phase Cloud Conditions

AbstractClouds 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.

Ice-nucleating particle concentrations unaffected by urban air pollution in Beijing, China

Abstract. Exceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated whether anthropogenic PM2.5 may significantly contribute to ice-nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (NINP) in the range from −6 to −25 ∘C in Beijing. No correlations between NINP and either PM2.5 or black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and either total particle number concentration or number concentrations for particles with diameters >500 nm. Furthermore, there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range.

Comparative measurements of ambient atmospheric concentrations of ice nucleating particles using multiple immersion freezing methods and a continuous flow diffusion chamber

Abstract. A number of new measurement methods for ice nucleating particles (INPs) have been introduced in recent years, and it is important to address how these methods compare. Laboratory comparisons of instruments sampling major INP types are common, but few comparisons have occurred for ambient aerosol measurements exploring the utility, consistency and complementarity of different methods to cover the large dynamic range of INP concentrations that exists in the atmosphere. In this study, we assess the comparability of four offline immersion freezing measurement methods (Colorado State University ice spectrometer, IS; North Carolina State University cold stage, CS; National Institute for Polar Research Cryogenic Refrigerator Applied to Freezing Test, CRAFT; University of British Columbia micro-orifice uniform deposit impactor–droplet freezing technique, MOUDI-DFT) and an online method (continuous flow diffusion chamber, CFDC) used in a manner deemed to promote/maximize immersion freezing, for the detection of INPs in ambient aerosols at different locations and in different sampling scenarios. We also investigated the comparability of different aerosol collection methods used with offline immersion freezing instruments. Excellent agreement between all methods could be obtained for several cases of co-sampling with perfect temporal overlap. Even for sampling periods that were not fully equivalent, the deviations between atmospheric INP number concentrations measured with different methods were mostly less than 1 order of magnitude. In some cases, however, the deviations were larger and not explicable without sampling and measurement artifacts. Overall, the immersion freezing methods seem to effectively capture INPs that activate as single particles in the modestly supercooled temperature regime (> −20 °C), although more comparisons are needed in this temperature regime that is difficult to access with online methods. Relative to the CFDC method, three immersion freezing methods that disperse particles into a bulk liquid (IS, CS, CRAFT) exhibit a positive bias in measured INP number concentrations below −20 °C, increasing with decreasing temperature. This bias was present but much less pronounced for a method that condenses separate water droplets onto limited numbers of particles prior to cooling and freezing (MOUDI-DFT). Potential reasons for the observed differences are discussed, and further investigations proposed to elucidate the role of all factors involved.

On the role of ice-nucleating aerosol in the formation of ice particles in tropical mesoscale convective systems.

Over decades, the cloud physics community has debated the nature and role of aerosol particles in ice initiation. The present study shows that the measured concentration of ice crystals in tropical mesoscale convective systems exceeds the concentration of ice nucleating particles (INPs) by several orders of magnitude. The concentration of INPs was assessed from the measured aerosol particles concentration in the size range of 0.5 to 1 µm. The observations from this study suggest that primary ice crystals formed on INPs make only a minor contribution to the total concentration of ice crystals in tropical mesoscale convective systems. This is found by comparing the predicted INP number concentrations with in-situ ice particle number concentrations. The obtained measurements suggest that ice multiplication is the likely explanation for the observed high concentrations of ice crystals in this type of convective system.

Size-resolved measurements of ice-nucleating particles at six locations in North America and one in Europe

Abstract. Detailed information on the size of ice-nucleating particles (INPs) may be useful in source identification, modeling their transport in the atmosphere to improve climate predictions, and determining how effectively or ineffectively instrumentation used for quantifying INPs in the atmosphere captures the full INP population. In this study we report immersion-mode INP number concentrations as a function of size at six ground sites in North America and one in Europe using the micro-orifice uniform-deposit impactor droplet freezing technique (MOUDI-DFT), which combines particle size-segregation by inertial impaction and a microscope-based immersion freezing apparatus. The lowest INP number concentrations were observed at Arctic and alpine locations and the highest at suburban and agricultural locations, consistent with previous studies of INP concentrations in similar environments. We found that 91 ± 9, 79 ± 17, and 63 ± 21 % of INPs had an aerodynamic diameter > 1 µm at ice activation temperatures of −15, −20, and −25 °C, respectively, when averaging over all sampling locations. In addition, 62 ± 20, 55 ± 18, and 42 ± 17 % of INPs were in the coarse mode (> 2.5 µm) at ice activation temperatures of −15, −20, and −25 °C, respectively, when averaging over all sampling locations. These results are consistent with six out of the nine studies in the literature that have focused on the size distribution of INPs in the atmosphere. Taken together, these findings strongly suggest that supermicron and coarse-mode aerosol particles are a significant component of the INP population in many different ground-level environments. Further size-resolved studies of INPs as a function of altitude are required since the size distribution of INPs may be different at high altitudes due to size-dependent removal processes of atmospheric particles.

Sea spray aerosol as a unique source of ice nucleating particles

Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using “dry” geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean.

Ice nucleating particles at a coastal marine boundary layer site: correlations with aerosol type and meteorological conditions

Abstract. Information on what aerosol particle types are the major sources of ice nucleating particles (INPs) in the atmosphere is needed for climate predictions. To determine which aerosol particles are the major sources of immersion-mode INPs at a coastal site in Western Canada, we investigated correlations between INP number concentrations and both concentrations of different atmospheric particles and meteorological conditions. We show that INP number concentrations are strongly correlated with the number concentrations of fluorescent bioparticles between −15 and −25 °C, and that the size distribution of INPs is most consistent with the size distribution of fluorescent bioparticles. We conclude that biological particles were likely the major source of ice nuclei at freezing temperatures between −15 and −25 °C at this site for the time period studied. At −30 °C, INP number concentrations are also well correlated with number concentrations of the total aerosol particles ≥ 0.5 μm, suggesting that non-biological particles may have an important contribution to the population of INPs active at this temperature. As we found that black carbon particles were unlikely to be a major source of ice nuclei during this study, these non-biological INPs may include mineral dust. Furthermore, correlations involving chemical tracers of marine aerosols and marine biological activity, sodium and methanesulfonic acid, indicate that the majority of INPs measured at the coastal site likely originated from terrestrial rather than marine sources. Finally, six existing empirical parameterizations of ice nucleation were tested to determine if they accurately predict the measured INP number concentrations. We found that none of the parameterizations selected are capable of predicting INP number concentrations with high accuracy over the entire temperature range investigated. This finding illustrates that additional measurements are needed to improve parameterizations of INPs and their subsequent climatic impacts.