scholarly journals Sources and nature of ice-nucleating particles in the free troposphere at Jungfraujoch in winter 2017

2021 ◽  
Vol 21 (22) ◽  
pp. 16925-16953
Author(s):  
Larissa Lacher ◽  
Hans-Christian Clemen ◽  
Xiaoli Shen ◽  
Stephan Mertes ◽  
Martin Gysel-Beer ◽  
...  
Keyword(s):  
Time Series ◽  
Laser Ablation ◽  
Source Region ◽  
Mixed Phase ◽  
Dust Particles ◽  
Sea Spray ◽  
Free Troposphere ◽  
Mass Spectrometers ◽  
Air Masses ◽  
Mixed Phase Clouds

Abstract. Primary ice formation in mixed-phase clouds is initiated by a minute subset of the ambient aerosol population, called ice-nucleating particles (INPs). The knowledge about their atmospheric concentration, composition, and source in cloud-relevant environments is still limited. During the 2017 joint INUIT/CLACE (Ice Nuclei research UnIT/CLoud–Aerosol Characterization Experiment) field campaign, observations of INPs as well as of aerosol physical and chemical properties were performed, complemented by source region modeling. This aimed at investigating the nature and sources of INPs. The campaign took place at the High-Altitude Research Station Jungfraujoch (JFJ), a location where mixed-phase clouds frequently occur. Due to its altitude of 3580 m a.s.l., the station is usually located in the lower free troposphere, but it can also receive air masses from terrestrial and marine sources via long-range transport. INP concentrations were quasi-continuously detected with the Horizontal Ice Nucleation Chamber (HINC) under conditions representing the formation of mixed-phase clouds at −31 ∘C. The INP measurements were performed in parallel to aerosol measurements from two single-particle mass spectrometers, the Aircraft-based Laser ABlation Aerosol MAss Spectrometer (ALABAMA) and the laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF). The chemical identity of INPs is inferred by correlating the time series of ion signals measured by the mass spectrometers with the time series of INP measurements. Moreover, our results are complemented by the direct analysis of ice particle residuals (IPRs) by using an ice-selective inlet (Ice-CVI) coupled with the ALABAMA. Mineral dust particles and aged sea spray particles showed the highest correlations with the INP time series. Their role as INPs is further supported by source emission sensitivity analysis using atmospheric transport modeling, which confirmed that air masses were advected from the Sahara and marine environments during times of elevated INP concentrations and ice-active surface site densities. Indeed, the IPR analysis showed that, by number, mineral dust particles dominated the IPR composition (∼58 %), and biological and metallic particles are also found to a smaller extent (∼10 % each). Sea spray particles are also found as IPRs (17 %), and their fraction in the IPRs strongly varied according to the increased presence of small IPRs, which is likely due to an impact from secondary ice crystal formation. This study shows the capability of combining INP concentration measurements with chemical characterization of aerosol particles using single-particle mass spectrometry, source region modeling, and analysis of ice residuals in an environment directly relevant for mixed-phase cloud formation.

scholarly journals Sources and nature of ice-nucleating particles in the free troposphere at Jungfraujoch in winter 2017

2021 ◽  
Author(s):  
Larissa Lacher ◽  
Hans-Christian Clemen ◽  
Xiaoli Shen ◽  
Stephan Mertes ◽  
Martin Gysel-Beer ◽  
...  
Keyword(s):  
Time Series ◽  
Laser Ablation ◽  
Source Region ◽  
Mixed Phase ◽  
Dust Particles ◽  
Sea Spray ◽  
Free Troposphere ◽  
Mass Spectrometers ◽  
Air Masses ◽  
Mixed Phase Clouds

Abstract. Primary ice formation in mixed-phase clouds is initiated by a minute subset of the ambient aerosol population, called ice-nucleating particles (INPs). The knowledge about their atmospheric concentration, their composition, and source in cloud-relevant environments is still limited. During the joint INUIT/CLACE (Ice Nuclei research UnIT/ CLoud–Aerosol Characterization Experiment) 2017 field campaign, observations of INPs, as well as of aerosol physical and chemical properties were performed, complemented by source region modelling. This aimed at investigating the nature and sources of INPs. The campaign took place at the High-Altitude Research Station Jungfraujoch (JFJ), a location where mixed-phase clouds frequently occur. Due to its altitude of 3580 m a.s.l., the station is usually located in the lower free troposphere, but can also receive air masses from terrestrial and marine sources via long-range transport. INP concentrations were quasi-continuously detected with the Horizontal Ice Nucleation Chamber (HINC) under conditions representing the formation of mixed-phase clouds at −31 °C. The INP measurements were performed in parallel to aerosol measurements from two single particle mass spectrometers, the Aircraft-based Laser ABlation Aerosol MAss Spectrometer (ALABAMA) and the Laser Ablation Aerosol Particle Time-Of-Flight mass spectrometer (LAAPTOF). The chemical identity of INPs is inferred by correlating the time series of ion signals measured by the mass spectrometers with the time series of INP measurements. Moreover, our results are complemented by the direct analysis of ice particle residuals (IPRs) by using an ice-selective inlet (Ice-CVI) coupled with the ALABAMA. Mineral dust particles and aged sea spray particles showed the highest correlations with the INP time series. Their role as INP is further supported by source emission sensitivity analysis using atmospheric transport modelling, which confirmed that air masses were advected from the Saharan desert and marine environments during times of elevated INP concentrations and ice-active surface site densities. Indeed, the IPR analysis showed that by number, mineral dust particles dominated the IPR composition (~58 %), and also biological and metallic particles are found to a smaller extent (~10 %). Sea spray particles are also found as IPRs (17 %), and their fraction in the IPRs strongly varied according to the increased presence of small IPRs, which is likely due to an impact from secondary ice crystal formation. This study shows the capability of combining INP concentration measurements with chemical characterization of aerosol particles using single particle mass spectrometry, source region modelling, and analysis of ice-residuals in an environment directly relevant for mixed-phase cloud formation.

The ice nucleating ability of macromolecules in immersion freezing decreases in the presence of salts: Implications for freezing point depression calculations

2021 ◽  
Author(s):  
Jon F. Went ◽  
Jeanette D. Wheeler ◽  
François J. Peaudecerf ◽  
Nadine Borduas-Dedekind
Keyword(s):  
Sea Water ◽  
Freezing Point ◽  
Pure Water ◽  
Salt Content ◽  
Mixed Phase ◽  
Cloud Formation ◽  
Sea Spray ◽  
Freezing Point Depression ◽  
Immersion Freezing ◽  
Mixed Phase Clouds

<p>Cloud formation represents a large uncertainty in current climate predictions. In particular, ice in mixed-phase clouds requires the presence of ice nucleating particles (INPs) or ice nucleating macromolecules (INMs). An influential population of INPs has been proposed to be organic sea spray aerosols in otherwise pristine ocean air. However, the interactions between INMs present in sea water and their freezing behavior under atmospheric immersion freezing conditions warrants further research to constrain the role of sea spray aerosols on cloud formation. Indeed, salt is known to lower the freezing temperature of water, through a process called freezing point depression (FPD). Yet, current FPD corrections are solely based on the salt content and assume that the INMs’ ice nucleation abilities are identical with and without salt. Thus, we measured the effect of salt content on the ice nucleating ability of INMs, known to be associated with marine phytoplankton, in immersion freezing experiments in the Freezing Ice Nuclei Counter (FINC) (Miller et al., AMTD, 2020). We measured eight INMs, namely taurine, isethionate, xylose, mannitol, dextran, laminarin, and xanthan as INMs in pure water at temperatures relevant for mixed-phase clouds (e.g. 50% activated fraction at temperatures above –23 °C at 10 mM concentration). Subsequently, INMs were analyzed in artificial sea water containing 36 g salt L<sup>-1</sup>. Most INMs, except laminarin and xanthan, showed a loss of ice activity in artificial sea water compared to pure water, even after FPD correction. Based on our results, we hypothesize sea salt has an inhibitory effect on the ice activity of INMs. This effect influences our understanding of how INMs nucleate ice as well as challenges our use of FPD correction and subsequent extrapolation to ice activity under mixed-phase cloud conditions.</p>

scholarly journals The efficiency of secondary organic aerosol particles to act as ice nucleating particles at mixed-phase cloud conditions

2018 ◽  
Author(s):  
Wiebke Frey ◽  
Dawei Hu ◽  
James Dorsey ◽  
M. Rami Alfarra ◽  
Aki Pajunoja ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Aerosol Particles ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Dust Particles ◽  
Ice Cloud ◽  
Liquid Saturation ◽  
Reference Experiment ◽  
Mixed Phase Clouds

Abstract. Secondary Organic Aerosol (SOA) particles have been found to be efficient ice nucleating particles under the cold conditions of (tropical) upper tropospheric cirrus clouds. Whether they also are efficient at initiating freezing at slightly warmer conditions as found in mixed phase clouds remains undetermined. Here, we study the ice nucleating ability of photo-chemically produced SOA particles with the combination of the Manchester Aerosol and Ice Cloud Chambers. Three SOA systems were tested resembling biogenic/anthropogenic particles and particles of different phase state. After the aerosol particles were formed, they were transferred into the cloud chamber where subsequent quasi-adiabatic cloud evacuations were performed. Additionally, the ice forming abilities of ammonium sulfate and kaolinite were investigated as a reference to test the experimental setup. Clouds were formed in the temperature range of −20 °C to −28.6 °C. Only the reference experiment using dust particles showed evidence of ice nucleation. No ice particles were observed in any other experiment. Thus, we conclude that SOA particles produced under the conditions of the reported experiments are not efficient ice nucleating particles starting at liquid saturation under mixed-phase cloud conditions.

scholarly journals The potential influence of Asian and African mineral dust on ice, mixed-phase and liquid water clouds

2010 ◽  
Vol 10 (2) ◽  
pp. 4027-4077 ◽  
Author(s):  
A. Wiacek ◽  
T. Peter ◽  
U. Lohmann
Keyword(s):  
Liquid Water ◽  
Mineral Dust ◽  
Dust Emission ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Specific Humidity ◽  
Dust Particles ◽  
Ice Clouds ◽  
Cloud Processing ◽  
Mixed Phase Clouds

Abstract. This modelling study explores the availability of mineral dust particles as ice nuclei for interactions with ice, mixed-phase and liquid water clouds, also tracking the particles' history of cloud-processing. We performed 61 320 one-week forward trajectory calculations originating near the surface of major dust emitting regions in Africa and Asia using high-resolution meteorological analysis fields for the year 2007. Without explicitly modelling dust emission and deposition processes, dust-bearing trajectories were assumed to be those coinciding with known dust emission seasons. We found that dust emissions from Asian deserts lead to a higher potential for interactions with high clouds, despite being the climatologically much smaller dust emission source. This is due to Asian regions experiencing significantly more ascent than African regions, with strongest ascent in the Asian Taklimakan desert at ~25%, ~40% and 10% of trajectories ascending to 300 hPa in spring, summer and fall, respectively. The specific humidity at each trajectory's starting point was transported in a Lagrangian manner and relative humidities with respect to water and ice were calculated in 6-h steps downstream, allowing us to estimate the formation of liquid, mixed-phase and ice clouds. Practically none of the simulated air parcels reached regions where homogeneous ice nucleation can take place (T≲−40 °C) along trajectories that have not experienced water saturation first. By far the largest fraction of cloud forming trajectories entered conditions of mixed-phase clouds, where mineral dust will potentially exert the biggest influence. The majority of trajectories also passed through regions supersaturated with respect to ice but subsaturated with respect to water, where "warm" (T≳−40 °C) ice clouds may form prior to supercooled water or mixed-phase clouds. The importance of "warm" ice clouds and the general influence of dust in the mixed-phase cloud region are highly uncertain due to considerable scatter in recent laboratory data from ice nucleation experiments, which we briefly review in this work. For "classical" cirrus-forming temperatures, our results show that only mineral dust IN that underwent mixed-phase cloud-processing previously are likely to be relevant, and, therefore, we recommend further systematic studies of immersion mode ice nucleation on mineral dust suspended in atmospherically relevant coatings.

scholarly journals Ice nucleation by combustion ash particles at conditions relevant to mixed-phase clouds

2014 ◽  
Vol 14 (21) ◽  
pp. 28845-28883
Author(s):  
N. S. Umo ◽  
B. J. Murray ◽  
M. T. Baeza-Romero ◽  
J. M. Jones ◽  
A. R. Lea-Langton ◽  
...  
Keyword(s):  
Hydrological Cycle ◽  
Coal Fly Ash ◽  
Aerosol Particles ◽  
Bottom Ash ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Dust Particles ◽  
Cloud Properties ◽  
Mixed Phase Clouds ◽  
The Impact

Abstract. Ice nucleating particles can modify cloud properties with implications for climate and the hydrological cycle; hence, it is important to understand which aerosol particle types nucleate ice and how efficiently they do so. It has been shown that aerosol particles such as natural dusts, volcanic ash, bacteria and pollen can act as ice nucleating particles, but the ice nucleating ability of combustion ashes has not been studied. Combustion ashes are major by-products released during the combustion of solid fuels and a significant amount of these ashes are emitted into the atmosphere either during combustion or via aerosolization of bottom ashes. Here, we show that combustion ashes (coal fly ash, wood bottom ash, domestic bottom ash, and coal bottom ash) nucleate ice in the immersion mode at conditions relevant to mixed-phase clouds. Hence, combustion ashes could play an important role in primary ice formation in mixed-phase clouds, especially in clouds that are formed near the emission source of these aerosol particles. In order to quantitatively assess the impact of combustion ashes on mixed-phase clouds, we propose that the atmospheric abundance of combustion ashes should be quantified since up to now they have mostly been classified together with mineral dust particles. Also, in reporting ice residue compositions, a distinction should be made between natural mineral dusts and combustion ashes in order to quantify the contribution of combustion ashes to atmospheric ice nucleation.

scholarly journals Toward Improved Cloud-Phase Simulation with a Mineral Dust and Temperature-Dependent Parameterization for Ice Nucleation in Mixed-Phase Clouds

2019 ◽  
Vol 76 (11) ◽  
pp. 3655-3667
Author(s):  
Songmiao Fan ◽  
Paul Ginoux ◽  
Charles J. Seman ◽  
Levi G. Silvers ◽  
Ming Zhao
Keyword(s):  
Mineral Dust ◽  
Supercooled Liquid ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Dust Particles ◽  
Geophysical Fluid Dynamics Laboratory ◽  
Temperature Dependent ◽  
Model Simulations ◽  
Cloud Properties ◽  
Mixed Phase Clouds

Abstract Mixed-phase clouds are frequently observed in the atmosphere. Here we present a parameterization for ice crystal concentration and ice nucleation rate based on parcel model simulations for mixed-phase stratocumulus clouds, as a complement to a previous parameterization for stratus clouds. The parcel model uses a singular (time independent) description for deposition nucleation and a time-dependent description for condensation nucleation and immersion freezing on mineral dust particles. The mineral dust and temperature-dependent parameterizations have been implemented in the Geophysical Fluid Dynamics Laboratory atmosphere model, version 4.0 (AM4.0) (new), while the standard AM4.0 (original) uses a temperature-dependent parameterization. Model simulations with the new and original AM4.0 show significant changes in cloud properties and radiative effects. In comparison to measurements, cloud-phase (i.e., liquid and ice partitioning) simulation appears to be improved in the new AM4.0. More supercooled liquid cloud is predicted in the new model, it is sustained even at temperatures lower than −25°C unlike in the original model. A more accurate accounting of ice nucleating particles and ice crystals is essential for improved cloud-phase simulation in the global atmosphere.

scholarly journals Implementation of a comprehensive ice crystal formation parameterization for cirrus and mixed-phase clouds in the EMAC model (based on MESSy 2.53)

2018 ◽  
Vol 11 (10) ◽  
pp. 4021-4041 ◽  
Author(s):  
Sara Bacer ◽  
Sylvia C. Sullivan ◽  
Vlassis A. Karydis ◽  
Donifan Barahona ◽  
Martina Krämer ◽  
...  
Keyword(s):  
Climate Model ◽  
Ice Nucleation ◽  
Cirrus Clouds ◽  
Mixed Phase ◽  
Ice Crystals ◽  
Dust Particles ◽  
Crystal Formation ◽  
Ice Crystal ◽  
Upper Troposphere ◽  
Mixed Phase Clouds

Abstract. A comprehensive ice nucleation parameterization has been implemented in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations (ICNCs). The parameterization of Barahona and Nenes (2009, hereafter BN09) allows for the treatment of ice nucleation taking into account the competition for water vapour between homogeneous and heterogeneous nucleation in cirrus clouds. Furthermore, the influence of chemically heterogeneous, polydisperse aerosols is considered by applying one of the multiple ice nucleating particle parameterizations which are included in BN09 to compute the heterogeneously formed ice crystals. BN09 has been modified in order to consider the pre-existing ice crystal effect and implemented to operate both in the cirrus and in the mixed-phase regimes. Compared to the standard EMAC parameterizations, BN09 produces fewer ice crystals in the upper troposphere but higher ICNCs in the middle troposphere, especially in the Northern Hemisphere where ice nucleating mineral dust particles are relatively abundant. Overall, ICNCs agree well with the observations, especially in cold cirrus clouds (at temperatures below 205 K), although they are underestimated between 200 and 220 K. As BN09 takes into account processes which were previously neglected by the standard version of the model, it is recommended for future EMAC simulations.

scholarly journals Effects of marine organic aerosols as sources of immersion-mode ice-nucleating particles on high-latitude mixed-phase clouds

2021 ◽  
Vol 21 (4) ◽  
pp. 2305-2327
Author(s):  
Xi Zhao ◽  
Xiaohong Liu ◽  
Susannah M. Burrows ◽  
Yang Shi
Keyword(s):  
Southern Ocean ◽  
High Latitude ◽  
Ice Nucleation ◽  
Surface Energy Budget ◽  
Mixed Phase ◽  
Sea Spray ◽  
Earth System ◽  
Cloud Forcing ◽  
Model Version ◽  
Mixed Phase Clouds

Abstract. Mixed-phase clouds are frequently observed in high-latitude regions and have important impacts on the surface energy budget and regional climate. Marine organic aerosol (MOA), a natural source of aerosol emitted over ∼ 70 % of Earth's surface, may significantly modify the properties and radiative forcing of mixed-phase clouds. However, the relative importance of MOA as a source of ice-nucleating particles (INPs) in comparison to mineral dust, and MOA's effects as cloud condensation nuclei (CCN) and INPs on mixed-phase clouds are still open questions. In this study, we implement MOA as a new aerosol species into the Community Atmosphere Model version 6 (CAM6), the atmosphere component of the Community Earth System Model version 2 (CESM2), and allow the treatment of aerosol–cloud interactions of MOA via droplet activation and ice nucleation. CAM6 reproduces observed seasonal cycles of marine organic matter at Mace Head and Amsterdam Island when the MOA fraction of sea spray aerosol in the model is assumed to depend on sea spray biology but fails when this fraction is assumed to be constant. Model results indicate that marine INPs dominate primary ice nucleation below 400 hPa over the Southern Ocean and Arctic boundary layer, while dust INPs are more abundant elsewhere. By acting as CCN, MOA exerts a shortwave cloud forcing change of −2.78 W m−2 over the Southern Ocean in the austral summer. By acting as INPs, MOA enhances the longwave cloud forcing by 0.35 W m−2 over the Southern Ocean in the austral winter. The annual global mean net cloud forcing changes due to CCN and INPs of MOA are −0.35 and 0.016 W m−2, respectively. These findings highlight the vital importance for Earth system models to consider MOA as an important aerosol species for the interactions of biogeochemistry, hydrological cycle, and climate change.

scholarly journals Ice nucleation by combustion ash particles at conditions relevant to mixed-phase clouds

2015 ◽  
Vol 15 (9) ◽  
pp. 5195-5210 ◽  
Author(s):  
N. S. Umo ◽  
B. J. Murray ◽  
M. T. Baeza-Romero ◽  
J. M. Jones ◽  
A. R. Lea-Langton ◽  
...  
Keyword(s):  
Hydrological Cycle ◽  
Coal Fly Ash ◽  
Aerosol Particles ◽  
Bottom Ash ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Dust Particles ◽  
Cloud Properties ◽  
Mixed Phase Clouds ◽  
The Impact

Abstract. Ice-nucleating particles can modify cloud properties with implications for climate and the hydrological cycle; hence, it is important to understand which aerosol particle types nucleate ice and how efficiently they do so. It has been shown that aerosol particles such as natural dusts, volcanic ash, bacteria and pollen can act as ice-nucleating particles, but the ice-nucleating ability of combustion ashes has not been studied. Combustion ashes are major by-products released during the combustion of solid fuels and a significant amount of these ashes are emitted into the atmosphere either during combustion or via aerosolization of bottom ashes. Here, we show that combustion ashes (coal fly ash, wood bottom ash, domestic bottom ash, and coal bottom ash) nucleate ice in the immersion mode at conditions relevant to mixed-phase clouds. Hence, combustion ashes could play an important role in primary ice formation in mixed-phase clouds, especially in clouds that are formed near the emission source of these aerosol particles. In order to quantitatively assess the impact of combustion ashes on mixed-phase clouds, we propose that the atmospheric abundance of combustion ashes should be quantified since up to now they have mostly been classified together with mineral dust particles. Also, in reporting ice residue compositions, a distinction should be made between natural mineral dusts and combustion ashes in order to quantify the contribution of combustion ashes to atmospheric ice nucleation.

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