scholarly journals The effect of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> on the freezing properties of non-mineral dust ice-nucleating substances of atmospheric relevance

2021 ◽  
Vol 21 (19) ◽  
pp. 14631-14648
Author(s):  
Soleil E. Worthy ◽  
Anand Kumar ◽  
Yu Xi ◽  
Jingwei Yun ◽  
Jessie Chen ◽  
...  

Abstract. A wide range of materials including mineral dust, soil dust, and bioaerosols have been shown to act as ice nuclei in the atmosphere. During atmospheric transport, these materials can become coated with inorganic and organic solutes which may impact their ability to nucleate ice. While a number of studies have investigated the impact of solutes at low concentrations on ice nucleation by mineral dusts, very few studies have examined their impact on non-mineral dust ice nuclei. We studied the effect of dilute (NH4)2SO4 solutions (0.05 M) on immersion freezing of a variety of non-mineral dust ice-nucleating substances (INSs) including bacteria, fungi, sea ice diatom exudates, sea surface microlayer substances, and humic substances using the droplet-freezing technique. We also studied the effect of (NH4)2SO4 solutions (0.05 M) on the immersion freezing of several types of mineral dust particles for comparison purposes. (NH4)2SO4 had no effect on the median freezing temperature (ΔT50) of 9 of the 10 non-mineral dust materials tested. There was a small but statistically significant decrease in ΔT50 (−0.43 ± 0.19 ∘C) for the bacteria Xanthomonas campestris in the presence of (NH4)2SO4 compared to pure water. Conversely, (NH4)2SO4 increased the median freezing temperature of four different mineral dusts (potassium-rich feldspar, Arizona Test Dust, kaolinite, montmorillonite) by 3 to 9 ∘C and increased the ice nucleation active site density per gram of material (nm(T)) by a factor of ∼ 10 to ∼ 30. This significant difference in the response of mineral dust and non-mineral dust ice-nucleating substances when exposed to (NH4)2SO4 suggests that they nucleate ice and/or interact with (NH4)2SO4 via different mechanisms. This difference suggests that the relative importance of mineral dust to non-mineral dust particles for ice nucleation in mixed-phase clouds could potentially increase as these particles become coated with (NH4)2SO4 in the atmosphere. This difference also suggests that the addition of (NH4)2SO4 (0.05 M) to atmospheric samples of unknown composition could potentially be used as an indicator or assay for the presence of mineral dust ice nuclei, although additional studies are still needed as a function of INS concentration to confirm the same trends are observed for different INS concentrations than those used here. A comparison with results in the literature does suggest that our results may be applicable to a range of mineral dust and non-mineral dust INS concentrations.

2021 ◽  
Author(s):  
Soleil E. Worthy ◽  
Anand Kumar ◽  
Yu Xi ◽  
Jingwei Yun ◽  
Jessie Chen ◽  
...  

Abstract. A wide range of materials including mineral dust, soil dust, and bioaerosols have been shown to act as ice nuclei in the atmosphere. During atmospheric transport, these materials can become coated with inorganic and organic solutes which may impact their ability to nucleate ice. While a number of studies have investigated the impact of solutes at low concentrations on ice nucleation by mineral dusts, very few studies have examined their impact on non-mineral dust ice nuclei. We studied the effect of dilute (NH4)2SO4 solutions on immersion freezing of a variety of non-mineral dust ice nucleating substances including bacteria, fungi, sea ice diatom exudates, sea surface microlayer, and humic substances using the droplet freezing technique. We also studied the effect of (NH4)2SO4 on immersion freezing of mineral dust particles for comparison purposes. (NH4)2SO4 had no effect on the median freezing temperature of nine of the ten tested non-mineral dust materials. There was a small but statistically significant decrease in the median freezing temperature of the bacteria X. campestris (change in median freezing temperature ∆T_50 = -0.43 ± 0.19 °C) in the presence of (NH4)2SO4 compared to pure water. Conversely, (NH4)2SO4 increased the median freezing temperature of four different mineral dusts (Potassium-rich feldspar, Arizona Test Dust, Kaolinite, Montmorillonite) by 3 °C to 8 °C. This significant difference in the response of mineral dust and non-mineral dust ice nucleating substances when exposed to (NH4)2SO4 suggests that they nucleate ice and/or interact with (NH4)2SO4 via different mechanisms. This difference suggests that the relative importance of mineral dust to non-mineral dust particles for ice nucleation in mixed-phase clouds could increase as these particles become coated with ammonium sulfate in the atmosphere. This difference also suggests that the addition of (NH4)2SO4 to atmospheric samples of unknown composition could be used as an indicator or assay for the presence of mineral dust ice nuclei.


2009 ◽  
Vol 9 (18) ◽  
pp. 6705-6715 ◽  
Author(s):  
A. Welti ◽  
F. Lüönd ◽  
O. Stetzer ◽  
U. Lohmann

Abstract. The recently developed Zurich Ice Nucleation Chamber (ZINC) was used to explore ice nucleation of size-selected mineral dust particles at temperatures between −20°C and −55°C. Four different mineral dust species have been tested: montmorillonite, kaolinite, illite and Arizona test dust (ATD). The selected particle diameters are 100 nm, 200 nm, 400 nm and 800 nm. Relative humidities with respect to ice (RHi) required to activate 1% of the dust particles as ice nuclei (IN) are reported as a function of temperature. An explicit size dependence of the ice formation efficiency has been observed for all dust types. 800 nm particles required the lowest RHi to activate. Deposition nucleation below water saturation was found only below −30°C or −35°C dependent on particle size. Minimum RHi for 1% activation were 105% for illite, kaolinite and montmorillonite at −40°C, respectively 110% for ATD at −45°C. In addition, a possible parameterisation for the measured activation spectra is proposed, which could be used in modeling studies.


2019 ◽  
Vol 19 (7) ◽  
pp. 5091-5110 ◽  
Author(s):  
Zamin A. Kanji ◽  
Ryan C. Sullivan ◽  
Monika Niemand ◽  
Paul J. DeMott ◽  
Anthony J. Prenni ◽  
...  

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.


2018 ◽  
Author(s):  
Zamin A. Kanji ◽  
Ryan C. Sullivan ◽  
Monika Niemand ◽  
Paul J. DeMott ◽  
Anthony J. Prenni ◽  
...  

Abstract. Ice nucleation abilities of surface collected mineral dust particles from the Sahara (SD) and Asia (AD) are investigated for the temperature range 253–233 K and for supersaturated humidity 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 poly-disperse 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 (AF) 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 differences observed are mostly 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 poly-disperse aerosol measurements which may show variable composition with particle size. In the atmosphere, coatings with similar properties to that of the SOA tested here for a thickness up to 60 nm, the maximum thickness tested here, is not expected to impede or enhance the ice nucleation ability by immersion mode of mineral dust in the mixed-phase cloud regime.


2009 ◽  
Vol 9 (2) ◽  
pp. 6929-6955 ◽  
Author(s):  
A. Welti ◽  
F. Lüönd ◽  
O. Stetzer ◽  
U. Lohmann

Abstract. The recently developed Zurich Ice Nucleation Chamber (ZINC) was used to explore ice nucleation of size-selected mineral dust particles at temperatures between −20°C and −55°C. Four different mineral dust species have been tested: montmorillonite, kaolinite, illite and Arizona test dust (ATD). The selected particle diameters are 100 nm, 200 nm, 400 nm and 800 nm. Relative humidities with respect to ice (RHi) required to activate 1% of the dust particles as ice nuclei (IN) are reported as a function of temperature. An explicit size dependence of the ice formation efficiency has been observed for all dust types. Deposition nucleation was found only below −30°C or −35°C dependent on particle size. 800 nm particles required the lowest RHi to activate. Minimum RHi for 1% activation were 105% for illite, kaolinite and montmorillonite at −40°C, respectively 110% for ATD at −45°C. In addition, a possible parameterisation for the measured activation spectra is proposed, which could be used in modeling studies.


2020 ◽  
Author(s):  
Luka Ilić ◽  
Aleksandar Jovanović ◽  
Maja Kuzmanoski ◽  
Fabio Madonna ◽  
Marco Rosoldi ◽  
...  

&lt;p&gt;The Sahara Desert is the major source of mineral dust, which is a significant portion of atmospheric aerosol. Mineral dust particles play a role in radiative balance, with a direct effect and by influencing cloud formation and lifetime. They have been recognized as highly efficient ice nuclei, fostering the development of parameterizations for immersion and deposition freezing involving dust particles. Feldspar minerals have shown to be a significantly more efficient ice nucleating agents than other dust minerals which led to the development of a &amp;#8216;mineralogy sensitive&amp;#8217; immersion freezing parameterization. The investigation of the relative efficiency of quartz compared to feldspars for the immersion ice nucleation, based upon literature data and new experiments, led to the development of a new parameterization to be applied to mineral dust concentrations. Within numerical models, explicit simulation of mineral dust fractions enables the use of &amp;#8216;mineralogy sensitive&amp;#8217; immersion parameterizations.&lt;/p&gt;&lt;p&gt;The operational DREAM model calculates the number of ice nuclei,but does not take into consideration the mineral composition of dust. In this study, instead, we use DREAM model to simulate the atmospheric cycle of feldspar and quartz fractions of dust. Dust mineral composition is used to calculate ice nucleating particle concentrations based on mineral-specific immersion freezing parameterizations. A case study related to the observations of geometrical and microphysical characteristics of the clouds formed in the Mediterranean, in April 2016 is considered. We compare the model results with ice nucleating particle concentrations retrieved using lidar and radar ground-based remote sensing observations at Cyprus and Potenza. The analysis explores how the mineral composition of dust and the parameterization of its effects on ice initiation could further improve ice nucleation representation in numerical models.&lt;/p&gt;


2016 ◽  
Author(s):  
Claudia Marcolli ◽  
Baban Nagare ◽  
André Welti ◽  
Ulrike Lohmann

Abstract. AgI is one of the best investigated ice nuclei. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Theoretical and experimental studies over the last sixty years provide a complex picture of silver iodide as ice nucleating agent with conflicting and inconsistent results. This review compares experimental ice nucleation studies in order to analyse the factors that influence the ice nucleation ability of AgI. We have performed experiments to compare contact and immersion freezing by AgI. This is one of three papers that describe and analyse contact and immersion freezing experiments with AgI. In Nagare et al. (Nagare, B., Marcolli, C., Stetzer, O., and Lohmann, U.: Comparison of measured and calculated collision efficiencies at low temperatures, Atmos. Chem. Phys., 15, 13759–13776, doi:10.5194/acp-15-13759-2015, 2015) collision efficiencies based on contact freezing experiments with AgI are determined and compared with theoretical formulations. In a companion paper, contact freezing experiments are compared with immersion freezing experiments conducted with AgI, kaolinite, and ATD as ice nuclei. The following picture emerges from this analysis: The ice nucleation ability of AgI seems to be enhanced when the AgI particle is on the surface of a droplet, which is indeed the position that a particle takes when it can freely move in a droplet. Ice nucleation by particles with surfaces exposed to air, depends on water adsorption. AgI surfaces seem to be most efficient as ice nuclei when they are exposed to relative humidity at or even above water saturation. For AgI particles that are totally immersed in water, the freezing temperature increases with increasing AgI surface area. Higher threshold freezing temperature seem to correlate with improved lattice matches as can be seen for AgI-AgCl solid solutions and 3AgI•NH4I•6H2O, which have slightly better lattice matches with ice than AgI and also higher threshold freezing temperatures. However, the effect of a good lattice match is annihilated when the surfaces have charges. Also, the ice nucleation ability seems to decrease during dissolution of AgI particles. This introduces an additional history and time dependence of ice nucleation in cloud chambers with short residence times.


2015 ◽  
Vol 15 (1) ◽  
pp. 393-409 ◽  
Author(s):  
P. J. DeMott ◽  
A. J. Prenni ◽  
G. R. McMeeking ◽  
R. C. Sullivan ◽  
M. D. Petters ◽  
...  

Abstract. Data from both laboratory studies and atmospheric measurements are used to develop an empirical parameterization for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RHw) are taken as a measure of the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterization developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A calibration factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RHw of 105% vs. maximum fractions active at higher RHw. Instrumental factors that affect activation behavior vs. RHw in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this calibration factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization, including calibration correction, to predictions of the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first-order approximation in numerical modeling investigations.


2014 ◽  
Vol 14 (4) ◽  
pp. 1853-1867 ◽  
Author(s):  
D. O'Sullivan ◽  
B. J. Murray ◽  
T. L. Malkin ◽  
T. F. Whale ◽  
N. S. Umo ◽  
...  

Abstract. Agricultural dust emissions have been estimated to contribute around 20% to the global dust burden. In contrast to dusts from arid source regions, the ice-nucleating abilities of which have been relatively well studied, soil dusts from fertile sources often contain a substantial fraction of organic matter. Using an experimental methodology which is sensitive to a wide range of ice nucleation efficiencies, we have characterised the immersion mode ice-nucleating activities of dusts (d < 11 μm) extracted from fertile soils collected at four locations around England. By controlling droplet sizes, which ranged in volume from 10−12 to 10−6 L (concentration = 0.02 to 0.1 wt% dust), we have been able to determine the ice nucleation behaviour of soil dust particles at temperatures ranging from 267 K (−6 °C) down to the homogeneous limit of freezing at about 237 K (−36 °C). At temperatures above 258 K (−15 °C) we find that the ice-nucleating activity of soil dusts is diminished by heat treatment or digestion with hydrogen peroxide, suggesting that a major fraction of the ice nuclei stems from biogenic components in the soil. However, below 258 K, we find that the ice active site densities tend towards those expected from the mineral components in the soils, suggesting that the inorganic fraction of soil dusts, in particular the K-feldspar fraction, becomes increasingly important in the initiation of the ice phase at lower temperatures. We conclude that dusts from agricultural activities could contribute significantly to atmospheric IN concentrations, if such dusts exhibit similar activities to those observed in the current laboratory study.


2015 ◽  
Vol 15 (13) ◽  
pp. 7523-7536 ◽  
Author(s):  
G. P. Schill ◽  
K. Genareau ◽  
M. A. Tolbert

Abstract. Ice nucleation of volcanic ash controls both ash aggregation and cloud glaciation, which affect atmospheric transport and global climate. Previously, it has been suggested that there is one characteristic ice nucleation efficiency for all volcanic ash, regardless of its composition, when accounting for surface area; however, this claim is derived from data from only two volcanic eruptions. In this work, we have studied the depositional and immersion freezing efficiency of three distinct samples of volcanic ash using Raman microscopy coupled to an environmental cell. Ash from the Fuego (basaltic ash, Guatemala), Soufrière Hills (andesitic ash, Montserrat), and Taupo (Oruanui eruption, rhyolitic ash, New Zealand) volcanoes were chosen to represent different geographical locations and silica content. All ash samples were quantitatively analyzed for both percent crystallinity and mineralogy using X-ray diffraction. In the present study, we find that all three samples of volcanic ash are excellent depositional ice nuclei, nucleating ice from 225 to 235 K at ice saturation ratios of 1.05 ± 0.01, comparable to the mineral dust proxy kaolinite. Since depositional ice nucleation will be more important at colder temperatures, fine volcanic ash may represent a global source of cold-cloud ice nuclei. For immersion freezing relevant to mixed-phase clouds, however, only the Oruanui ash exhibited appreciable heterogeneous ice nucleation activity. Similar to recent studies on mineral dust, we suggest that the mineralogy of volcanic ash may dictate its ice nucleation activity in the immersion mode.


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