scholarly journals Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

2015 ◽  
Vol 15 (1) ◽  
pp. 393-409 ◽  
Author(s):  
P. J. DeMott ◽  
A. J. Prenni ◽  
G. R. McMeeking ◽  
R. C. Sullivan ◽  
M. D. Petters ◽  
...  
Keyword(s):  
Mineral Dust ◽  
Order Approximation ◽  
Ice Nucleation ◽  
Calibration Factor ◽  
Dust Particles ◽  
Single Type ◽  
Aerosol Layer ◽  
Atmospheric Measurements ◽  
Immersion Freezing ◽  
Nucleation Activity

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.

scholarly journals Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

2014 ◽  
Vol 14 (11) ◽  
pp. 17359-17400 ◽  
Author(s):  
P. J. DeMott ◽  
A. J. Prenni ◽  
G. R. McMeeking ◽  
R. C. Sullivan ◽  
M. D. Petters ◽  
...  
Keyword(s):  
Correction Factor ◽  
Mineral Dust ◽  
Order Approximation ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Single Type ◽  
Aerosol Layer ◽  
Atmospheric Measurements ◽  
Immersion Freezing ◽  
Nucleation Activity

Abstract. Data from both laboratory studies and atmospheric measurements are used to develop a simple parametric description 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 to approximate 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 correction 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 correction 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 to 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.

scholarly journals A comprehensive laboratory study on the immersion freezing behavior of illite NX particles: a comparison of 17 ice nucleation measurement techniques

2015 ◽  
Vol 15 (5) ◽  
pp. 2489-2518 ◽  
Author(s):  
N. Hiranuma ◽  
S. Augustin-Bauditz ◽  
H. Bingemer ◽  
C. Budke ◽  
J. Curtius ◽  
...  
Keyword(s):  
Cooling Rate ◽  
Surface Area ◽  
Mineral Dust ◽  
Measurement Techniques ◽  
Ice Nucleation ◽  
Measurement Methods ◽  
Dust Particles ◽  
Immersion Freezing ◽  
Nucleation Activity ◽  
Ice Nucleation Activity

Abstract. Immersion freezing is the most relevant heterogeneous ice nucleation mechanism through which ice crystals are formed in mixed-phase clouds. In recent years, an increasing number of laboratory experiments utilizing a variety of instruments have examined immersion freezing activity of atmospherically relevant ice-nucleating particles. However, an intercomparison of these laboratory results is a difficult task because investigators have used different ice nucleation (IN) measurement methods to produce these results. A remaining challenge is to explore the sensitivity and accuracy of these techniques and to understand how the IN results are potentially influenced or biased by experimental parameters associated with these techniques. Within the framework of INUIT (Ice Nuclei Research Unit), we distributed an illite-rich sample (illite NX) as a representative surrogate for atmospheric mineral dust particles to investigators to perform immersion freezing experiments using different IN measurement methods and to obtain IN data as a function of particle concentration, temperature (T), cooling rate and nucleation time. A total of 17 measurement methods were involved in the data intercomparison. Experiments with seven instruments started with the test sample pre-suspended in water before cooling, while 10 other instruments employed water vapor condensation onto dry-dispersed particles followed by immersion freezing. The resulting comprehensive immersion freezing data set was evaluated using the ice nucleation active surface-site density, ns, to develop a representative ns(T) spectrum that spans a wide temperature range (−37 °C < T < −11 °C) and covers 9 orders of magnitude in ns. In general, the 17 immersion freezing measurement techniques deviate, within a range of about 8 °C in terms of temperature, by 3 orders of magnitude with respect to ns. In addition, we show evidence that the immersion freezing efficiency expressed in ns of illite NX particles is relatively independent of droplet size, particle mass in suspension, particle size and cooling rate during freezing. A strong temperature dependence and weak time and size dependence of the immersion freezing efficiency of illite-rich clay mineral particles enabled the ns parameterization solely as a function of temperature. We also characterized the ns(T) spectra and identified a section with a steep slope between −20 and −27 °C, where a large fraction of active sites of our test dust may trigger immersion freezing. This slope was followed by a region with a gentler slope at temperatures below −27 °C. While the agreement between different instruments was reasonable below ~ −27 °C, there seemed to be a different trend in the temperature-dependent ice nucleation activity from the suspension and dry-dispersed particle measurements for this mineral dust, in particular at higher temperatures. For instance, the ice nucleation activity expressed in ns was smaller for the average of the wet suspended samples and higher for the average of the dry-dispersed aerosol samples between about −27 and −18 °C. Only instruments making measurements with wet suspended samples were able to measure ice nucleation above −18 °C. A possible explanation for the deviation between −27 and −18 °C is discussed. Multiple exponential distribution fits in both linear and log space for both specific surface area-based ns(T) and geometric surface area-based ns(T) are provided. These new fits, constrained by using identical reference samples, will help to compare IN measurement methods that are not included in the present study and IN data from future IN instruments.

scholarly journals Deposition and immersion-mode nucleation of ice by three distinct samples of volcanic ash

2015 ◽  
Vol 15 (13) ◽  
pp. 7523-7536 ◽  
Author(s):  
G. P. Schill ◽  
K. Genareau ◽  
M. A. Tolbert
Keyword(s):  
Volcanic Ash ◽  
Mineral Dust ◽  
Global Climate ◽  
Volcanic Eruptions ◽  
Silica Content ◽  
Ice Nucleation ◽  
Ice Nuclei ◽  
Immersion Freezing ◽  
Nucleation Activity ◽  
Ice Nucleation Activity

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.

Influence of organic and biogenic substances on the ice nucleation properties of mineral dust particles

2020 ◽  
Author(s):  
Kristian Klumpp ◽  
Claudia Marcolli ◽  
Thomas Peter
Keyword(s):  
Amino Acids ◽  
Organic Acids ◽  
Mineral Dust ◽  
Particle Surface ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Biogenic Substances ◽  
Immersion Freezing ◽  
Mixed Phase Clouds ◽  
Ice Nucleation Activity

&lt;p&gt;The formation of ice in mixed phase clouds occurs in the presence of aerosol particles with the ability to nucleate ice on their surface. These ice-nucleating particles (INPs) represent usually a small fraction of particles in an atmospheric aerosol. One of the main particle types which act as INPs are mineral dust particles. Among other factors, the accumulation of semivolatile substances on the particle surface can alter the ice nucleation properties of such particles.&lt;/p&gt;&lt;p&gt;In recent immersion freezing experiments, we investigated the influence of organic acids, amino acids and polyols on the highly ice nucleation active K-feldspar microcline. Microcline dust was suspended in solutions of the above-mentioned substances and frozen in a differential scanning calorimeter (DSC). These experiments give us insight into the ice nucleation characteristics of the particles in the presence of the tested organic and biogenic substances. Our measurements show an overall decrease in ice nucleation activity of microcline in the presence of organic acids and amino acids. &lt;br&gt;&lt;br&gt;&lt;/p&gt;

scholarly journals Laboratory-generated mixtures of mineral dust particles with biological substances: characterization of the particle mixing state and immersion freezing behavior

2016 ◽  
Vol 16 (9) ◽  
pp. 5531-5543 ◽  
Author(s):  
Stefanie Augustin-Bauditz ◽  
Heike Wex ◽  
Cyrielle Denjean ◽  
Susan Hartmann ◽  
Johannes Schneider ◽  
...  
Keyword(s):  
Biological Material ◽  
Mineral Dust ◽  
Research Unit ◽  
Ice Nucleation ◽  
Freezing Behavior ◽  
Dust Particles ◽  
Mixing State ◽  
Nucleation Behavior ◽  
Immersion Freezing

Abstract. Biological particles such as bacteria, fungal spores or pollen are known to be efficient ice nucleating particles. Their ability to nucleate ice is due to ice nucleation active macromolecules (INMs). It has been suggested that these INMs maintain their nucleating ability even when they are separated from their original carriers. This opens the possibility of an accumulation of such INMs in soils, resulting in an internal mixture of mineral dust and INMs. If particles from such soils which contain biological INMs are then dispersed into the atmosphere due to wind erosion or agricultural processes, they could induce ice nucleation at temperatures typical for biological substances, i.e., above −20 up to almost 0 °C, while they might be characterized as mineral dust particles due to a possibly low content of biological material. We conducted a study within the research unit INUIT (Ice Nucleation research UnIT), where we investigated the ice nucleation behavior of mineral dust particles internally mixed with INM. Specifically, we mixed a pure mineral dust sample (illite-NX) with ice active biological material (birch pollen washing water) and quantified the immersion freezing behavior of the resulting particles utilizing the Leipzig Aerosol Cloud Interaction Simulator (LACIS). A very important topic concerning the investigations presented here as well as for atmospheric application is the characterization of the mixing state of aerosol particles. In the present study we used different methods like single-particle aerosol mass spectrometry, Scanning Electron Microscopy (SEM), Energy Dispersive X-ray analysis (EDX), and a Volatility–Hygroscopicity Tandem Differential Mobility Analyser (VH-TDMA) to investigate the mixing state of our generated aerosol. Not all applied methods performed similarly well in detecting small amounts of biological material on the mineral dust particles. Measuring the hygroscopicity/volatility of the mixed particles with the VH-TDMA was the most sensitive method. We found that internally mixed particles, containing ice active biological material, follow the ice nucleation behavior observed for the pure biological particles. We verified this by modeling the freezing behavior of the mixed particles with the Soccerball model (SBM). It can be concluded that a single INM located on a mineral dust particle determines the freezing behavior of that particle with the result that freezing occurs at temperatures at which pure mineral dust particles are not yet ice active.

scholarly journals Deposition and immersion mode nucleation of ice by three distinct samples of volcanic ash using Raman spectroscopy

2015 ◽  
Vol 15 (2) ◽  
pp. 1385-1420 ◽  
Author(s):  
G. P. Schill ◽  
K. Genareau ◽  
M. A. Tolbert
Keyword(s):  
Volcanic Ash ◽  
Mineral Dust ◽  
Global Climate ◽  
Volcanic Eruptions ◽  
Silica Content ◽  
Ice Nucleation ◽  
Ice Nuclei ◽  
Immersion Freezing ◽  
Nucleation Activity ◽  
Ice Nucleation Activity

Abstract. Ice nucleation on 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 euption, 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 225–235 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 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.

scholarly journals The immersion freezing behavior of mineral dust particles mixed with biological substances

2015 ◽  
Vol 15 (20) ◽  
pp. 29639-29671 ◽  
Author(s):  
S. Augustin-Bauditz ◽  
H. Wex ◽  
C. Denjean ◽  
S. Hartmann ◽  
J. Schneider ◽  
...  
Keyword(s):  
Biological Material ◽  
Mineral Dust ◽  
Fungal Spores ◽  
Birch Pollen ◽  
Ice Nucleation ◽  
Freezing Behavior ◽  
Dust Particles ◽  
Nucleation Behavior ◽  
Biological Particles ◽  
Immersion Freezing

Abstract. Biological particles such as bacteria, fungal spores or pollen are known to be efficient ice nucleating particles. Their ability to nucleate ice is due to ice nucleation active macromolecules (INM). It has been suggested that these INM maintain their nucleating ability even when they are separated from their original carriers. This opens the possibility of an accumulation of such INM in e.g., soils, resulting in an internal mixture of mineral dust and INM. If particles from such soils which contain biological INM are then dispersed into the atmosphere due to wind erosion or agricultural processes, they could induce ice nucleation at temperatures typical for biological substances, i.e., above −20 up to almost 0 °C. To explore this hypothesis, we performed a measurement campaign within the research unit INUIT, where we investigated the ice nucleation behavior of mineral dust particles internally mixed with INM. Specifically, we mixed a pure mineral dust sample (illite-NX) with ice active biological material (birch pollen washing water) and quantified the immersion freezing behavior of the resulting particles utilizing the Leipzig Aerosol Cloud Interaction Simulator (LACIS). To characterize the mixing state of the generated aerosol we used different methods which will also be discussed. We found that internally mixed particles, containing ice active biological material, follow the ice nucleation behavior observed for the purely biological particles, i.e. freezing occurs at temperatures at which mineral dusts themselves are not yet ice active. It can be concluded that INM located on a mineral dust particle determine the freezing behavior of that particle.

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

2019 ◽  
Vol 19 (7) ◽  
pp. 5091-5110 ◽  
Author(s):  
Zamin A. Kanji ◽  
Ryan C. Sullivan ◽  
Monika Niemand ◽  
Paul J. DeMott ◽  
Anthony J. Prenni ◽  
...  
Keyword(s):  
Coating Thickness ◽  
Secondary Organic Aerosol ◽  
Mineral Dust ◽  
Size Fraction ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Expansion Chamber ◽  
Significant Difference ◽  
Immersion Freezing

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.

scholarly journals Heterogeneous Ice Nucleation Properties of Natural Desert Dust Particles Coated with a Surrogate of Secondary Organic Aerosol

2018 ◽  
Author(s):  
Zamin A. Kanji ◽  
Ryan C. Sullivan ◽  
Monika Niemand ◽  
Paul J. DeMott ◽  
Anthony J. Prenni ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Mineral Dust ◽  
Size Fraction ◽  
Diffusion Chamber ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Expansion Chamber ◽  
Significant Difference ◽  
Immersion Freezing

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.

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