scholarly journals Bacteria as Cloud Condensation Nuclei (CCN) in the Atmosphere

Atmosphere ◽  
2019 ◽  
Vol 10 (12) ◽  
pp. 786
Author(s):  
Mihalis Lazaridis
Keyword(s):  
Contact Angle ◽  
Sulfuric Acid ◽  
Cloud Condensation Nuclei ◽  
Sulfuric Acid Concentration ◽  
Contact Angles ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Condensation Nuclei ◽  
Critical Cluster ◽  
Model Simulations

Bacteria activation and cloud condensation nuclei (CCN) formation have been studied in the atmosphere using the classical theory of heterogeneous nucleation. Simulations were performed for the binary system of sulfuric acid/water using laboratory-determined contact angles. Realistic model simulations were performed at different atmospheric heights for a set of 140 different bacteria. Model simulations showed that bacteria activation is a potentially favorable process in the atmosphere which may be enhanced at lower temperatures. CCN formation from bacteria nuclei is dependent on ambient atmospheric conditions (temperature, relative humidity), bacteria size, and sulfuric acid concentration. Furthermore, a critical parameter for the determination of bacteria activation is the value of the intermolecular potential between the bacteria’s surface and the critical cluster formed at their surface. In the classical nucleation theory, this is parameterized with the contact angle between substrate and critical cluster. Therefore, the dataset of laboratory values for the contact angle of water on different bacteria substrates needs to be enriched for realistic simulations of bacteria activation in the atmosphere.

scholarly journals Deposition nucleation on mineral dust particles: a case against classical nucleation theory with the assumption of a single contact angle

2012 ◽  
Vol 12 (2) ◽  
pp. 1189-1201 ◽  
Author(s):  
M. J. Wheeler ◽  
A. K. Bertram
Keyword(s):  
Contact Angle ◽  
Surface Area ◽  
Deterministic Model ◽  
Optical Microscope ◽  
Contact Angles ◽  
Nucleation Theory ◽  
Dust Particles ◽  
Classical Nucleation Theory ◽  
Site Model ◽  
Single Contact

Abstract. Deposition nucleation on two mineral species, kaolinite and illite, was studied using a flow cell coupled to an optical microscope. The results show that the Sice conditions when ice first nucleated, defined as the onset Sice (Sice,onset), is a strong function of the surface area available for nucleation, varying from 100% to 125% at temperatures between 242 and 239 K. The surface area dependent data could not be described accurately using classical nucleation theory and the assumption of a single contact angle (defined here as the single-α model). These results suggest that caution should be applied when using contact angles determined from Sice,onset data and the single-α model. In contrast to the single-α model, the active site model, the deterministic model, and a model with a distribution of contact angles fit the data within experimental uncertainties. Parameters from the fits to the data are presented.

scholarly journals Deposition freezing on mineral dust particles: a case against classical nucleation theory with the assumption of a single contact angle

2011 ◽  
Vol 11 (7) ◽  
pp. 21171-21200 ◽  
Author(s):  
M. J. Wheeler ◽  
A. K. Bertram
Keyword(s):  
Contact Angle ◽  
Surface Area ◽  
Deterministic Model ◽  
Optical Microscope ◽  
Contact Angles ◽  
Nucleation Theory ◽  
Dust Particles ◽  
Classical Nucleation Theory ◽  
Site Model ◽  
Single Contact

Abstract. Deposition freezing on two mineral species, kaolinite and illite, was studied using a flow cell coupled to an optical microscope at ∼240 K. The results show that the onset Sice (defined as the Sice conditions when ice first nucleated) is a strong function of the surface area available for nucleation, varying from 100 % to 125 %. The surface area dependent data could not be described accurately using classical nucleation theory and the assumption of a single contact angle (defined here as the single-α model). These results suggest that caution should be applied when using contact angles determined from onset Sice data and the single-α model. In contrast to the single-α model, the active site model, the deterministic model, and a model with a normal distribution of contact angles fit the data within experimental uncertainties. Parameters from the fits to the data are presented.

scholarly journals Efficiency of immersion mode ice nucleation on surrogates of mineral dust

2007 ◽  
Vol 7 (19) ◽  
pp. 5081-5091 ◽  
Author(s):  
C. Marcolli ◽  
S. Gedamke ◽  
T. Peter ◽  
B. Zobrist
Keyword(s):  
Contact Angle ◽  
Active Sites ◽  
Quantitative Agreement ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Aqueous Suspensions ◽  
Freezing Temperatures ◽  
Good Agreement ◽  
Heterogeneous Ice Nucleation

Abstract. A differential scanning calorimeter (DSC) was used to explore heterogeneous ice nucleation of emulsified aqueous suspensions of two Arizona test dust (ATD) samples with particle diameters of nominally 0–3 and 0–7 μm, respectively. Aqueous suspensions with ATD concentrations of 0.01–20 wt% have been investigated. The DSC thermograms exhibit a homogeneous and a heterogeneous freezing peak whose intensity ratios vary with the ATD concentration in the aqueous suspensions. Homogeneous freezing temperatures are in good agreement with recent measurements by other techniques. Depending on ATD concentration, heterogeneous ice nucleation occurred at temperatures as high as 256 K or down to the onset of homogeneous ice nucleation (237 K). For ATD-induced ice formation Classical Nucleation Theory (CNT) offers a suitable framework to parameterize nucleation rates as a function of temperature, experimentally determined ATD size, and emulsion droplet volume distributions. The latter two quantities serve to estimate the total heterogeneous surface area present in a droplet, whereas the suitability of an individual heterogeneous site to trigger nucleation is described by the compatibility function (or contact angle) in CNT. The intensity ratio of homogeneous to heterogeneous freezing peaks is in good agreement with the assumption that the ATD particles are randomly distributed amongst the emulsion droplets. The observed dependence of the heterogeneous freezing temperatures on ATD concentrations cannot be described by assuming a constant contact angle for all ATD particles, but requires the ice nucleation efficiency of ATD particles to be (log)normally distributed amongst the particles. Best quantitative agreement is reached when explicitly assuming that high-compatibility sites are rare and that therefore larger particles have on average more and better active sites than smaller ones. This analysis suggests that a particle has to have a diameter of at least 0.1 μm to exhibit on average one active site.

scholarly journals A new temperature- and humidity-dependent surface site density approach for deposition ice nucleation

2015 ◽  
Vol 15 (7) ◽  
pp. 3703-3717 ◽  
Author(s):  
I. Steinke ◽  
C. Hoose ◽  
O. Möhler ◽  
P. Connolly ◽  
T. Leisner
Keyword(s):  
Contact Angle ◽  
Relative Humidity ◽  
Active Surface ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Aerosol Size Distribution ◽  
Surface Site ◽  
Linear Behavior ◽  
Temperature And Humidity

Abstract. Deposition nucleation experiments with Arizona Test Dust (ATD) as a surrogate for mineral dusts were conducted at the AIDA cloud chamber at temperatures between 220 and 250 K. The influence of the aerosol size distribution and the cooling rate on the ice nucleation efficiencies was investigated. Ice nucleation active surface site (INAS) densities were calculated to quantify the ice nucleation efficiency as a function of temperature, humidity and the aerosol surface area concentration. Additionally, a contact angle parameterization according to classical nucleation theory was fitted to the experimental data in order to relate the ice nucleation efficiencies to contact angle distributions. From this study it can be concluded that the INAS density formulation is a very useful tool to describe the temperature- and humidity-dependent ice nucleation efficiency of ATD particles. Deposition nucleation on ATD particles can be described by a temperature- and relative-humidity-dependent INAS density function ns(T, Sice) with ns(xtherm) = 1.88 ×105 · exp(0.2659 · xtherm) [m−2] , (1) where the temperature- and saturation-dependent function xtherm is defined as xtherm = −(T−273.2)+(Sice−1) ×100, (2) with the saturation ratio with respect to ice Sice >1 and within a temperature range between 226 and 250 K. For lower temperatures, xtherm deviates from a linear behavior with temperature and relative humidity over ice. Also, two different approaches for describing the time dependence of deposition nucleation initiated by ATD particles are proposed. Box model estimates suggest that the time-dependent contribution is only relevant for small cooling rates and low number fractions of ice-active particles.

scholarly journals Immersion freezing of water and aqueous ammonium sulfate droplets initiated by humic-like substances as a function of water activity

2013 ◽  
Vol 13 (13) ◽  
pp. 6603-6622 ◽  
Author(s):  
Y. J. Rigg ◽  
P. A. Alpert ◽  
D. A. Knopf
Keyword(s):  
Water Activity ◽  
Active Sites ◽  
Melting Curve ◽  
Contact Angles ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Surface Areas ◽  
Immersion Freezing ◽  
Freezing Temperatures

Abstract. Immersion freezing of water and aqueous (NH4)2SO4 droplets containing leonardite (LEO) and Pahokee peat (PP) serving as surrogates for humic-like substances (HULIS) has been investigated. Organic aerosol containing HULIS are ubiquitous in the atmosphere; however, their potential for ice cloud formation is uncertain. Immersion freezing has been studied for temperatures as low as 215 K and solution water activity, aw, from 0.85 to 1.0. The freezing temperatures of water and aqueous solution droplets containing LEO and PP are 5–15 K warmer than homogeneous ice nucleation temperatures. Heterogeneous freezing temperatures can be represented by a horizontal shift of the ice melting curve as a function of solution aw by Δaw = 0.2703 and 0.2466, respectively. Corresponding hetrogeneous ice nucleation rate coefficients, Jhet, are (9.6 ± 2.5)×104 and (5.4 ± 1.4)×104 cm−2 s−1 for LEO and PP containing droplets, respectively, and remain constant along freezing curves characterized by Δaw. Consequently predictions of freezing temperatures and kinetics can be made without knowledge of the solute type when relative humidity and ice nuclei (IN) surface areas are known. The acquired ice nucleation data are applied to evaluate different approaches to fit and reproduce experimentally derived frozen fractions. In addition, we apply a basic formulation of classical nucleation theory (α(T)-model) to calculate contact angles and frozen fractions. Contact angles calculated for each ice nucleus as a function of temperature, α(T)-model, reproduce exactly experimentally derived frozen fractions without involving free-fit parameters. However, assigning the IN a single contact angle for the entire population (single-α model) is not suited to represent the frozen fractions. Application of α-PDF, active sites, and deterministic model approaches to measured frozen fractions yield similar good representations. Furthermore, when using a single parameterization of α-PDF or active sites distribution to fit all individual aw immersion freezing data simultaneously, frozen fraction curves are not reproduced. This implies that these fitting formulations cannot be applied to immersion freezing of aqueous solutions, and suggests that derived fit parameters do not represent independent particle properties. Thus, from fitting frozen fractions only, the underlying ice nucleation mechanism and nature of the ice nucleating sites cannot be inferred. In contrast to using fitted functions obtained to represent experimental conditions only, we suggest to use experimentally derived Jhet as a function of temperature and aw that can be applied to conditions outside of those probed in laboratory. This is because Jhet(T) is independent of time and IN surface areas in contrast to the fit parameters obtained by representation of experimentally derived frozen fractions.

scholarly journals Ice nucleation by water-soluble macromolecules

2014 ◽  
Vol 14 (17) ◽  
pp. 24273-24309 ◽  
Author(s):  
B. G. Pummer ◽  
C. Budke ◽  
S. Augustin-Bauditz ◽  
D. Niedermeier ◽  
L. Felgitsch ◽  
...  
Keyword(s):  
Pure Water ◽  
Global Radiation ◽  
Ice Nucleation ◽  
Biological Species ◽  
Water Soluble ◽  
Nucleation Theory ◽  
Radiation Budget ◽  
Classical Nucleation Theory ◽  
Critical Cluster ◽  
Ice Nucleators

Abstract. Cloud glaciation is critically important for the global radiation budget (albedo) and for initiation of precipitation. But the freezing of pure water droplets requires cooling to temperatures as low as 235 K. Freezing at higher temperatures requires the presence of an ice nucleator, which is a foreign body in the water that functions as a template for arranging water molecules in an ice-like manner. It is often assumed that these ice nucleators have to be insoluble particles. We put in perspective that also dissolved single macromolecules can induce ice nucleation: they are several nanometers in size, which is also the size range of the necessary critical cluster. As the critical cluster size is temperature-dependent, we see a correlation between the size of such ice nucleating macromolecules and the ice nucleation temperature. Such ice nucleating macromolecules have been already found in many different biological species and are as manifold in their chemistry. Therefore, we additionally compare them to each other, based on a composition of former, recent and yet unpublished studies. Combining these data with calculations from Classical Nucleation Theory, we want to foster a more molecular view of ice nucleation among scientists.

scholarly journals An aerosol chamber investigation of the heterogeneous ice nucleating potential of refractory nanoparticles

2010 ◽  
Vol 10 (3) ◽  
pp. 1227-1247 ◽  
Author(s):  
R. W. Saunders ◽  
O. Möhler ◽  
M. Schnaiter ◽  
S. Benz ◽  
R. Wagner ◽  
...  
Keyword(s):  
Silicon Oxide ◽  
Cloud Model ◽  
Active Surface ◽  
Accommodation Coefficient ◽  
Contact Angles ◽  
Nucleation Theory ◽  
Cloud Formation ◽  
Classical Nucleation Theory ◽  
Ice Nuclei

Abstract. Nanoparticles of iron oxide (crystalline and amorphous), silicon oxide and magnesium oxide were investigated for their propensity to nucleate ice over the temperature range 180–250 K, using the AIDA chamber in Karlsruhe, Germany. All samples were observed to initiate ice formation via the deposition mode at threshold ice super-saturations (RHithresh) ranging from 105% to 140% for temperatures below 220 K. Approximately 10% of amorphous Fe2O3 particles (modal diameter = 30 nm) generated in situ from a photochemical aerosol reactor, led to ice nucleation at RHithresh = 140% at an initial chamber temperature of 182 K. Quantitative analysis using a singular hypothesis treatment provided a fitted function [ns(190 K)=10(3.33×sice)+8.16] for the variation in ice-active surface site density (ns:m−2) with ice saturation (sice) for Fe2O3 nanoparticles. This was implemented in an aerosol-cloud model to determine a predicted deposition (mass accommodation) coefficient for water vapour on ice of 0.1 at temperatures appropriate for the upper atmosphere. Classical nucleation theory was used to determine representative contact angles (θ) for the different particle compositions. For the in situ generated Fe2O3 particles, a slight inverse temperature dependence was observed with θ = 10.5° at 182 K, decreasing to 9.0° at 200 K (compared with 10.2° and 11.4° respectively for the SiO2 and MgO particle samples at the higher temperature). These observations indicate that such refractory nanoparticles are relatively efficient materials for the nucleation of ice under the conditions studied in the chamber which correspond to cirrus cloud formation in the upper troposphere. The results also show that Fe2O3 particles do not act as ice nuclei under conditions pertinent for tropospheric mixed phase clouds, which necessarily form above ~233 K. At the lower temperatures (<150 K) where noctilucent clouds form during summer months in the high latitude mesosphere, higher contact angles would be expected, which may reduce the effectiveness of these particles as ice nuclei in this part of the atmosphere.

scholarly journals African biomass burning plumes over the Atlantic: aircraft based measurements and implications for H<sub>2</sub>SO<sub>4</sub> and HNO<sub>3</sub> mediated smoke particle activation

2011 ◽  
Vol 11 (7) ◽  
pp. 3211-3225 ◽  
Author(s):  
V. Fiedler ◽  
F. Arnold ◽  
S. Ludmann ◽  
A. Minikin ◽  
T. Hamburger ◽  
...  
Keyword(s):  
Water Vapor ◽  
Sulfuric Acid ◽  
Biomass Burning ◽  
Vapor Condensation ◽  
Condensation Nuclei ◽  
Smoke Particle ◽  
Model Simulations ◽  
Airborne Measurements ◽  
Smoke Particles ◽  
Water Vapor Condensation

Abstract. Airborne measurements of trace gases and aerosol particles have been made in two aged biomass burning (BB) plumes over the East Atlantic (Gulf of Guinea). The plumes originated from BB in the Southern-Hemisphere African savanna belt. On the day of our measurements (13 August 2006), the plumes had ages of about 10 days and were respectively located in the middle troposphere (MT) at 3900–5500 m altitude and in the upper troposphere (UT) at 10 800–11 200 m. Probably, the MT plume was lifted by dry convection and the UT plume was lifted by wet convection. In the more polluted MT-plume, numerous measured trace species had markedly elevated abundances, particularly SO2 (up to 1400 pmol mol−1), HNO3 (5000–8000 pmol mol−1) and smoke particles with diameters larger than 270 nm (up to 2000 cm−3). Our MT-plume measurements indicate that SO2 released by BB had not experienced significant loss by deposition and cloud processes but rather had experienced OH-induced conversion to gas-phase sulfuric acid. By contrast, a significant fraction of the released NOy had experienced loss, most likely as HNO3 by deposition. In the UT-plume, loss of NOy and SO2 was more pronounced compared to the MT-plume, probably due to cloud processes. Building on our measurements and accompanying model simulations, we have investigated trace gas transformations in the ageing and diluting plumes and their role in smoke particle processing and activation. Emphasis was placed upon the formation of sulfuric acid and ammonium nitrate, and their influence on the activation potential of smoke particles. Our model simulations reveal that, after 13 August, the lower plume traveled across the Atlantic and descended to 1300 m and hereafter ascended again. During the travel across the Atlantic, the soluble mass fraction of smoke particles and their mean diameter increased sufficiently to allow the processed smoke particles to act as water vapor condensation nuclei already at very low water vapor supersaturations of only about 0.04%. Thereby, aged smoke particles had developed a potential to act as water vapor condensation nuclei in the formation of maritime clouds.

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