D. Niedermeier

Heterogeneous freezing of droplets with immersed mineral dust particles - measurements and parameterization

During the measurement campaign FROST (FReezing Of duST), LACIS (Leipzig Aerosol Cloud Interaction Simulator) was used to investigate the immersion freezing behavior of size selected, coated and uncoated Arizona Test Dust (ATD) particles with a mobility diameter of 300 nm. Particles were coated with succinic acid (C 4H6O4), sulfuric acid (H2SO4) and ammonium sulfate ((NH 4)2SO4). Ice fractions at mixed-phase cloud temperatures ranging from 233.15 K to 239.15 K ( ±0.60 K) were determined for all types of particles. In this temperature range, pure ATD particles and those coated with C 4H6O4 or small amounts of H2SO4 were found to be the most efficient ice nuclei (IN). ATD particles coated with (NH4)2SO4 were the most inefficient IN. Since the supercooled droplets were highly diluted before freezing occurred, a freezing point suppression due to the soluble material on the particles (and therefore in the droplets) cannot explain this observation. Therefore, it is reasonable to assume that the coatings lead to particle surface alterations which cause the differences in the IN abilities. Two different theoretical approaches based on the stochastic and the singular hypotheses were applied to clarify and parameterize the freezing behavior of the particles investigated. Both approaches describe the experimentally determined results, yielding parameters that can subsequently be used to compare our results to those from other studies. HowCorrespondence to: D. Niedermeier (niederm@tropos.de) ever, we cannot clarify at the current state which of the two approaches correctly describes the investigated immersion freezing process. But both approaches confirm the assumption that the coatings lead to particle surface modifications lowering the nucleation efficiency. The stochastic approach interprets the reduction in nucleation rate from coating as primarily due to an increase in the thermodynamic barrier for ice formation (i.e., changes in interfacial free energies). The singular approach interprets the reduction as resulting from a reduced surface density of active sites.

The immersion mode ice nucleation behavior of mineral dusts: A comparison of different pure and surface modified dusts

In this study we present results from immersion freezing experiments with size-segregated mineral dust particles. Besides two already existing data sets for Arizona Test Dust (ATD), and Fluka kaolinite, we show two new data sets for illite-NX, which consists mainly of illite, a clay mineral, and feldspar, a common crustal material. The experiments were carried out with the Leipzig Aerosol Cloud Interaction Simulator. After comparing the different dust samples, it became obvious that the freezing ability was positively correlated with the K-feldspar content. Furthermore, a comparison of the composition of the ATD, illite-NX, and feldspar samples suggests that within the K-feldspars, microcline is more ice nucleation active than orthoclase. A coating with sulfuric acid leads to a decrease in the ice nucleation ability of all mineral dusts, with the effect being more pronounced for the feldspar sample.

A computationally efficient description of heterogeneous freezing: A simplified version of the Soccer ball model

In a recent study, the Soccer ball model (SBM) was introduced for modeling and/or parameterizing heterogeneous ice nucleation processes. The model applies classical nucleation theory. It allows for a consistent description of both apparently singular and stochastic ice nucleation behavior, by distributing contact angles over the nucleation sites of a particle population assuming a Gaussian probability density function. The original SBM utilizes the Monte Carlo technique, which hampers its usage in atmospheric models, as fairly time-consuming calculations must be performed to obtain statistically significant results. Thus, we have developed a simplified and computationally more efficient version of the SBM. We successfully used the new SBM to parameterize experimental nucleation data of, e.g., bacterial ice nucleation. Both SBMs give identical results; however, the new model is computationally less expensive as confirmed by cloud parcel simulations. Therefore, it is a suitable tool for describing heterogeneous ice nucleation processes in atmospheric models.

Aerosol indirect effect from turbulence-induced broadening of cloud-droplet size distributions

Significance Atmospheric aerosol concentration is linked to cloud brightness and lifetime through the modulation of precipitation. Generally speaking, larger cloud droplets and wider-droplet size distributions form precipitation more efficiently. We create steady-state clouds in the laboratory through a balance of constant aerosol injection and cloud-droplet removal due to settling. As aerosol concentration is decreased, the cloud-droplet mean diameter increases, as expected, but also the width of the size distribution increases sharply. Theory, simulations, and measurements point to greater supersaturation variability as the cause of this broadening in what can be considered a low aerosol/slow microphysics limit. The influence of aerosol concentration on the cloud-droplet size distribution is investigated in a laboratory chamber that enables turbulent cloud formation through moist convection. The experiments allow steady-state microphysics to be achieved, with aerosol input balanced by cloud-droplet growth and fallout. As aerosol concentration is increased, the cloud-droplet mean diameter decreases, as expected, but the width of the size distribution also decreases sharply. The aerosol input allows for cloud generation in the limiting regimes of fast microphysics (τcτt) for low aerosol concentration; here, τc is the phase-relaxation time and τt is the turbulence-correlation time. The increase in the width of the droplet size distribution for the low aerosol limit is consistent with larger variability of supersaturation due to the slow microphysical response. A stochastic differential equation for supersaturation predicts that the standard deviation of the squared droplet radius should increase linearly with a system time scale defined as τs−1=τc−1+τt−1, and the measurements are in excellent agreement with this finding. The result underscores the importance of droplet size dispersion for aerosol indirect effects: increasing aerosol concentration changes the albedo and suppresses precipitation formation not only through reduction of the mean droplet diameter but also by narrowing of the droplet size distribution due to reduced supersaturation fluctuations. Supersaturation fluctuations in the low aerosol/slow microphysics limit are likely of leading importance for precipitation formation.

Can we define an asymptotic value for the ice active surface site density for heterogeneous ice nucleation

The immersion freezing behavior of droplets containing size-segregated, monodisperse feldspar particles was investigated. For all particle sizes investigated, a leveling off of the frozen droplet fraction was observed reaching a plateau within the heterogeneous freezing temperature regime (T >− 38°C). The frozen fraction in the plateau region was proportional to the particle surface area. Based on these findings, an asymptotic value for ice active surface site density ns, which we named ns⋆, could be determined for the investigated feldspar sample. The comparison of these results with those of other studies not only elucidates the general feasibility of determining such an asymptotic value but also shows that the value of ns⋆ strongly depends on the method of the particle surface area determination. However, such an asymptotic value might be an important input parameter for atmospheric modeling applications. At least it shows that care should be taken when ns is extrapolated to lower or higher temperature.

Immersion Freezing of Kaolinite: Scaling with Particle Surface Area

AbstractThis study presents an analysis showing that the freezing probability of kaolinite particles from Fluka scales exponentially with particle surface area for different atmospherically relevant particle sizes. Immersion freezing experiments were performed at the Leipzig Aerosol Cloud Interaction Simulator (LACIS). Size-selected kaolinite particles with mobility diameters of 300, 700, and 1000 nm were analyzed with one particle per droplet. First, it is demonstrated that immersion freezing is independent of the droplet volume. Using the mobility analyzer technique for size selection involves the presence of multiply charged particles in the quasi-monodisperse aerosol, which are larger than singly charged particles. The fractions of these were determined using cloud droplet activation measurements. The development of a multiple charge correction method has proven to be essential for deriving ice fractions and other quantities for measurements in which the here-applied method of size selection is used. ...

A laboratory facility to study gas-aerosol-cloud interactions in a turbulent environment: The Π Chamber

AbstractA detailed understanding of interactions of aerosols, cloud droplets/ice crystals, and trace gases within the atmosphere is of prime importance for an accurate understanding of Earth’s weather and climate. One aspect that remains especially vexing is that clouds are ubiquitously turbulent, and therefore thermodynamic and compositional variables, such as water vapor supersaturation, fluctuate in space and time. With these problems in mind, a multiphase, turbulent reaction chamber—called the Π chamber because of the internal volume of 3.14 m3 with the cylindrical insert installed—has been developed. It is capable of pressures ranging from 1,000 to –60 hPa and can sustain temperatures of –55° to 55°C, thereby spanning much of the range of tropospheric clouds. To control the relative humidity in the chamber, it can be operated with a stable, unstable, or neutral temperature difference between the top and bottom surfaces, with or without expansion. A negative temperature difference induces turbulent Ra...

Heterogeneous ice nucleation on biological particles: Bacteria and pollen

In the atmosphere the importance of biological ice nuclei is still not well understood. Therefore we investigated the ice nucleation behavior of Snomax™, used as a model for bacterial ice nucleation, and birch pollen washing water, used as a model for pollen induced ice nucleation. Thereby we quantified the ice nucleation behavior of the INA protein complexes controlling the ice nucleation ability of Pseudomonas syringae, and that of sugar-like macromolecules controlling the ice nucleation ability of birch pollen. The given parameterizations can be used to describe the ice nucleation behavior of the respective ice active bacteria and pollen in atmospheric models.