The importance of feldspar for ice nucleation by mineral dust in mixed-phase clouds.

The amount of ice present in mixed-phase clouds, which contain both supercooled liquid water droplets and ice particles, affects cloud extent, lifetime, particle size and radiative properties. The freezing of cloud droplets can be catalysed by the presence of aerosol particles known as ice nuclei. One of the most important ice nuclei is thought to be mineral dust aerosol from arid regions. It is generally assumed that clay minerals, which contribute approximately two-thirds of the dust mass, dominate ice nucleation by mineral dust, and many experimental studies have therefore focused on these materials. Here we use an established droplet-freezing technique to show that feldspar minerals dominate ice nucleation by mineral dusts under mixed-phase cloud conditions, despite feldspar being a minor component of dust emitted from arid regions. We also find that clay minerals are relatively unimportant ice nuclei. Our results from a global aerosol model study suggest that feldspar ice nuclei are globally distributed and that feldspar particles may account for a large proportion of the ice nuclei in Earth's atmosphere that contribute to freezing at temperatures below about -15 °C.

Characterizing the morphology of organic aerosols at ambient temperature and pressure.

The aerosol direct effect, which characterizes the interaction of radiation with aerosol particles, remains poorly understood. By determining aerosol composition, shape, and internal structure, we can predict aerosol optical properties. In this study, we performed a feasibility study to determine if tapping-mode atomic force microscopy (TM-AFM) and Raman microscopy can be effectively used to obtain information on aerosol composition, shape, and structure. These techniques are advantageous because they operate under ambient pressure and temperature. We worked with model aerosol particles composed of organic components of varying solubility mixed with ammonium sulfate. In particular, we explored whether aerosols could be differentiated on the basis of the solubility of the organic component. We also characterized the aerosol internal structure and investigated how this structure changes as the solubility of the organic compound is varied. To obtain indirect chemical information from AFM, we imaged particles supported on both polar, SiO(x)/Si(100), and nonpolar, highly ordered pyrolytic graphite, surfaces. We have found that AFM can be used to differentiate the solubility of the organic component. In some cases, AFM can also be used to identify internal structure. With Raman microscopy, we can differentiate between core-shell structures and homogeneous structures. Surprisingly, we find that even for the most soluble compounds, core-shell structures are observed. To discuss consequences of our results for climate studies, we calculate the difference in radiative forcing caused by having a core-shell aerosol rather than a homogeneous particle. Overall, these techniques are promising for characterizing composition, shape, and internal structure of atmospheric particles.

Internally mixed sulfate and organic particles as potential ice nuclei in the tropical tropopause region.

Cirrus clouds are ubiquitous in the tropical tropopause region and play a major role in the Earth's climate. Any changes to cirrus abundance due to natural or anthropogenic influences must be considered to evaluate future climate change. The detailed impact of cirrus clouds on climate depends on ice particle number, size, morphology, and composition. These properties depend in turn on the nucleation mechanism of the ice particles. Although it is often assumed that ice nucleates via a homogeneous mechanism, recent work points to the possibility that heterogeneous ice nucleation is important in the tropical tropopause region. However, there are very few studies of depositional ice nucleation on the complex types of particles likely to be found in this region of the atmosphere. Here, we use a unique method to probe depositional ice nucleation on internally mixed ammonium sulfate/palmitic acid particles, namely optical microscopy coupled with Raman microscopy. The deliquescence and efflorescence phase transitions of the mixed particles were first studied to gain insight into whether the particles are likely to be liquid or solid in the tropical tropopause region. The ice nucleating ability of the particles was then measured under typical upper tropospheric conditions. It was found that coating the particles with insoluble palmitic acid had little effect on the deliquescence, efflorescence, or ice nucleating ability of ammonium sulfate. Additional experiments involving Raman mapping provide new insights into how the composition and morphology of mixed particles impact their ability to nucleate ice.