Homogeneous nucleation rates are determined for micrometer sized water droplets levitated inside an electrodynamic Paul-trap. The size of a single droplet is continuously measured by analyzing the angle-resolved light scattering pattern of the droplets with classical Mie theory. The freezing process is detected by a pronounced increase in the depolarization of the scattered light. By statistical analysis of the freezing process of some thousand individual droplets, we obtained the homogeneous nucleation rate of water between 236 and 237 K. The values are in agreement with former expansion cloud chamber measurements but could be determined with considerably higher precision. The measurements are discussed in the light of classical nucleation theory in order to obtain the size and the formation energy of the critical nucleus.
Homogeneous ice nucleation rates in single isolated micro droplets of water are determined under various atmospheric conditions inside an electrodynamic Paul-trap. The droplet size is measured by angle-resolved detection of the scattered light from a Helium-Neon laser. The freezing process is detected by a sudden change of the depolarization ratio which is an indication for the formation of nonspherical particles.The experimentally determined homogeneous ice nucleation rates JLs are JLs = ( 2 . 2~0 0 . 4 ) . 1 0 8 c m~3 s -' at T = (-37.2kO.15)'C and JLs = (5.6e 1.0). 10' c r K 3 sat T = ( -37.7 * 0.15)OC.These values are much more precise as determined by measurements inside a cloud expansion chamber. The method of single particle observation eliminates complications arising from these nucleation rate measurements. The results underline the theory that one single ice germ of certain size is sufficient to induce the freezing of the whole droplet. The depolarization ratio of the scattered intensity in the parallel and perpendicular polarization plane I, / I p from the frozen particles exhibits a broad distribution with a mean value of Zs(Ip = 0.3.
Luminescence-encoded microbeads are important tools for many applications in the life and material sciences that utilize luminescence detection as well as multiplexing and barcoding strategies. The preparation of such beads often involves the staining of premanufactured beads with molecular luminophores using simple swelling procedures or surface functionalization with layer-by-layer (LbL) techniques. Alternatively, these luminophores are sterically incorporated during the polymerization reaction yielding the polymer beads. The favorable optical properties of semiconductor quantum dots (QDs), which present broadly excitable, size-tunable, narrow emission bands and low photobleaching sensitivity, triggered the preparation of beads stained with QDs. However, the colloidal nature and the surface chemistry of these QDs, which largely controls their luminescence properties, introduce new challenges to bead encoding that have been barely systematically assessed. To establish a straightforward approach for the bead encoding with QDs with minimized loss in luminescence, we systematically assessed the incorporation of oleic acid/oleylamine-stabilized CdSe/CdS-core/shell-QDs into 0.5–2.5 µm-sized polystyrene (PS) microspheres by a simple dispersion polymerization synthesis that was first optimized with the organic dye Nile Red. Parameters addressed for the preparation of luminophore-encoded beads include the use of a polymer-compatible ligand such as benzyldimethyloctadecylammonium chloride (OBDAC) for the QDs, and crosslinking to prevent luminophore leakage. The physico-chemical and optical properties of the resulting beads were investigated with electron microscopy, dynamic light scattering, optical spectroscopy, and fluorescence microscopy. Particle size distribution, fluorescence quantum yield of the encapsulated QDs, and QD leaking stability were used as measures for bead quality. The derived optimized bead encoding procedure enables the reproducible preparation of bright PS microbeads encoded with organic dyes as well as with CdSe/CdS-QDs. Although these beads show a reduced photoluminescence quantum yield compared to the initially very strongly luminescent QDs, with values of about 35%, their photoluminescence quantum yield is nevertheless still moderate.
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