Monday, 31 October 2005 - 12:30 PM
73a
The Properties of Small Water Clusters from Isothermal Nucleation Rate Measurements
Barbara E. Wyslouzil1, Yoojeong Kim
2, Gerald Wilemski
3, Judith Wölk
4, and Reinhard Strey
4. (1) Chemical and Biomolecular Engineering, The Ohio State University, 140 W 19th Avenue, Columbus, OH 43210, (2) Chemical Engineering, Worcester Polytechnic Institute, 100 Institute Road, Worcester, MA 01609, (3) Physics, University of Missouri - Rolla, Rolla, MO 65409, (4) Institut für Physikalische Chemie, Universität zu Köln, 116 Luxemburgerstrasse, Köln, Germany
We have made direct measurements of the stationary, homogeneous nucleation rates, J=N/Δt, in supersonic Laval nozzles. The number densities, N, of droplets formed are measured using small angle neutron scattering (SANS) experiments and the time intervals during which nucleation occurs, Δt <10 μs, are derived from static pressure measurements along the axis of the nozzle. By using nozzles with different expansion rates, we obtain the first isothermal nucleation rate measurements as a function of supersaturation for these devices with a relatively small error margin in J of +/-50%. At temperatures T of 210, 220, and 230 K, the maximum nucleation rates for D2O range between 4•1016< J /cm-3s-1 < 3•1017 for supersaturations S ranging from 46 to 143. Applying the first and second nucleation theorems to isothermal nucleation rate data directly yields estimates for the number of molecules in the critical cluster n* and the excess internal energy Ex(n*), respectively. The agreement between these values and the classical values predicted assuming the critical cluster is a compact spherical object are really quite good even though under our conditions n* is less than 10 and the water is highly supercooled.
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