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Observation of a transition in the water-nanoparticle formation process at 167 K.

Rapid-scan Fourier transform infrared spectroscopy of the vapor/solid formation process of water nanoparticles in the 180-140 K temperature range at thermal-equilibrium conditions is reported. At 167 K a transition in the formation process was observed: the particle volume quintuples and the particle formation time triples within a temperature interval of +/-0.4 K caused by the temperature control. The authors interpret this behavior by an abrupt change in the nucleation rate of the H2O monomers in He buffer gas kept at 167 K and 200 mbar. A size and shape analysis of the particles during the formation process was carried out by application of the discrete dipole approximation method which delivers excellent accordance between experimental and calculated mid-IR spectra. Compared to other compact shapes (cube, prolate ellipsoid, and hexagonal prism) the ideal spherical shape fits the experimental spectra best. A distinct change in shape by particle conversion or agglomeration could be excluded to be involved in the formation process. As a possible explanation of the observed phenomenon, a transition from vapor/liquid/solid to vapor/solid nucleation with decreasing temperature is considered which was recently theoretically predicted by van Dongen and co-workers [J. Chem. Phys. 117, 5647 (2002); private communication; J. Chem. Phys. 120, 6314 (2004)].