Water nucleation at extreme supersaturation.
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Lippe M
Laboratory of Physical Chemistry, ETH Zürich, Vladimir-Prelog Weg 2, CH-8093 Zürich, Switzerland.
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Chakrabarty S
Laboratory of Physical Chemistry, ETH Zürich, Vladimir-Prelog Weg 2, CH-8093 Zürich, Switzerland.
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Ferreiro JJ
Laboratory of Physical Chemistry, ETH Zürich, Vladimir-Prelog Weg 2, CH-8093 Zürich, Switzerland.
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Tanaka KK
Institute of Low Temperature Science, Hokkaido University, Sapporo 060-0819, Japan.
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Signorell R
Laboratory of Physical Chemistry, ETH Zürich, Vladimir-Prelog Weg 2, CH-8093 Zürich, Switzerland.
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Published in:
- The Journal of chemical physics. - 2018
English
We report water cluster formation in the uniform postnozzle flow of a Laval nozzle at low temperatures of 87.0 and 47.5 K and high supersaturations of lnS ∼ 41 and 104, respectively. Cluster size distributions were measured after soft single-photon ionization at 13.8 eV with mass spectrometry. Critical cluster sizes were determined from cluster size distributions recorded as a function of increasing supersaturation, resulting in critical sizes of 6-15 and 1, respectively. Comparison with previous data for propane and toluene reveals a systematic trend in the nucleation behavior, i.e., a change from a steplike increase to a gradual increase of the maximum cluster size with increasing supersaturation. Experimental nucleation rates of 5 · 1015 cm-3 s-1 and 2 · 1015 cm-3 s-1 for lnS ∼ 41 and 104, respectively, were retrieved from cluster size distributions recorded as a function of nucleation time. These lie 2-3 orders of magnitude below the gas kinetic collision limit assuming unit sticking probability, but they agree very well with a recent prediction by a master equation model based on ab initio transition state theory. The experimental observations are consistent with barrierless growth at 47.5 K, but they hint at a more complex nucleation behavior for the measurement at 87.0 K.
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green
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https://sonar.ch/global/documents/100825
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