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Igniting homogeneous nucleation
Transient homogeneous nucleation is studied in the limit of large critical
sizes. Starting from pure monomers, three eras of transient nucleation are
characterized in the classic Becker-D\"oring kinetic equations with two
different models of discrete diffusivity: the classic Turnbull-Fisher formula
and an expression describing thermally driven growth of the nucleus. The latter
diffusivity yields time lags for nucleation which are much closer to values
measured in experiments with disilicate glasses. After an initial stage in
which the number of monomers decreases, many clusters of small size are
produced and a continuous size distribution is created. During the second era,
nucleii are increasing steadily in size in such a way that their distribution
appears as a wave front advancing towards the critical size for steady
nucleation. The nucleation rate at critical size is negligible during this era.
After the wave front reaches critical size, it ignites the creation of
supercritical clusters at a rate that increases monotonically until its steady
value is reached. Analytical formulas for the transient nucleation rate and the
time lag are obtained that improve classical ones and compare very well with
direct numerical solutions.Comment: 32 pages, 6 figures, to appear in Phys. Rev.
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