6533b7d4fe1ef96bd12627c5

RESEARCH PRODUCT

Nucleation kinetics in deionized charged colloidal model systems: A quantitative study by means of classical nucleation theory

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We have studied the nucleation kinetics of charged colloidal model systems under salt free conditions crystallizing in bcc structure covering a wide range of particle number densities $18\phantom{\rule{0.3em}{0ex}}\mathrm{\ensuremath{\mu}}{\mathrm{m}}^{\ensuremath{-}3}\ensuremath{\le}n\ensuremath{\le}66.3\phantom{\rule{0.3em}{0ex}}\mathrm{\ensuremath{\mu}}{\mathrm{m}}^{\ensuremath{-}3}$. We employed direct video-microscopic observation of individual nucleation events to obtain time resolved nucleation rate densities. Polarization microscopy and static light scattering on the resulting solids in combination with Avrami theory is used to determine the steady state nucleation rate at high undercoolings. The final nucleation rate densities $J$ from different methods are observed to be consistent with each other. By increasing the difference in the chemical potential between melt and crystal $\mathrm{\ensuremath{\Delta}}\mathrm{\ensuremath{\mu}}$ about one order of magnitude $J$ increases from ${10}^{9}\phantom{\rule{0.3em}{0ex}}{\mathrm{m}}^{\ensuremath{-}3}{\mathrm{s}}^{\ensuremath{-}1}$ to ${10}^{17}\phantom{\rule{0.3em}{0ex}}{\mathrm{m}}^{\ensuremath{-}3}{\mathrm{s}}^{\ensuremath{-}1}$ over approximately seven orders of magnitude. The data can be well analyzed and interpreted using classical nucleation theory (CNT) leading to a linearly increasing melt-crystal surface tension. Surprisingly, the reduced surface tension is about one order of magnitude larger compared to other system (metals; hard sphere colloids). The critical radius of the crystal nuclei is decreasing down to a very small value of 1.5 coordination shells. The determined kinetic prefactors are up to 10 orders of magnitude smaller than the prefactor calculated by CNT.