Angular intensity of nonequilibrium interfacial dynamic light scattering: Succinonitrile and naphthalene

We have investigated the phenomenon of intense dynamic light scattering at the nonequilibrium crystal-melt interface in succinonitrile and naphthalene, in order to resolve the ongoing controversy over its origin. Of the several models that have been proposed to explain this phenomenon, the microbubble model of H. Z. Cummins et al. [Solid State Commun. 60, 857 (1986)] and the mesophase model proposed by J. Bilgram and co-workers [P. Boni, J. H. Bilgram, and W. Kanzig, Phys. Rev. A 28, 2953 (1983)] are the only two still considered to be consistent with most of the experimental observations. In these experiments the angular dependence of the scattered light was investigated. In the mesophase model the angular dependence of the scattered light is described by the Ornstein-Zernike form I(q)=${\mathit{I}}_0$(1+${\mathit{q}}^2$ ${\xi }^2$ ${)}^{\mathrm{-}1}$, whereas light scattered by bubbles can be modeled by the Mie scattering theory. The data for both materials were found to be incompatible with the Ornstein-Zernike form, but could be reasonably well fit by the Mie theory. The behavior of the onset of scattering was also investigated, and it was found that the product ${\mathit{R}}_0$ ${\mathit{t}}_0$ ${\mathit{v}}_{\mathit{g}}^2$ was a constant, where ${\mathit{R}}_0$ is the onset radius, ${\mathit{t}}_0$ the onset time, and ${\mathit{v}}_{\mathit{g}}$ the crystal growth velocity. This result is consistent with the analysis of Mesquita et al. [Phys. Rev. B 38, 1550 (1988)], in which the onset of the scattering was modeled by considering the rate of buildup of dissolved gas at the advancing crystal-melt interface. The time taken for the disappearance of the scattering after growth was terminated was also investigated. Lastly, the gases dissolved in our samples of succinonitrile were identified by mass spectroscopy and found to have a composition similar to air.