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On the self-purification cascade during crystal growth from solution

机译：从溶液中晶体生长过程中的自纯化级联

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We report on the failure of the Cabrera-Vermilyea (CV) step pinning model to reproduce the elementary step kinetics for the case of tetragonal lysozyme crystals growing from contaminated solutions. We measured the supersaturation dependency of the step velocity using confocal microscopy for three different commercially available lysozyme batches with varying levels of impurity content, that is, Seikagaku, Fluka, and Sigma. Strong nonlinear dependencies are obtained in the high to intermediate supersaturation range and near-linear dependencies at lower driving forces. The clear absence of a dead zone for the Fluka and Seikagaku data is in direct contradiction to the CV model. As such, we developed a time-dependent impurity model based on Bliznakov kinetics assuming Langmuir adsorption. Admissible fits are obtained for Fluka and Seikagaku lysozyme corroborating the self-purification interpretation due to the diminishing terrace exposure times at higher supersaturation levels. The steeper recovery toward pure kinetics for Sigma lysozyme than predicted by Langmuir adsorption prompted us to expand the model to allow for impurity-impurity interaction. The resultant kinetic model, which assumes a Kisliuk-like mode of impurity adsorption, did yield acceptable fits with Sigma step kinetics. This Bliznakov-Kisliuk model also predicts clustering of impurity molecules on the surface, which is corroborated by our in situ experimental atomic force microscopy observations.
机译：我们报告的Cabrera-Vermilyea（CV）步骤钉扎模型的失败，无法再现从污染溶液中生长的四方溶菌酶晶体的基本步骤动力学。我们使用共聚焦显微镜对三种不同杂质含量水平的市售溶菌酶批次进行了共聚焦显微镜测量，测量了步速的过饱和依赖性，这些批次的杂质含量不同，分别为Seikagaku，Fluka和Sigma。在高到中级的过饱和度范围内获得强的非线性相关性，在较低的驱动力下获得接近线性的相关性。 Fluka和Seikagaku数据显然没有死区，这与CV模型直接矛盾。因此，我们在假设Langmuir吸附的基础上，基于Bliznakov动力学开发了时间相关的杂质模型。对于Fluka和Seikagaku溶菌酶，由于在较高的过饱和度水平下平台暴露时间减少而获得了可证实的拟合，从而佐证了自我纯化的解释。 Sigma溶菌酶向纯动力学的恢复比Langmuir吸附预测的要陡峭，这促使我们扩展模型以允许杂质与杂质的相互作用。所得的动力学模型（假设采用Kisliuk样的杂质吸附模式）确实产生了与Sigma阶跃动力学相符的可接受的拟合。这种Bliznakov-Kisliuk模型还预测了表面上杂质分子的聚集，这在我们的原位实验原子力显微镜观察中得到了证实。

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