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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Growth Dynamics of Crystalline Ar Hydrate
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Growth Dynamics of Crystalline Ar Hydrate

机译：结晶Ar水合物的生长动态

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The formation of a clathrate hydrate crystal is characterized by several steps, each of them distinguished by a different structural arrangement and temporal duration. A precise definition of these different forms is a challenging task, because the entirety of the formation dynamics spans over a time interval ranging from few nanoseconds to several days. Computational methods are powerful and essential to define the nucleation step, but they fail in providing a reliable picture of the long-range order establishment. On the other side, the experimental methods employed in the study of the growth dynamics usually monitor the hydrate growth at the interface with the fluid and thus are limited by the diffusion of the guest molecules through the newly formed hydrate phase. This problem is overcome here by the confinement of an argon hydrate sample in a sapphire anvil cell, allowing monitoring of the melting and crystallization of hydrates under moderate pressures by FTIR and Raman spectroscopies. This approach, besides providing a spectroscopic characterization of this hydrate, allowed the time windows characteristic of the formation of a macroscopic amorphous phase to be identified, possibly coincident with the so-called blob, and its rapid evolution toward the achievement of the local structure. Long-range ordering takes place on a longer time scale, most of it is realized in few hours but still evolving for weeks. No hints for supporting the so-called memory effect are gained through this study.
机译：克拉酸水合物晶体的形成特征在于几个步骤，每个步骤通过不同的结构布置和时间持续时间来区分。这些不同形式的精确定义是一个具有挑战性的任务，因为整个地层动力学跨越了几天内的时间间隔范围为几天。计算方法是强大的，可以定义成核步骤，但它们无法提供远程订单建立的可靠图像。另一方面，在生长动力学研究中使用的实验方法通常监测与流体界面处的水合物生长，因此受到客体分子通过新形成的水合物相的扩散的限制。这里通过在蓝宝石砧座细胞中限制氩水合物样品来克服该问题，允许通过FTIR和拉曼光谱法监测水合物在中等压力下的熔化和结晶。除了提供这种水合物的光谱表征之外，这种方法允许鉴定宏观非晶相的形成的时间窗特性，可能与所谓的斑点相吻合，并且其朝向局部结构的实现快速进化。长范围的命令在较长的时间尺度上进行，大部分时间都在几个小时内实现，但仍然在不断发展。通过本研究获得了支持所谓的记忆效应的提示。

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