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Link between the diversity, heterogeneity and kinetic properties of amorphous ice structures

机译:无定形冰结构的多样性,异质性和动力学性质之间的联系

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摘要

Based on neutron wide-angle diffraction and small-angle neutron scattering experiments, we show that there is a correlation between the preparational conditions of amorphous ice structures, their microscopic structural properties, the extent of heterogeneities on a mesoscopic spatial scale and the transformation kinetics. There are only two modifications that can be identified as homogeneous disordered structures, namely the very high-density vHDA and the low-density amorphous LDA ice. Structures showing an intermediate static structure factor with respect to vHDA and LDA are heterogeneous phases. This holds independently from their preparation procedure, i.e. either obtained by pressure antorphization of ice I-h or by heating of vHDA. The degree of heterogeneity can be progressively suppressed when higher pressures and temperatures are applied for the sample preparation. In accordance with the suppressed heterogeneity the maximum of the static structure factor displays a pronounced narrowing of the first strong peak, shifting towards higher Q-numbers. Moreover, the less heterogeneous the obtained structures are the slower is the transformation kinetics from the high-density modifications into LDA. The well known high-density amorphous structure HDA does not constitute any particular state of the amorphous water network. It is formed due to the preparational procedure working in liquid nitrogen as thermal bath, i.e. at about 77 K. (c) 2006 Elsevier B.V. All rights reserved.
机译:基于中子广角衍射和小角中子散射实验,我们表明非晶态冰结构的制备条件,其微观结构性质,介观空间尺度上的不均匀程度与转化动力学之间存在相关性。只有两种修饰可以被识别为均质的无序结构,即非常高密度的vHDA和低密度无定形LDA冰。显示相对于vHDA和LDA的中间静态结构因子的结构是异质相。这与它们的制备方法无关,即通过冰I-h的压力胶凝或通过加热vHDA获得。当为样品制备施加更高的压力和温度时,可以逐步抑制异质性程度。根据抑制的异质性,静态结构因子的最大值显示出第一个强峰的明显变窄,向更高的Q值移动。而且,获得的结构越不均匀,从高密度修饰到LDA的转化动力学就越慢。众所周知的高密度非晶结构HDA不构成非晶水网络的任何特定状态。它的形成是由于在液氮中以热浴的方式进行的制备程序,即在约77 K下进行。(c)2006 Elsevier B.V.保留所有权利。

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