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From parallel to single crystallization kinetics in high-density amorphous ice

机译:在高密度无定形冰中从平行结晶到单结晶动力学

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摘要

The isobaric transformation behavior of unannealed (uHDA) and expanded (eHDA) high-density amorphous ice at pressures up to 0.20 GPa is compared using powder x-ray diffraction and dilatometry. eHDA shows high thermal stability and crystallizes to a single ice phase only, whereas uHDA shows much lower thermal stability and always crystallizes to a mixture of ice phases. Unexpectedly, at low temperatures hexagonal ice grows first from uHDA, whereas this phase never crystallizes from eHDA. This leads us to conclude that hidden structural order in the form of nanocrystalline domains is present in uHDA, which triggers growth of hexagonal ice. By contrast, these ordered domains are absent in eHDA, which appears to be a homogeneous material and, thus, could be considered as a candidate for the low-temperature proxy of the proposed high-density liquid phase of water. The present work provides the basis for further experimental studies aiming at investigating this possibility since it establishes that the well-studied uHDA is not the right material to be studied in this context, whereas the more recently discovered eHDA is.
机译:使用粉末X射线衍射和膨胀法比较了未退火(uHDA)和膨胀(eHDA)高密度非晶冰在压力高达0.20 GPa时的等压转变行为。 eHDA显示出高的热稳定性,仅结晶成单一冰相,而uHDA显示出低得多的热稳定性,并始终结晶成冰相的混合物。出乎意料的是,在低温下,六方冰首先从uHDA中生长出来,而此相从未从eHDA中结晶出来。这使我们得出结论,uHDA中存在以纳米晶域形式存在的隐藏结构顺序,这会触发六角形冰的生长。相比之下,eHDA中似乎缺少这些有序域,而eHDA似乎是均质材料,因此可以被视为拟议的高密度水液相的低温替代物的候选者。当前的工作为进一步研究旨在研究这种可能性的实验提供了基础,因为它确定了经过充分研究的uHDA不是在这种情况下要研究的正确材料,而最近发现的eHDA是。

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