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Absence of amorphous forms when ice is compressed at low temperature

机译：当冰在低温下压缩时不存在无定形形式

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Amorphous water ice comes in at least three distinct structural forms, all lacking long-range crystalline order. High-density amorphous ice (HDA) was first produced by compressing ice I to 11 kilobar at temperatures below 130 kelvin, and the process was described as thermodynamic melting(1), implying that HDA is a glassy state of water. This concept, and the ability to transform HDA reversibly into low-density amorphous ice, inspired the two-liquid water model, which relates the amorphous phases to two liquid waters in the deeply supercooled regime (below 228 kelvin) to explain many of the anomalies of water(2) (such as density and heat capacity anomalies). However, HDA formation has also been ascribed3 to a mechanical instability causing structural collapse and associated with kinetics too sluggish for recrystallization to occur. This interpretation is supported by simulations(3), analogy with a structurally similar system(4), and the observation of lattice-vibration softening as ice is compressed(5,6). It also agrees with recent observations of ice compression at higher temperatures-in the 'no man's land' regime, between 145 and 200 kelvin, where kinetics are faster-resulting in crystalline phases(7,8). Here we further probe the role of kinetics and show that, if carried out slowly, compression of ice I even at 100 kelvin (a region in which HDA typically forms) gives proton-ordered, but non-interpenetrating, ice IX', then proton-ordered and interpenetrating ice XV', and finally ice VIII'. By contrast, fast compression yields HDA but no ice IX, and direct transformation of ice I to ice XV' is structurally inhibited. These observations suggest that HDA formation is a consequence of a kinetically arrested transformation between low-density ice I and high-density ice XV' and challenge theories that connect amorphous ice to supercooled liquid water.
机译：无定形水冰至少有三种不同的结构形式，缺乏远程晶体顺序。首先通过在低于130 kelvin的温度下压缩冰I至11千巴岩生产高密度无定形冰（HDA），并且该方法被描述为热力学熔融（1），这意味着HDA是玻璃状水状态。这种概念，以及转换HDA的能力可逆地进入低密度无定形冰，启发了双液体水模型，它将无定形阶段与两种液体水域相关联（低于228kelvin）以解释许多异常的异常水（2）（如密度和热容异常）。然而，HDA形成也已归因于机械不稳定，导致结构崩溃，与动力学相关的，用于再结晶的转贷过于缓慢。这些解释是通过模拟（3）的支持，与结构类似的系统（4）进行类比，并且作为冰的晶格振动软化的观察被压缩（5,6）。它还同意最近在较高温度下的冰压缩观察 - 在“没有人的土地”制度中，在145到200个开尔文之间，其中动力学较快导致结晶阶段（7,8）。在这里，我们进一步探讨了动力学的作用，并表明，如果慢慢地进行，即使在100个开尔文（通常是形成HDA的区域）给予质子有序，但不互通，冰Ix'的压缩均匀的冰I甚至的压缩甚至的压缩甚至的冰I甚至压缩。 - 冰和互相冰XV'，最后冰六。相比之下，快速压缩产生HDA但没有冰IX，并且在结构上抑制了冰XV的直接转变。这些观察结果表明，HDA形成是低密度冰I和高密度冰XV'与将无定形冰连接到过冷液体水的攻击理论之间的动力学变化的结果。

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  • 来源
    《Nature》 |2019年第7757期|542-545|共4页
  • 作者

    Tulk Chris A.; Molaison Jamie J.; Makhluf Adam R.; Manning Craig E.; Klug Dennis D.;

  • 作者单位

    Oak Ridge Natl Lab Neutron Sci Directorate Oak Ridge TN 37830 USA;

    Oak Ridge Natl Lab Neutron Sci Directorate Oak Ridge TN 37830 USA;

    Univ Calif Los Angeles Dept Earth Planetary & Space Sci Los Angeles CA USA;

    Univ Calif Los Angeles Dept Earth Planetary & Space Sci Los Angeles CA USA;

    Natl Res Council Canada Ottawa ON Canada;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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