An Approximate Criterion for Morphological Transformations in Small Vapor Grown Ice Crystals

J. Y. Harrington, G. Pokrifka
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Abstract

Observations and measurements show that crystals remain relatively compact at low ice supersaturations, but become increasingly hollowed and complex as the ice supersaturation rises. Prior measurements at temperatures >−25°C indicate that the transition from compact, solid ice to morphologically complex crystals occurs when the excess vapor density exceeds a threshold value of about 0.05 g m−3. A comparable threshold is not available at low temperatures. A temperature-dependent criterion for the excess vapor density threshold (Δρthr) that defines morphological transformations to complex ice is derived from laboratory measurements of vapor grown ice at temperatures below −40°C. This criterion depends on the difference between the equilibrium vapor density of liquid () and ice (ρei) multiplied by a measurement-determined constant, . The new criterion is consistent with prior laboratory measurements, theoretical estimates, and it reproduces the classical result of about 0.05 g m−3 above −25°C. Since Δρthr defines the excess vapor density above which crystals transition to a morphologically complex (lower density) growth mode, we can estimate the critical supersaturation (scrit) for step nucleation during vapor growth. The derived values of scrit are consistent with previous measurements at temperatures above −20°C. No direct measurements of scrit are available for temperatures below −40°C; however, our derived values suggest some measurement-based estimates may be too high while estimates from molecular dynamics simulations may be too low.
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小型蒸汽生长冰晶体形态变化的近似标准
观察和测量结果表明,在低冰过饱和度时,晶体保持相对紧凑,但随着冰过饱和度的升高,晶体变得越来越空洞和复杂。之前在温度大于 25°C 时进行的测量表明,当过量蒸汽密度超过约 0.05 g m-3 的临界值时,就会从紧密的实心冰转变为形态复杂的晶体。在低温条件下,还没有可比的临界值。过剩蒸汽密度阈值 (Δρthr)随温度变化的标准定义了向复杂冰的形态转变,该标准是通过对温度低于 -40°C 的蒸汽生长冰进行实验室测量得出的。该标准取决于液体()和冰的平衡蒸气密度(ρei)之间的差值乘以一个测量确定的常数,即 。新标准与之前的实验室测量结果和理论估计值一致,并且重现了-25°C 以上约 0.05 g m-3 的经典结果。由于 Δρthr 定义了晶体过渡到形态复杂(密度较低)生长模式的过高蒸汽密度,因此我们可以估算出蒸汽生长过程中阶跃成核的临界过饱和度 (scrit)。得出的 scrit 值与之前在 -20°C 以上温度条件下的测量值一致。然而,我们的推导值表明,一些基于测量的估计值可能过高,而分子动力学模拟的估计值可能过低。
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