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Defect pair separation as the controlling step in homogeneous ice melting.

Abstract：

:On being heated, ice melts into liquid water. Although in practice this process tends to be heterogeneous, it can occur homogeneously inside bulk ice. The thermally induced homogeneous melting of solids is fairly well understood, and involves the formation and growth of melting nuclei. But in the case of water, resilient hydrogen bonds render ice melting more complex. We know that the first defects appearing during homogeneous ice melting are pairs of five- and seven-membered rings, which appear and disappear repeatedly and randomly in space and time in the crystalline ice structure. However, the accumulation of these defects to form an aggregate is nearly additive in energy, and results in a steep free energy increase that suppresses further growth. Here we report molecular dynamics simulations of homogeneous ice melting that identify as a crucial first step not the formation but rather the spatial separation of a defect pair. We find that once it is separated, the defect pair--either an interstitial (I) and a vacancy (V) defect pair (a Frenkel pair), or an L and a D defect pair (a Bjerrum pair)--is entropically stabilized, or 'entangled'. In this state, defects with threefold hydrogen-bond coordination persist and grow, and thereby prepare the system for subsequent rapid melting.

journal_name

Nature

journal_title

Nature

authors

Mochizuki K,Matsumoto M,Ohmine I

doi

10.1038/nature12190

subject

Has Abstract

pub_date

2013-06-20 00:00:00

pages

350-4

issue

7454

eissn

0028-0836

issn

1476-4687

pii

nature12190

journal_volume

498

pub_type

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