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The Relation between Chemical Bonding and Ultrafast Crystal Growth

Accepted version
Peer-reviewed

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Authors

Lee, T 
Elliott, SR 

Abstract

Glasses are often described as supercooled liquids, whose structures are topologically disordered like a liquid, but nevertheless retain short-range structural order. Structural complexity is often associated with complicated electron-charge distributions in glassy systems, making a detailed investigation challenging even for short-range structural order, let alone their atomic dynamics. This is particularly problematic for lone-pair-rich, semiconducting materials, such as phase-change materials (PCMs). Here, this study shows that analytical methods for studying bonding, based on the electron-charge density, rather than a conventional atomic pair-correlation-function approach, allows an in-depth investigation into the chemical-bonding network, as well as lone pairs, of the prototypical PCM, Ge2Sb2Te5 (GST). It is demonstrated that the structurally flexible building units of the amorphous GST network, intimately linked to the presence of distinctly coexisting weak covalent and lone-pair interactions, give rise to cooperative structural-ordering processes, by which ultrafast crystal growth becomes possible. This finding may universally apply to other PCMs.

Description

Keywords

chemical bonding, crystal growth, DFT calculations, phase-change materials

Journal Title

Advanced Materials

Conference Name

Journal ISSN

0935-9648
1521-4095

Volume Title

Publisher

Wiley
Sponsorship
EPSRC (via University of Southampton) (EP/M015130/1)
Engineering and Physical Sciences Research Council (EP/M015130/1)
Engineering and Physical Sciences Research Council (EP/N022009/1)
Engineering and Physical Sciences Research Council (EP/I018050/1)
The authors acknowledge financial support from the Engineering and Physical Sciences Research Council (UK). The AIMD simulations were partially performed using the Cambridge High-Performance Computing Facility (Darwin).
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