Designing intermediate-range order in amorphous materials

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Abstract

Amorphous materials are commonly understood to consist of random organizations of molecular-type structural units. However, it has long been known that structural organizations intermediate between discrete chemical bonds and periodic crystalline lattices are present even in liquids1,2. Numerous models—including random networks and crystalline-type structures with networks composed of clusters3,4 and voids5,6—have been proposed to account for this intermediate-range order7. Nevertheless, understanding and controlling structural features that determine intermediate-range order in amorphous materials remain fundamental, yet presently unresolved, issues7,8,9. The most characteristic signature of such order is the first peak in the total structure factor, referred to as the first sharp diffraction peak or ‘low Q’ structure. These features correspond to large real-space distances in the materials, and understanding their origin is key to unravelling details of intermediate-range order. Here we employ principles of crystal engineering to design specific patterns of intermediate-range order within amorphous zinc-chloride networks. Using crystalline models, we demonstrate the impact of various structural features on diffraction at low values of Q. Such amorphous network engineering is anticipated to provide the structure/property relationships necessary to tailor specific optical, electronic and mechanical properties.

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Figure 1: Structural models of templates and networks.
Figure 2: Total structure factors and power diffraction patterns for amorphous materials and crystalline models.

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Acknowledgements

The assistance of GLAD-IPNS beamline scientists Y. Badyal and C. Benmore is gratefully acknowledged. This work was supported by the NSF, and the US DOE-BES Division of Materials Sciences. J. D. M. is a Cottrell Scholar of the Research Corporation.

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Correspondence to James D. Martin.

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A US patent title “Templated Compositions of Inorganic Liquids and Glasses” has been filed by J.D.M. and North Carolina State University.

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Martin, J., Goettler, S., Fossé, N. et al. Designing intermediate-range order in amorphous materials. Nature 419, 381–384 (2002) doi:10.1038/nature01022

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