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Direct insight into the structure-property relation of interfaces from constrained crystal structure prediction

L. Sun, M. Marques, S. Botti

Nature Communications, 12, 811, (2021)

DOI: 10.1038/s41467-020-20855-0

Download: BibTEX

A major issue that prevents a full understanding of heterogeneous materials is the lack of systematic first-principles methods to consistently predict energetics and electronic properties of reconstructed interfaces. In this work we address this problem with an efficient and accurate computational scheme. We extend the minima-hopping method implementing constraints crafted for two-dimensional atomic relaxation and enabling variations of the atomic density close to the interface. A combination of density-functional and accurate density-functional tight-binding calculations supply energy and forces to structure prediction. We demonstrate the power of this method by applying it to extract structure-property relations for a large and varied family of symmetric and asymmetric tilt boundaries in polycrystalline silicon. We find a rich polymorphism in the interface reconstructions, with recurring bonding patterns that we classify in increasing energetic order. Finally, a clear relation between bonding patterns and electrically active grain boundary states is unveiled and discussed.

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{"type":"article", "name":"l.sun20212", "author":"L. Sun and M. Marques and S. Botti", "title":"Direct insight into the structureproperty relation of interfaces from constrained crystal structure prediction", "journal":"Nature Communications", "volume":"12", "OPTnumber":"1", "OPTmonth":"2", "year":"2021", "OPTpages":"811", "OPTnote":"", "OPTkey":"", "DOI":"10.1038/s41467-020-20855-0"}
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