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

Authors: L. Sun, M.A.L. Marques, and S. Botti

Ref.: Nat. Comm. 12, 811 (2021)

Abstract: A major issue that prevents a full understanding of heterogeneous materials is the lack of systematic first-principles methods to predict consistently both energetics and electronic properties of reconstructed interfaces. In this work we develop an efficient and accurate computational scheme aimed at solving this problem. Our approach is a variant of the minima-hopping method for global crystal structure prediction, conceived for quasi-two-dimensional systems. Specifically, we implement the minima hopping method with a constraint library crafted for two-dimensional atomic relaxation and we enable variations of the atomic density in proximity to the interface. A combination of density-functional and a highly accurate density-functional tight-binding calculations efficiently supply energy and forces to the structure prediction procedure. 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 reconstructions of the grain boundaries, with recurring bonding patterns that we classify in increasing energetic order. In several cases, we succeed in identifying atomic arrangements that are significantly more stable than previously predicted structures, while in other cases we show that the algorithm can recover, without experimental input, geometries that had been built by hand to match experimental data. Finally, a clear relation between bonding patterns and electrically active grain boundary states is unveiled and discussed.

Citations: 1 (Google scholar)

DOI: 10.1038/s41467-020-20855-0

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Bibtex:

@article{Sun_2021,
	doi = {10.1038/s41467-020-20855-0},
	url = {https://doi.org/10.1038%2Fs41467-020-20855-0},
	year = 2021,
	month = {feb},
	publisher = {Springer Science and Business Media {LLC}},
	volume = {12},
	number = {1},
	author = {Lin Sun and Miguel A. L. Marques and Silvana Botti},
	title = {Direct insight into the structure-property relation of interfaces from constrained crystal structure prediction},
	journal = {Nature Communications}
}