Unprecedented generation of 3D heterostructures by mechanochemical disassembly and re-ordering of incommensurate metal chalcogenides

Oleksandr Dolotko, Ihor Z. Hlova, Arjun K. Pathak, Yaroslav Mudryk, Vitalij K. Pecharsky, Prashant Singh, Duane D. Johnson, Brett W. Boote, Jingzhe Li, Emily A. Smith, Scott L. Carnahan, Aaron J. Rossini, Lin Zhou, Ely M. Eastman and Viktor P. Balema ()
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Oleksandr Dolotko: Iowa State University
Ihor Z. Hlova: Iowa State University
Arjun K. Pathak: Iowa State University
Yaroslav Mudryk: Iowa State University
Vitalij K. Pecharsky: Iowa State University
Prashant Singh: Iowa State University
Duane D. Johnson: Iowa State University
Brett W. Boote: Iowa State University
Jingzhe Li: Iowa State University
Emily A. Smith: Iowa State University
Scott L. Carnahan: Iowa State University
Aaron J. Rossini: Iowa State University
Lin Zhou: Iowa State University
Ely M. Eastman: Iowa State University
Viktor P. Balema: Iowa State University

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract Three-dimensional heterostructures are usually created either by assembling two-dimensional building blocks into hierarchical architectures or using stepwise chemical processes that sequentially deposit individual monolayers. Both approaches suffer from a number of issues, including lack of suitable precursors, limited reproducibility, and poor scalability of the preparation protocols. Therefore, development of alternative methods that enable preparation of heterostructured materials is desired. We create heterostructures with incommensurate arrangements of well-defined building blocks using a synthetic approach that comprises mechanical disassembly and simultaneous reordering of layered transition-metal dichalcogenides, MX2, and non-layered monochalcogenides, REX, where M = Ta, Nb, RE = Sm, La, and X = S, Se. We show that the discovered solid-state processes are rooted in stochastic mechanochemical transformations directed by electronic interaction between chemically and structurally dissimilar solids toward atomic-scale ordering, and offer an alternative to conventional heterostructuring. Details of composition–structure–properties relationships in the studied materials are also highlighted.

Date: 2020
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DOI: 10.1038/s41467-020-16672-0

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