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

Dolotko, Oleksandr
Hlova, Ihor
Pathak, Arjun
Mudryk, Yaroslav
Pecharsky, Vitalij
Singh, Prashant
Johnson, Duane
Boote, Brett
Li, Jingzhe
Smith, Emily
Carnahan, Scott
Rossini, Aaron
Zhou, Lin
Eastman, Ely
Balema, Viktor
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Ames Laboratory
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Physics and Astronomy
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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.


This article is published as Dolotko, Oleksandr, 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. "Unprecedented generation of 3D heterostructures by mechanochemical disassembly and re-ordering of incommensurate metal chalcogenides." Nature Communications 11 (2020): 3005. DOI: 10.1038/s41467-020-16672-0. Posted with permission.