Interface-Driven Structural Distortions and Composition Segregation in Two-Dimensional Heterostructures

Ditto, Jeffrey; Merrill, Devin R.; Mitchson, Gavin; Gabriel, Joshua J.; Mathew, Kiran; Hennig, Richard G.; Medlin, Douglas L.; Browning, Nigel D.; Johnson, David C.

doi:10.1002/anie.201707270

Interface-Driven Structural Distortions and Composition Segregation in Two-Dimensional Heterostructures

Journal Article · Wed Sep 06 00:00:00 EDT 2017 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201707270· OSTI ID:1399573

Ditto, Jeffrey ^[1]; Merrill, Devin R. ^[1]; Mitchson, Gavin ^[1]; Gabriel, Joshua J. ^[2]; Mathew, Kiran ^[2]; Hennig, Richard G. ^[2]; Medlin, Douglas L. ^[3]; Browning, Nigel D. ^[4]; ^[1]

Univ. of Oregon, Eugene, OR (United States)
Univ. of Florida, Gainesville, FL (United States)
Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

The discovery of emergent phenomena in 2D materials has sparked substantial research efforts in the materials community. A significant experimental challenge for this field is exerting atomistic control over the structure and composition of the constituent 2D layers and understanding how the interactions between layers drive both structure and properties. While no segregation for single bilayers was observed, segregation of Pb to the surface of three bilayer thick PbSe–SnSe alloy layers was discovered within [(Pb_xSn_1–xSe)_1+δ]_n(TiSe₂)₁ heterostructures using electron microscopy. This segregation is thermodynamically favored to occur when Pb_xSn_1–xSe layers are interdigitated with TiSe₂ monolayers. DFT calculations indicate that the observed segregation depends on what is adjacent to the Pb_xSn_1–xSe layers. As a result, the interplay between interface- and volume-free energies controls both the structure and composition of the constituent layers, which can be tuned using layer thickness.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: National Institute of Standards and Technology (NIST); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000; AC05-76RL01830; NA0003525

OSTI ID:: 1399573

Report Number(s):: SAND--2017-10353J; 657273

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 46 Vol. 56; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
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