Interface-Driven Structural Distortions and Composition Segregation in Two-Dimensional Heterostructures
Abstract
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 [(PbxSn1–xSe)1+δ]n(TiSe2)1 heterostructures using electron microscopy. This segregation is thermodynamically favored to occur when PbxSn1–xSe layers are interdigitated with TiSe2 monolayers. DFT calculations indicate that the observed segregation depends on what is adjacent to the PbxSn1–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.
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); National Institute of Standards and Technology (NIST)
- OSTI Identifier:
- 1399573
- Report Number(s):
- SAND-2017-10353J
Journal ID: ISSN 1433-7851; 657273
- Grant/Contract Number:
- AC04-94AL85000; AC05-76RL01830; DMR-1266217; DMR-1729613; 00095176; NA0003525
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 56; Journal Issue: 46; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 2D materials; heterostructures; monolayers; surface segregation; transition metal dichalcogenides
Citation Formats
Ditto, Jeffrey, Merrill, Devin R., Mitchson, Gavin, Gabriel, Joshua J., Mathew, Kiran, Hennig, Richard G., Medlin, Douglas L., Browning, Nigel D., and Johnson, David C. Interface-Driven Structural Distortions and Composition Segregation in Two-Dimensional Heterostructures. United States: N. p., 2017.
Web. doi:10.1002/anie.201707270.
Ditto, Jeffrey, Merrill, Devin R., Mitchson, Gavin, Gabriel, Joshua J., Mathew, Kiran, Hennig, Richard G., Medlin, Douglas L., Browning, Nigel D., & Johnson, David C. Interface-Driven Structural Distortions and Composition Segregation in Two-Dimensional Heterostructures. United States. https://doi.org/10.1002/anie.201707270
Ditto, Jeffrey, Merrill, Devin R., Mitchson, Gavin, Gabriel, Joshua J., Mathew, Kiran, Hennig, Richard G., Medlin, Douglas L., Browning, Nigel D., and Johnson, David C. Wed .
"Interface-Driven Structural Distortions and Composition Segregation in Two-Dimensional Heterostructures". United States. https://doi.org/10.1002/anie.201707270. https://www.osti.gov/servlets/purl/1399573.
@article{osti_1399573,
title = {Interface-Driven Structural Distortions and Composition Segregation in Two-Dimensional Heterostructures},
author = {Ditto, Jeffrey and Merrill, Devin R. and Mitchson, Gavin and Gabriel, Joshua J. and Mathew, Kiran and Hennig, Richard G. and Medlin, Douglas L. and Browning, Nigel D. and Johnson, David C.},
abstractNote = {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 [(PbxSn1–xSe)1+δ]n(TiSe2)1 heterostructures using electron microscopy. This segregation is thermodynamically favored to occur when PbxSn1–xSe layers are interdigitated with TiSe2 monolayers. DFT calculations indicate that the observed segregation depends on what is adjacent to the PbxSn1–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.},
doi = {10.1002/anie.201707270},
journal = {Angewandte Chemie (International Edition)},
number = 46,
volume = 56,
place = {United States},
year = {Wed Sep 06 00:00:00 EDT 2017},
month = {Wed Sep 06 00:00:00 EDT 2017}
}
Web of Science
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