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Title: Large Area Atomically Flat Surfaces via Exfoliation of Bulk Bi2Se3 Single Crystals

Abstract

In this paper, we present an exfoliation method that produces cm2-area atomically flat surfaces from bulk layered single crystals, with broad applications such as for the formation of lateral heterostructures and for use as substrates for van der Waals epitaxy. Single crystals of Bi2Se3 were grown using the Bridgman method and examined with X-ray reciprocal space maps, Auger spectroscopy, low-energy electron diffraction, and X-ray photoelectron spectroscopy. An indium-bonding exfoliation technique was developed that produces multiple ~100 um thick atomically flat, macroscopic (>1 cm2) slabs from each Bi2Se3 source crystal. Two-dimensional X-ray diffraction and reciprocal space maps confirm the high crystalline quality of the exfoliated surfaces. Atomic force microscopy reveals that the exfoliated surfaces have an average root-mean-square (RMS) roughness of ~0.04 nm across 400 μm2 scans and an average terrace width of 70 um between step edges. First-principles calculations reveal exfoliation energies of Bi2Se3 and a number of other layered compounds, which demonstrate relevance of our method across the field of 2D materials. While many potential applications exist, excellent lattice matching with the III-V alloy space suggests immediate potential for the use of these exfoliated layered materials as epitaxial substrates for photovoltaic development.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1];  [1];  [3]; ORCiD logo [3];  [1];  [3];  [3];  [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
  2. Colorado School of Mines, Golden, CO (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Solar Energy Technologies Office (EE-4S), SunShot National Laboratory Multiyear Partnership (SuNLaMP)
OSTI Identifier:
1400368
Report Number(s):
NREL/JA-5K00-70317
Journal ID: ISSN 0897-4756
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 19; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; exfoliation; crystals; substrates; epitaxy

Citation Formats

Melamed, Celeste L., Ortiz, Brenden R., Gorai, Prashun, Martinez, Aaron D., McMahon, William E., Miller, Elisa M., Stevanovic, Vladan, Tamboli, Adele C., Norman, Andrew G., and Toberer, Eric S. Large Area Atomically Flat Surfaces via Exfoliation of Bulk Bi2Se3 Single Crystals. United States: N. p., 2017. Web. doi:10.1021/acs.chemmater.7b03198.
Melamed, Celeste L., Ortiz, Brenden R., Gorai, Prashun, Martinez, Aaron D., McMahon, William E., Miller, Elisa M., Stevanovic, Vladan, Tamboli, Adele C., Norman, Andrew G., & Toberer, Eric S. Large Area Atomically Flat Surfaces via Exfoliation of Bulk Bi2Se3 Single Crystals. United States. https://doi.org/10.1021/acs.chemmater.7b03198
Melamed, Celeste L., Ortiz, Brenden R., Gorai, Prashun, Martinez, Aaron D., McMahon, William E., Miller, Elisa M., Stevanovic, Vladan, Tamboli, Adele C., Norman, Andrew G., and Toberer, Eric S. Tue . "Large Area Atomically Flat Surfaces via Exfoliation of Bulk Bi2Se3 Single Crystals". United States. https://doi.org/10.1021/acs.chemmater.7b03198. https://www.osti.gov/servlets/purl/1400368.
@article{osti_1400368,
title = {Large Area Atomically Flat Surfaces via Exfoliation of Bulk Bi2Se3 Single Crystals},
author = {Melamed, Celeste L. and Ortiz, Brenden R. and Gorai, Prashun and Martinez, Aaron D. and McMahon, William E. and Miller, Elisa M. and Stevanovic, Vladan and Tamboli, Adele C. and Norman, Andrew G. and Toberer, Eric S.},
abstractNote = {In this paper, we present an exfoliation method that produces cm2-area atomically flat surfaces from bulk layered single crystals, with broad applications such as for the formation of lateral heterostructures and for use as substrates for van der Waals epitaxy. Single crystals of Bi2Se3 were grown using the Bridgman method and examined with X-ray reciprocal space maps, Auger spectroscopy, low-energy electron diffraction, and X-ray photoelectron spectroscopy. An indium-bonding exfoliation technique was developed that produces multiple ~100 um thick atomically flat, macroscopic (>1 cm2) slabs from each Bi2Se3 source crystal. Two-dimensional X-ray diffraction and reciprocal space maps confirm the high crystalline quality of the exfoliated surfaces. Atomic force microscopy reveals that the exfoliated surfaces have an average root-mean-square (RMS) roughness of ~0.04 nm across 400 μm2 scans and an average terrace width of 70 um between step edges. First-principles calculations reveal exfoliation energies of Bi2Se3 and a number of other layered compounds, which demonstrate relevance of our method across the field of 2D materials. While many potential applications exist, excellent lattice matching with the III-V alloy space suggests immediate potential for the use of these exfoliated layered materials as epitaxial substrates for photovoltaic development.},
doi = {10.1021/acs.chemmater.7b03198},
journal = {Chemistry of Materials},
number = 19,
volume = 29,
place = {United States},
year = {Tue Sep 12 00:00:00 EDT 2017},
month = {Tue Sep 12 00:00:00 EDT 2017}
}

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