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Title: Atomic-resolution visualization and doping effects of complex structures in intercalated bilayer graphene

Abstract

Molecules intercalating two-dimensional materials form complex structures that have been characterized primarily by spatially averaged techniques. In this work, we use aberration-corrected scanning transmission electron microscopy and density-functional-theory (DFT) calculations to study the atomic structure of bilayer graphene (BLG) and few-layer graphene (FLG) intercalated with FeC l 3 . In BLG, we discover two distinct intercalated structures that we identify as monolayer FeC l 3 and monolayer FeC l 2 . The two structures are separated by atomically sharp boundaries and induce large free-carrier densities on the order of 10 13 c m - 2 in the graphene layers. In FLG, we observe multiple FeC l 3 layers stacked in a variety of possible configurations with respect to one another. Lastly, we find that the microscope's electron beam can convert the FeC l 3 monolayer into FeOCl monolayers in a rectangular lattice. These results reveal the need for a combination of atomically resolved microscopy, spectroscopy, and DFT calculations to identify intercalated structures and study their properties.

Authors:
 [1];  [1];  [2];  [3];  [1];  [4];  [4];  [4];  [5];  [1];  [3];  [1]
  1. Vanderbilt Univ., Nashville, TN (United States)
  2. Vanderbilt Univ., Nashville, TN (United States); Chinese Academy of Sciences (CAS), Beijing (China)
  3. Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Freie Univ., Berlin (Germany)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF); European Research Council (ERC)
OSTI Identifier:
1597942
Alternate Identifier(s):
OSTI ID: 1546419
Grant/Contract Number:  
[FG02-09ER46554; AC05-00OR22725; ACI-1053575]
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
[ Journal Volume: 3; Journal Issue: 6]; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Bonacum, Jason P., O’Hara, Andrew, Bao, De-Liang, Ovchinnikov, Oleg S., Zhang, Yan-Fang, Gordeev, Georgy, Arora, Sonakshi, Reich, Stephanie, Idrobo, Juan-Carlos, Haglund, Richard F., Pantelides, Sokrates T., and Bolotin, Kirill I. Atomic-resolution visualization and doping effects of complex structures in intercalated bilayer graphene. United States: N. p., 2019. Web. doi:10.1103/PhysRevMaterials.3.064004.
Bonacum, Jason P., O’Hara, Andrew, Bao, De-Liang, Ovchinnikov, Oleg S., Zhang, Yan-Fang, Gordeev, Georgy, Arora, Sonakshi, Reich, Stephanie, Idrobo, Juan-Carlos, Haglund, Richard F., Pantelides, Sokrates T., & Bolotin, Kirill I. Atomic-resolution visualization and doping effects of complex structures in intercalated bilayer graphene. United States. doi:10.1103/PhysRevMaterials.3.064004.
Bonacum, Jason P., O’Hara, Andrew, Bao, De-Liang, Ovchinnikov, Oleg S., Zhang, Yan-Fang, Gordeev, Georgy, Arora, Sonakshi, Reich, Stephanie, Idrobo, Juan-Carlos, Haglund, Richard F., Pantelides, Sokrates T., and Bolotin, Kirill I. Fri . "Atomic-resolution visualization and doping effects of complex structures in intercalated bilayer graphene". United States. doi:10.1103/PhysRevMaterials.3.064004.
@article{osti_1597942,
title = {Atomic-resolution visualization and doping effects of complex structures in intercalated bilayer graphene},
author = {Bonacum, Jason P. and O’Hara, Andrew and Bao, De-Liang and Ovchinnikov, Oleg S. and Zhang, Yan-Fang and Gordeev, Georgy and Arora, Sonakshi and Reich, Stephanie and Idrobo, Juan-Carlos and Haglund, Richard F. and Pantelides, Sokrates T. and Bolotin, Kirill I.},
abstractNote = {Molecules intercalating two-dimensional materials form complex structures that have been characterized primarily by spatially averaged techniques. In this work, we use aberration-corrected scanning transmission electron microscopy and density-functional-theory (DFT) calculations to study the atomic structure of bilayer graphene (BLG) and few-layer graphene (FLG) intercalated with FeCl3. In BLG, we discover two distinct intercalated structures that we identify as monolayer FeCl3 and monolayer FeCl2. The two structures are separated by atomically sharp boundaries and induce large free-carrier densities on the order of 1013cm-2 in the graphene layers. In FLG, we observe multiple FeCl3 layers stacked in a variety of possible configurations with respect to one another. Lastly, we find that the microscope's electron beam can convert the FeCl3 monolayer into FeOCl monolayers in a rectangular lattice. These results reveal the need for a combination of atomically resolved microscopy, spectroscopy, and DFT calculations to identify intercalated structures and study their properties.},
doi = {10.1103/PhysRevMaterials.3.064004},
journal = {Physical Review Materials},
number = [6],
volume = [3],
place = {United States},
year = {2019},
month = {6}
}

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