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Title: Breaking of Inversion Symmetry and Interlayer Electronic Coupling in Bilayer Graphene Heterostructure by Structural Implementation of High Electric Displacement Fields

Abstract

Controlling the interlayer coupling in two-dimensional (2D) materials generates novel electronic and topological phases. Its effective implementation is commonly done with a transverse electric field. However, phases generated by high displacement fields are elusive in this standard approach. Here, we introduce an exceptionally large displacement field by structural modification of a model system: AB-stacked bilayer graphene (BLG) on a SiC(0001) surface. We show that upon intercalation of gadolinium, electronic states in the top graphene layers exhibit a significant difference in the on-site potential energy, which effectively breaks the interlayer coupling between them. As a result, for energies close to the corresponding Dirac points, the BLG system behaves like two electronically isolated single graphene layers. This is proven by local scanning tunneling microscopy (STM)/spectroscopy, corroborated by density functional theory, tight binding, and multiprobe STM transport. Further, the work presents metal intercalation as a promising approach for the synthesis of 2D graphene heterostructures with electronic phases generated by giant displacement fields.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [3];  [4];  [5];  [1]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [3]
  1. Ames Lab., Ames, IA (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
  3. Ames Lab., and Iowa State Univ., Ames, IA (United States)
  4. Hainan University, Haikou (China)
  5. Southeast Univ., Nanjing (China)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1905244
Report Number(s):
IS-J-10,955
Journal ID: ISSN 1948-7185
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 13; Journal Issue: 49; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; graphene intercalation; epitaxial 2D materials; synthesis and processing; band structure manipulation; rare earths; scanning tunneling microscopy and spectroscopy

Citation Formats

Kolmer, Marek, Ko, Wonhee, Hall, Joseph, Chen, Shen, Zhang, Jianhua, Zhao, Haijun, Ke, Liqin, Wang, Cai-Zhuang, Li, An-Ping, and Tringides, Michael C. Breaking of Inversion Symmetry and Interlayer Electronic Coupling in Bilayer Graphene Heterostructure by Structural Implementation of High Electric Displacement Fields. United States: N. p., 2022. Web. doi:10.1021/acs.jpclett.2c02407.
Kolmer, Marek, Ko, Wonhee, Hall, Joseph, Chen, Shen, Zhang, Jianhua, Zhao, Haijun, Ke, Liqin, Wang, Cai-Zhuang, Li, An-Ping, & Tringides, Michael C. Breaking of Inversion Symmetry and Interlayer Electronic Coupling in Bilayer Graphene Heterostructure by Structural Implementation of High Electric Displacement Fields. United States. https://doi.org/10.1021/acs.jpclett.2c02407
Kolmer, Marek, Ko, Wonhee, Hall, Joseph, Chen, Shen, Zhang, Jianhua, Zhao, Haijun, Ke, Liqin, Wang, Cai-Zhuang, Li, An-Ping, and Tringides, Michael C. Thu . "Breaking of Inversion Symmetry and Interlayer Electronic Coupling in Bilayer Graphene Heterostructure by Structural Implementation of High Electric Displacement Fields". United States. https://doi.org/10.1021/acs.jpclett.2c02407. https://www.osti.gov/servlets/purl/1905244.
@article{osti_1905244,
title = {Breaking of Inversion Symmetry and Interlayer Electronic Coupling in Bilayer Graphene Heterostructure by Structural Implementation of High Electric Displacement Fields},
author = {Kolmer, Marek and Ko, Wonhee and Hall, Joseph and Chen, Shen and Zhang, Jianhua and Zhao, Haijun and Ke, Liqin and Wang, Cai-Zhuang and Li, An-Ping and Tringides, Michael C.},
abstractNote = {Controlling the interlayer coupling in two-dimensional (2D) materials generates novel electronic and topological phases. Its effective implementation is commonly done with a transverse electric field. However, phases generated by high displacement fields are elusive in this standard approach. Here, we introduce an exceptionally large displacement field by structural modification of a model system: AB-stacked bilayer graphene (BLG) on a SiC(0001) surface. We show that upon intercalation of gadolinium, electronic states in the top graphene layers exhibit a significant difference in the on-site potential energy, which effectively breaks the interlayer coupling between them. As a result, for energies close to the corresponding Dirac points, the BLG system behaves like two electronically isolated single graphene layers. This is proven by local scanning tunneling microscopy (STM)/spectroscopy, corroborated by density functional theory, tight binding, and multiprobe STM transport. Further, the work presents metal intercalation as a promising approach for the synthesis of 2D graphene heterostructures with electronic phases generated by giant displacement fields.},
doi = {10.1021/acs.jpclett.2c02407},
journal = {Journal of Physical Chemistry Letters},
number = 49,
volume = 13,
place = {United States},
year = {Thu Dec 08 00:00:00 EST 2022},
month = {Thu Dec 08 00:00:00 EST 2022}
}

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