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Title: Highly Asymmetric Graphene Layer Doping and Band Structure Manipulation in Rare Earth–Graphene Heterostructure by Targeted Bonding of the Intercalated Gadolinium

Abstract

Heterostructures consisting of vertically stacked two-dimensional (2D) materials have recently gained large attention due to their highly controllable electronic properties and resulting quantum phases. In contrast to the mechanically stacked multilayered systems, which offer exceptional control over a stacking sequence or interlayer twist angles, the epitaxially grown 2D materials express unprecedented quality and stability over wafer-scale lengths. However, controlling the growth conditions remains a major obstacle toward the formation of complex, epitaxial heterostructures with well-defined electronic properties. Here, we synthesized a trilayer graphene heterostructure on the SiC(0001) substrate with two specific interlayer locations occupied by gadolinium. We applied multitechnique methodology based on low-temperature scanning tunneling microscopy/spectroscopy (STM/S) and angle-resolved photoelectron spectroscopy (ARPES) to determine the intercalant’s locations in the complex, epitaxial graphene heterostructure. Our approach relies on very high quality and large, micrometer-scale homogeneity of the synthesized system. The experimentally determined electronic structure is dominated by the two topmost graphene layers. Overall, our spectroscopic results show quantitative agreement between global ARPES, local STM/S, and density functional theory predictions. The characterized electronic properties primarily reflect highly anisotropic doping levels between the two corresponding graphene layers, which significantly affect the band structure topology. Two pairs of hybridized massive Dirac bands from ourmore » initial synthesis–the bilayer graphene on the SiC(0001) substrate–are transformed upon Gd intercalation into two pairs of massless Dirac bands with a new hybridization region in between. Our results open perspectives in the realization of exotic 2D quantum materials via atomically precise synthesis of epitaxial, multilayered graphene–rare earth heterostructures.« less

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [2]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. Ames Lab., and Iowa State Univ., Ames, IA (United States)
  2. Hainan Univ., Haikou (China)
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1856815
Alternate Identifier(s):
OSTI ID: 1856830
Report Number(s):
IS-J 10,757; IS-J 10745
Journal ID: ISSN 1932-7447
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 126; Journal Issue: 15; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Electronic structure; layers; two dimensional materials; intercalation; scanning tunneling microscopy

Citation Formats

Kolmer, Marek, Schrunk, Benjamin, Hupalo, Myron, Hall, Joseph, Chen, Shen, Zhang, Jianhua, Wang, Cai-Zhuang, Kaminski, Adam, and Tringides, Michael C. Highly Asymmetric Graphene Layer Doping and Band Structure Manipulation in Rare Earth–Graphene Heterostructure by Targeted Bonding of the Intercalated Gadolinium. United States: N. p., 2022. Web. doi:10.1021/acs.jpcc.2c01332.
Kolmer, Marek, Schrunk, Benjamin, Hupalo, Myron, Hall, Joseph, Chen, Shen, Zhang, Jianhua, Wang, Cai-Zhuang, Kaminski, Adam, & Tringides, Michael C. Highly Asymmetric Graphene Layer Doping and Band Structure Manipulation in Rare Earth–Graphene Heterostructure by Targeted Bonding of the Intercalated Gadolinium. United States. https://doi.org/10.1021/acs.jpcc.2c01332
Kolmer, Marek, Schrunk, Benjamin, Hupalo, Myron, Hall, Joseph, Chen, Shen, Zhang, Jianhua, Wang, Cai-Zhuang, Kaminski, Adam, and Tringides, Michael C. Mon . "Highly Asymmetric Graphene Layer Doping and Band Structure Manipulation in Rare Earth–Graphene Heterostructure by Targeted Bonding of the Intercalated Gadolinium". United States. https://doi.org/10.1021/acs.jpcc.2c01332. https://www.osti.gov/servlets/purl/1856815.
@article{osti_1856815,
title = {Highly Asymmetric Graphene Layer Doping and Band Structure Manipulation in Rare Earth–Graphene Heterostructure by Targeted Bonding of the Intercalated Gadolinium},
author = {Kolmer, Marek and Schrunk, Benjamin and Hupalo, Myron and Hall, Joseph and Chen, Shen and Zhang, Jianhua and Wang, Cai-Zhuang and Kaminski, Adam and Tringides, Michael C.},
abstractNote = {Heterostructures consisting of vertically stacked two-dimensional (2D) materials have recently gained large attention due to their highly controllable electronic properties and resulting quantum phases. In contrast to the mechanically stacked multilayered systems, which offer exceptional control over a stacking sequence or interlayer twist angles, the epitaxially grown 2D materials express unprecedented quality and stability over wafer-scale lengths. However, controlling the growth conditions remains a major obstacle toward the formation of complex, epitaxial heterostructures with well-defined electronic properties. Here, we synthesized a trilayer graphene heterostructure on the SiC(0001) substrate with two specific interlayer locations occupied by gadolinium. We applied multitechnique methodology based on low-temperature scanning tunneling microscopy/spectroscopy (STM/S) and angle-resolved photoelectron spectroscopy (ARPES) to determine the intercalant’s locations in the complex, epitaxial graphene heterostructure. Our approach relies on very high quality and large, micrometer-scale homogeneity of the synthesized system. The experimentally determined electronic structure is dominated by the two topmost graphene layers. Overall, our spectroscopic results show quantitative agreement between global ARPES, local STM/S, and density functional theory predictions. The characterized electronic properties primarily reflect highly anisotropic doping levels between the two corresponding graphene layers, which significantly affect the band structure topology. Two pairs of hybridized massive Dirac bands from our initial synthesis–the bilayer graphene on the SiC(0001) substrate–are transformed upon Gd intercalation into two pairs of massless Dirac bands with a new hybridization region in between. Our results open perspectives in the realization of exotic 2D quantum materials via atomically precise synthesis of epitaxial, multilayered graphene–rare earth heterostructures.},
doi = {10.1021/acs.jpcc.2c01332},
journal = {Journal of Physical Chemistry. C},
number = 15,
volume = 126,
place = {United States},
year = {Mon Mar 21 00:00:00 EDT 2022},
month = {Mon Mar 21 00:00:00 EDT 2022}
}

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