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Title: Emergence of Interfacial Polarons from Electron–Phonon Coupling in Graphene/h-BN van der Waals Heterostructures

Abstract

van der Waals heterostructures, vertical stacks of layered materials, offer new opportunities for novel quantum phenomena which are absent in their constituent components. Here we report the emergence of polaron quasiparticles at the interface of graphene/hexagonal boron nitride (h-BN) heterostructures. Using nanospot angle-resolved photoemission spectroscopy, we observe zone-corner replicas of h-BN valence band maxima, with energy spacing coincident with the highest phonon energy of the heterostructure, an indication of Fröhlich polaron formation due to forward-scattering electron–phonon coupling. Parabolic fitting of the h-BN bands yields an effective mass enhancement of ~2.3, suggesting an intermediate coupling strength. Our theoretical simulations based on Migdal–Eliashberg theory corroborate the experimental results, allowing the extraction of microscopic physical parameters. Moreover, renormalization of graphene π-band is observed due to the hybridization with the h-BN band. Our work generalizes the polaron study from transition metal oxides to van der Waals heterostructures with higher material flexibility, highlighting interlayer coupling as an extra degree of freedom to explore emergent phenomena.

Authors:
ORCiD logo [1];  [1];  [2];  [3];  [4];  [2];  [2];  [5];  [6];  [2];  [1]
+ Show Author Affiliations
  1. Synchrotron SOLEIL and Univ. Paris-Saclay, Gif sur Yvette Cedex (France)
  2. Chinese Academy of Sciences (CAS), Beijing (China)
  3. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Univ. of Bath, Bath (United Kingdom)
  5. Chinese Academy of Sciences (CAS), Beijing (China); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1461624
Alternate Identifier(s):
OSTI ID: 1484748
Grant/Contract Number:  
2013CB934500; AC02-76SF00515; 61325021; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 2; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; electronic structure; electron−phonon coupling; Migdal-Eliashberg theory; NanoARPES; polaron; van der Waals heterostructure

Citation Formats

Chen, Chaoyu, Avila, Jose, Wang, Shuopei, Wang, Yao, Mucha-Kruczy?ski, Marcin, Shen, Cheng, Yang, Rong, Nosarzewski, Benjamin, Devereaux, Thomas P., Zhang, Guangyu, and Asensio, Maria Carmen. Emergence of Interfacial Polarons from Electron–Phonon Coupling in Graphene/h-BN van der Waals Heterostructures. United States: N. p., 2018. Web. doi:10.1021/acs.nanolett.7b04604.
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Chen, Chaoyu, Avila, Jose, Wang, Shuopei, Wang, Yao, Mucha-Kruczy?ski, Marcin, Shen, Cheng, Yang, Rong, Nosarzewski, Benjamin, Devereaux, Thomas P., Zhang, Guangyu, & Asensio, Maria Carmen. Emergence of Interfacial Polarons from Electron–Phonon Coupling in Graphene/h-BN van der Waals Heterostructures. United States. https://doi.org/10.1021/acs.nanolett.7b04604
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Chen, Chaoyu, Avila, Jose, Wang, Shuopei, Wang, Yao, Mucha-Kruczy?ski, Marcin, Shen, Cheng, Yang, Rong, Nosarzewski, Benjamin, Devereaux, Thomas P., Zhang, Guangyu, and Asensio, Maria Carmen. Fri . "Emergence of Interfacial Polarons from Electron–Phonon Coupling in Graphene/h-BN van der Waals Heterostructures". United States. https://doi.org/10.1021/acs.nanolett.7b04604. https://www.osti.gov/servlets/purl/1461624.
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@article{osti_1461624,
title = {Emergence of Interfacial Polarons from Electron–Phonon Coupling in Graphene/h-BN van der Waals Heterostructures},
author = {Chen, Chaoyu and Avila, Jose and Wang, Shuopei and Wang, Yao and Mucha-Kruczy?ski, Marcin and Shen, Cheng and Yang, Rong and Nosarzewski, Benjamin and Devereaux, Thomas P. and Zhang, Guangyu and Asensio, Maria Carmen},
abstractNote = {van der Waals heterostructures, vertical stacks of layered materials, offer new opportunities for novel quantum phenomena which are absent in their constituent components. Here we report the emergence of polaron quasiparticles at the interface of graphene/hexagonal boron nitride (h-BN) heterostructures. Using nanospot angle-resolved photoemission spectroscopy, we observe zone-corner replicas of h-BN valence band maxima, with energy spacing coincident with the highest phonon energy of the heterostructure, an indication of Fröhlich polaron formation due to forward-scattering electron–phonon coupling. Parabolic fitting of the h-BN bands yields an effective mass enhancement of ~2.3, suggesting an intermediate coupling strength. Our theoretical simulations based on Migdal–Eliashberg theory corroborate the experimental results, allowing the extraction of microscopic physical parameters. Moreover, renormalization of graphene π-band is observed due to the hybridization with the h-BN band. Our work generalizes the polaron study from transition metal oxides to van der Waals heterostructures with higher material flexibility, highlighting interlayer coupling as an extra degree of freedom to explore emergent phenomena.},
doi = {10.1021/acs.nanolett.7b04604},
journal = {Nano Letters},
number = 2,
volume = 18,
place = {United States},
year = {Fri Jan 05 00:00:00 EST 2018},
month = {Fri Jan 05 00:00:00 EST 2018}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acs.nanolett.7b04604
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Cited by: 44 works
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Figures / Tables:

FIG. 1 FIG. 1: General experimental geometry and sample characterisation a, Schematic focus mechanism of NanoARPES. b, Schematic of G/h-BN lattice structure. c, Overall photoemission core level spectrum taken with bean energy 350 eV and beam spot larger than 50 µm. The inset shows the detailed NanoARPES spectrum close to Fermi levelmore » taken with beam energy 100 eV. d, NanoARPES image shows the distribution of photoemission intensity integrated from the energy-angle window (dashed box) shown in c. e, Optical image of the measured sample. The heterostructure is grounded by Au contact. Pristine h-BN border is highlighted by dashed white lines, in panels d and e .« less
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    Works referencing / citing this record:

    Electron-polaron—electron-polaron bound states in mass-gap graphene-like planar quantum electrodynamics: s-wave bipolarons
    journal, October 2018

    Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields
    journal, September 2019

    Intervalley polaron in atomically thin transition metal dichalcogenides
    journal, July 2019

    Nanospot angle-resolved photoemission study of Bernal-stacked bilayer graphene on hexagonal boron nitride: Band structure and local variation of lattice alignment
    journal, April 2019

    • Joucken, Frédéric; Quezada-López, Eberth A.; Avila, Jose
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    Large local lattice expansion in graphene adlayers grown on copper
    journal, April 2018

    Ab initio theory of polarons: Formalism and applications
    journal, June 2019

    Ab initio theory of polarons: formalism and applications
    text, January 2019

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