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Title: Microscopy of hydrogen and hydrogen-vacancy defect structures on graphene devices

Abstract

Here, we have used scanning tunneling microscopy (STM) to investigate two types of hydrogen defect structures on monolayer graphene supported by hexagonal boron nitride (h-BN) in a gated field-effect transistor configuration. The first H-defect type is created by bombarding graphene with 1-keV ionized hydrogen and is identified as two hydrogen atoms bonded to a graphene vacancy via comparison of experimental data to first-principles calculations. The second type of H defect is identified as dimerized hydrogen and is created by depositing atomic hydrogen having only thermal energy onto a graphene surface. Scanning tunneling spectroscopy (STS) measurements reveal that hydrogen dimers formed in this way open a new elastic channel in the tunneling conductance between an STM tip and graphene.

Authors:
 [1];  [1];  [2];  [1];  [3];  [3];  [4];  [1];  [2];  [2];  [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Imperial College London, London (United Kingdom)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Univ. of California, Riverside, CA (United States); The Ohio State Univ., Columbus, OH (United States)
Publication Date:
Research Org.:
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1478653
Alternate Identifier(s):
OSTI ID: 1478693; OSTI ID: 1581315
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 98; Journal Issue: 15; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Graphene; Hydrogen; STM

Citation Formats

Wong, Dillon, Wang, Yang, Jin, Wuwei, Tsai, Hsin -Zon, Bostwick, Aaron, Rotenberg, Eli, Kawakami, Roland K., Zettl, Alex, Mostofi, Arash A., Lischner, Johannes, and Crommie, Michael F. Microscopy of hydrogen and hydrogen-vacancy defect structures on graphene devices. United States: N. p., 2018. Web. doi:10.1103/PhysRevB.98.155436.
Wong, Dillon, Wang, Yang, Jin, Wuwei, Tsai, Hsin -Zon, Bostwick, Aaron, Rotenberg, Eli, Kawakami, Roland K., Zettl, Alex, Mostofi, Arash A., Lischner, Johannes, & Crommie, Michael F. Microscopy of hydrogen and hydrogen-vacancy defect structures on graphene devices. United States. doi:10.1103/PhysRevB.98.155436.
Wong, Dillon, Wang, Yang, Jin, Wuwei, Tsai, Hsin -Zon, Bostwick, Aaron, Rotenberg, Eli, Kawakami, Roland K., Zettl, Alex, Mostofi, Arash A., Lischner, Johannes, and Crommie, Michael F. Mon . "Microscopy of hydrogen and hydrogen-vacancy defect structures on graphene devices". United States. doi:10.1103/PhysRevB.98.155436. https://www.osti.gov/servlets/purl/1478653.
@article{osti_1478653,
title = {Microscopy of hydrogen and hydrogen-vacancy defect structures on graphene devices},
author = {Wong, Dillon and Wang, Yang and Jin, Wuwei and Tsai, Hsin -Zon and Bostwick, Aaron and Rotenberg, Eli and Kawakami, Roland K. and Zettl, Alex and Mostofi, Arash A. and Lischner, Johannes and Crommie, Michael F.},
abstractNote = {Here, we have used scanning tunneling microscopy (STM) to investigate two types of hydrogen defect structures on monolayer graphene supported by hexagonal boron nitride (h-BN) in a gated field-effect transistor configuration. The first H-defect type is created by bombarding graphene with 1-keV ionized hydrogen and is identified as two hydrogen atoms bonded to a graphene vacancy via comparison of experimental data to first-principles calculations. The second type of H defect is identified as dimerized hydrogen and is created by depositing atomic hydrogen having only thermal energy onto a graphene surface. Scanning tunneling spectroscopy (STS) measurements reveal that hydrogen dimers formed in this way open a new elastic channel in the tunneling conductance between an STM tip and graphene.},
doi = {10.1103/PhysRevB.98.155436},
journal = {Physical Review B},
issn = {2469-9950},
number = 15,
volume = 98,
place = {United States},
year = {2018},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

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Cited by: 3 works
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Figures / Tables:

Fig. 1 Fig. 1: (a) STM topographic image of graphene/h-BN after bombarding the surface with 1 keV hydrogen ions (hydrogen dose procedure #1). Triangular defects with lima-bean-shaped (LB) centers are seen. (b) Zoomed-in topographic image of one triangular defect. (c) STM topographic image of a triangular defect before rotation of the LBmore » center. (d) Same triangular defect as in (c) after rotating the LB center by 120° due to STM tip raster scan. Tunneling parameters: (a) $V$s = 500 mV, $I$ = 2 pA; (b) $V$s = 200 mV, $I$ = 500 pA; (c,d) $V$s = 250 mV, $I$ = 50 pA.« less

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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Giant tunnel-electron injection in nitrogen-doped graphene
journal, March 2015


Electronic structure of N-doped graphene with native point defects
journal, April 2013


Tomography of a Probe Potential Using Atomic Sensors on Graphene
journal, November 2016


Atomic Hydrogen Adsorbate Structures on Graphene
journal, July 2009

  • Balog, Richard; Jørgensen, Bjarke; Wells, Justin
  • Journal of the American Chemical Society, Vol. 131, Issue 25
  • DOI: 10.1021/ja902714h

Imaging resonant dissipation from individual atomic defects in graphene
journal, December 2017


Scanning tunnelling microscopy and spectroscopy of ultra-flat graphene on hexagonal boron nitride
journal, February 2011

  • Xue, Jiamin; Sanchez-Yamagishi, Javier; Bulmash, Danny
  • Nature Materials, Vol. 10, Issue 4
  • DOI: 10.1038/nmat2968

Fabrication of Gate-tunable Graphene Devices for Scanning Tunneling Microscopy Studies with Coulomb Impurities
journal, January 2015

  • Jung, Han Sae; Tsai, Hsin-Zon; Wong, Dillon
  • Journal of Visualized Experiments, Issue 101
  • DOI: 10.3791/52711

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

  • Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
  • Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
  • DOI: 10.1088/0953-8984/21/39/395502

Unravelling the role of inelastic tunneling into pristine and defected graphene
journal, March 2015

  • Palsgaard, Mattias L. N.; Andersen, Nick P.; Brandbyge, Mads
  • Physical Review B, Vol. 91, Issue 12
  • DOI: 10.1103/PhysRevB.91.121403

Magnetic Moment Formation in Graphene Detected by Scattering of Pure Spin Currents
journal, November 2012


Prospects for hydrogen storage in graphene
journal, January 2013

  • Tozzini, Valentina; Pellegrini, Vittorio
  • Phys. Chem. Chem. Phys., Vol. 15, Issue 1
  • DOI: 10.1039/C2CP42538F

Mechanism of high-resolution STM/AFM imaging with functionalized tips
journal, August 2014


Bandgap opening in graphene induced by patterned hydrogen adsorption
journal, March 2010

  • Balog, Richard; Jørgensen, Bjarke; Nilsson, Louis
  • Nature Materials, Vol. 9, Issue 4
  • DOI: 10.1038/nmat2710

Graphane: A two-dimensional hydrocarbon
journal, April 2007


Theory of the scanning tunneling microscope
journal, January 1985


Stability and magnetism of hydrogen dimers on graphene
journal, August 2008


Real-space imaging of molecular structure and chemical bonding by single-molecule inelastic tunneling probe
journal, May 2014


Tuning charge and correlation effects for a single molecule on a graphene device
journal, November 2016

  • Wickenburg, Sebastian; Lu, Jiong; Lischner, Johannes
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13553

Characterization and manipulation of individual defects in insulating hexagonal boron nitride using scanning tunnelling microscopy
journal, August 2015


Probing Local Hydrogen Impurities in Quasi-Free-Standing Graphene
journal, November 2012

  • Scheffler, Martha; Haberer, Danny; Petaccia, Luca
  • ACS Nano, Vol. 6, Issue 12
  • DOI: 10.1021/nn303485c

Boron nitride substrates for high-quality graphene electronics
journal, August 2010

  • Dean, C. R.; Young, A. F.; Meric, I.
  • Nature Nanotechnology, Vol. 5, Issue 10, p. 722-726
  • DOI: 10.1038/nnano.2010.172

Observation of Carrier-Density-Dependent Many-Body Effects in Graphene via Tunneling Spectroscopy
journal, January 2010


Large-Area Synthesis of High-Quality and Uniform Graphene Films on Copper Foils
journal, May 2009


Structure and stability of hydrogenated carbon atom vacancies in graphene
journal, October 2014


Colossal enhancement of spin–orbit coupling in weakly hydrogenated graphene
journal, March 2013

  • Balakrishnan, Jayakumar; Kok Wai Koon, Gavin; Jaiswal, Manu
  • Nature Physics, Vol. 9, Issue 5
  • DOI: 10.1038/nphys2576

Realization of a tunable artificial atom at a supercritically charged vacancy in graphene
journal, February 2016

  • Mao, Jinhai; Jiang, Yuhang; Moldovan, Dean
  • Nature Physics, Vol. 12, Issue 6
  • DOI: 10.1038/nphys3665

Hydrogen on graphene: Electronic structure, total energy, structural distortions and magnetism from first-principles calculations
journal, January 2008


Sticking of atomic hydrogen on graphene
journal, June 2018

  • Bonfanti, Matteo; Achilli, Simona; Martinazzo, Rocco
  • Journal of Physics: Condensed Matter, Vol. 30, Issue 28
  • DOI: 10.1088/1361-648X/aac89f

Direct imaging of monovacancy-hydrogen complexes in a single graphitic layer
journal, April 2014


Molecular Self-Assembly in a Poorly Screened Environment: F 4 TCNQ on Graphene/BN
journal, October 2015


Pseudopotentials for high-throughput DFT calculations
journal, January 2014


Direct Imaging of Covalent Bond Structure in Single-Molecule Chemical Reactions
journal, May 2013


Ortho and Para Hydrogen Dimers on G/SiC(0001): Combined STM and DFT Study
journal, December 2014

  • Merino, P.; Švec, M.; Martínez, J. I.
  • Langmuir, Vol. 31, Issue 1
  • DOI: 10.1021/la504021x

Clustering of Chemisorbed H(D) Atoms on the Graphite (0001) Surface due to Preferential Sticking
journal, October 2006


Quasiparticle Transformation during a Metal-Insulator Transition in Graphene
journal, July 2009


Local Electronic Properties of Graphene on a BN Substrate via Scanning Tunneling Microscopy
journal, June 2011

  • Decker, Régis; Wang, Yang; Brar, Victor W.
  • Nano Letters, Vol. 11, Issue 6
  • DOI: 10.1021/nl2005115

Effect of hydrogen dimers on the electronic structure of graphene
journal, January 2014


Phonon-Mediated Tunneling into Graphene
journal, November 2008


Cluster expansion method for adsorption: Application to hydrogen chemisorption on graphene
journal, August 2003


Missing Atom as a Source of Carbon Magnetism
journal, March 2010


Atomically precise graphene nanoribbon heterojunctions from a single molecular precursor
journal, September 2017

  • Nguyen, Giang D.; Tsai, Hsin-Zon; Omrani, Arash A.
  • Nature Nanotechnology, Vol. 12, Issue 11
  • DOI: 10.1038/nnano.2017.155

Patterning Graphene at the Nanometer Scale via Hydrogen Desorption
journal, December 2009

  • Sessi, Paolo; Guest, Jeffrey R.; Bode, Matthias
  • Nano Letters, Vol. 9, Issue 12
  • DOI: 10.1021/nl902605t

Atomic-scale control of graphene magnetism by using hydrogen atoms
journal, April 2016

  • Gonzalez-Herrero, H.; Gomez-Rodriguez, J. M.; Mallet, P.
  • Science, Vol. 352, Issue 6284
  • DOI: 10.1126/science.aad8038

Scattering and Interference in Epitaxial Graphene
journal, July 2007

  • Rutter, G. M.; Crain, J. N.; Guisinger, N. P.
  • Science, Vol. 317, Issue 5835, p. 219-222
  • DOI: 10.1126/science.1142882

Metastable Structures and Recombination Pathways for Atomic Hydrogen on the Graphite (0001) Surface
journal, April 2006


Control of Graphene's Properties by Reversible Hydrogenation: Evidence for Graphane
journal, January 2009


First-principles study of structural stability, magnetism, and hyperfine coupling in hydrogen clusters adsorbed on graphene
journal, October 2010


Uncovering the dominant scatterer in graphene sheets on SiO 2
journal, August 2010


Giant phonon-induced conductance in scanning tunnelling spectroscopy of gate-tunable graphene
journal, July 2008

  • Zhang, Yuanbo; Brar, Victor W.; Wang, Feng
  • Nature Physics, Vol. 4, Issue 8
  • DOI: 10.1038/nphys1022

Bond-Order Discrimination by Atomic Force Microscopy
journal, September 2012


Crystalline hydrogenation of graphene by scanning tunneling microscope tip-induced field dissociation of H2
journal, November 2017


Graphene etching on SiC grains as a path to interstellar polycyclic aromatic hydrocarbons formation
journal, January 2014

  • Merino, P.; Švec, M.; Martinez, J. I.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4054

Exposure of Epitaxial Graphene on SiC(0001) to Atomic Hydrogen
journal, April 2009

  • Guisinger, Nathan P.; Rutter, Gregory M.; Crain, Jason N.
  • Nano Letters, Vol. 9, Issue 4
  • DOI: 10.1021/nl803331q

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.