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Title: Tuning charge and correlation effects for a single molecule on a graphene device

The ability to understand and control the electronic properties of individual molecules in a device environment is crucial for developing future technologies at the nanometre scale and below. Achieving this, however, requires the creation of three-terminal devices that allow single molecules to be both gated and imaged at the atomic scale. We have accomplished this by integrating a graphene field effect transistor with a scanning tunnelling microscope, thus allowing gate-controlled charging and spectroscopic interrogation of individual tetrafluoro-tetracyanoquinodimethane molecules. We observe a non-rigid shift in the molecule’s lowest unoccupied molecular orbital energy (relative to the Dirac point) as a function of gate voltage due to graphene polarization effects. Our results show that electron–electron interactions play an important role in how molecular energy levels align to the graphene Dirac point, and may significantly influence charge transport through individual molecules incorporated in graphene-based nanodevices.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [4] ;  [5] ;  [6] ;  [4] ;  [4] ;  [4] ;  [4] ; ORCiD logo [7] ;  [7] ;  [8] ;  [9] ;  [1] ;  [8]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  2. Univ. of California, Berkeley, CA (United States). Dept. of Physics; National Univ. of Singapore (Singapore). Dept. of Chemistry. Centre for Advanced 2D Materials and Graphene Research
  3. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Imperial College, London (United Kingdom). Dept. of Materials
  4. Univ. of California, Berkeley, CA (United States). Dept. of Physics
  5. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Technical Univ. of Munich, Garching (Germany). Dept. of Physics
  6. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Freie Univ., Berlin (Germany). Dahlem Center for Complex Quantum Systems. Dept. of Physics
  7. National Inst. for Materials Science (NIMS), Tsukuba (Japan)
  8. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Kavli Energy NanoSciences Inst., Berkeley, CA (United States)
  9. National Univ. of Singapore (Singapore). Centre for Advanced 2D Materials and Graphene Research. Dept. of Physics
Publication Date:
Grant/Contract Number:
AC02-05CH11231; DMR-1206512; DRM-1508412; R-144-000-295-281; EP/N005244/1; J3026-N16
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); National Univ. of Singapore (Singapore); National Inst. for Materials Science (NIMS), Tsukuba (Japan); Imperial College, London (United Kingdom)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); Ministry of Education, Culture, Sports, Science and Technology (MEXT) (Japan); Japan Society for the Promotion of Science (JSPS); National Research Foundation (NRF) (Singapore); Engineering and Physical Sciences Research Council (EPSRC); Austrian Science Fund (FWF)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; electronic properties and materials; molecular electronics; surfaces, interfaces and thin films
OSTI Identifier:
1411644

Wickenburg, Sebastian, Lu, Jiong, Lischner, Johannes, Tsai, Hsin-Zon, Omrani, Arash A., Riss, Alexander, Karrasch, Christoph, Bradley, Aaron, Jung, Han Sae, Khajeh, Ramin, Wong, Dillon, Watanabe, Kenji, Taniguchi, Takashi, Zettl, Alex, Neto, A. H. Castro, Louie, Steven G., and Crommie, Michael F.. Tuning charge and correlation effects for a single molecule on a graphene device. United States: N. p., Web. doi:10.1038/ncomms13553.
Wickenburg, Sebastian, Lu, Jiong, Lischner, Johannes, Tsai, Hsin-Zon, Omrani, Arash A., Riss, Alexander, Karrasch, Christoph, Bradley, Aaron, Jung, Han Sae, Khajeh, Ramin, Wong, Dillon, Watanabe, Kenji, Taniguchi, Takashi, Zettl, Alex, Neto, A. H. Castro, Louie, Steven G., & Crommie, Michael F.. Tuning charge and correlation effects for a single molecule on a graphene device. United States. doi:10.1038/ncomms13553.
Wickenburg, Sebastian, Lu, Jiong, Lischner, Johannes, Tsai, Hsin-Zon, Omrani, Arash A., Riss, Alexander, Karrasch, Christoph, Bradley, Aaron, Jung, Han Sae, Khajeh, Ramin, Wong, Dillon, Watanabe, Kenji, Taniguchi, Takashi, Zettl, Alex, Neto, A. H. Castro, Louie, Steven G., and Crommie, Michael F.. 2016. "Tuning charge and correlation effects for a single molecule on a graphene device". United States. doi:10.1038/ncomms13553. https://www.osti.gov/servlets/purl/1411644.
@article{osti_1411644,
title = {Tuning charge and correlation effects for a single molecule on a graphene device},
author = {Wickenburg, Sebastian and Lu, Jiong and Lischner, Johannes and Tsai, Hsin-Zon and Omrani, Arash A. and Riss, Alexander and Karrasch, Christoph and Bradley, Aaron and Jung, Han Sae and Khajeh, Ramin and Wong, Dillon and Watanabe, Kenji and Taniguchi, Takashi and Zettl, Alex and Neto, A. H. Castro and Louie, Steven G. and Crommie, Michael F.},
abstractNote = {The ability to understand and control the electronic properties of individual molecules in a device environment is crucial for developing future technologies at the nanometre scale and below. Achieving this, however, requires the creation of three-terminal devices that allow single molecules to be both gated and imaged at the atomic scale. We have accomplished this by integrating a graphene field effect transistor with a scanning tunnelling microscope, thus allowing gate-controlled charging and spectroscopic interrogation of individual tetrafluoro-tetracyanoquinodimethane molecules. We observe a non-rigid shift in the molecule’s lowest unoccupied molecular orbital energy (relative to the Dirac point) as a function of gate voltage due to graphene polarization effects. Our results show that electron–electron interactions play an important role in how molecular energy levels align to the graphene Dirac point, and may significantly influence charge transport through individual molecules incorporated in graphene-based nanodevices.},
doi = {10.1038/ncomms13553},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {11}
}

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Gate-controlled ionization and screening of cobalt adatoms on a graphene surface
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Large-Area Synthesis of High-Quality and Uniform Graphene Films on Copper Foils
journal, May 2009