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

• Published in: Nature communications Vol. 7; no. 1; p. 13553
• Main Authors: 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.
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 25-11-2016; Nature Publishing Group; Nature Portfolio
• Subjects: 639/766/119/544; 639/766/119/995; 639/766/119/998; Charge transport; electronic properties and materials; Energy; Energy levels; Field effect transistors; Graphene; Humanities and Social Sciences; Interrogation; Laboratories; MATERIALS SCIENCE; Microscopy; molecular electronics; Molecular energy levels; Molecular orbitals; multidisciplinary; Nanotechnology devices; Science; Science (multidisciplinary); Semiconductor devices; Stability; surfaces, interfaces and thin films; Tetracyanoquinodimethane; Transistors
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/ncomms13553

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.
The development of single-molecule electronics calls for precise tuning of the electronic properties of individual molecules that go beyond two-terminal control. Here, Wickenburg
et al
. show gate-tunable switch of charge states of an isolated molecule using a graphene-based field-effect transistor.