Spatially resolved, substrate-induced rectification in C60 bilayers on copper

J. A. Smerdon; P. Darancet; J. R. Guest

doi:10.1063/1.4975795

Spatially resolved, substrate-induced rectification in C₆₀ bilayers on copper

J. A. Smerdon, P. Darancet, J. R. Guest

MRC - Materials Research Center

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

We demonstrate rectification ratios (RR) of ≳1000 at biases of 1.3 V in bilayers of C₆₀ deposited on copper. Using scanning tunneling spectroscopy and first-principles calculations, we show that the strong coupling between C₆₀ and the Cu(111) surface leads to the metallization of the bottom C₆₀ layer, while the molecular orbitals of the top C₆₀ are essentially unaffected. Due to this substrate-induced symmetry breaking and to a tunneling transport mechanism, the system behaves as a hole-blocking layer, with a spatial dependence of the onset voltage on intra-layer coordination. Together with previous observations of strong electron-blocking character of pentacene/C₆₀ bilayers on Cu(111), this work further demonstrates the potential of strongly hybridized, C₆₀-coated electrodes to harness the electrical functionality of molecular components.

Original language	English (US)
Article number	092328
Journal	Journal of Chemical Physics
Volume	146
Issue number	9
DOIs	https://doi.org/10.1063/1.4975795
State	Published - Mar 7 2017

Funding

Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Primary support for this work was provided by the Department of Energy Office of Basic Energy Sciences (SISGR Grant No. DE-FG02-09ER16109). We thank our anonymous referees for bringing some references to our attention, and for suggesting that static non-local correlations may explain the coordination-dependent turn-on voltage.26

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

Access to Document

10.1063/1.4975795

Cite this

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title = "Spatially resolved, substrate-induced rectification in C60 bilayers on copper",

abstract = "We demonstrate rectification ratios (RR) of ≳1000 at biases of 1.3 V in bilayers of C60 deposited on copper. Using scanning tunneling spectroscopy and first-principles calculations, we show that the strong coupling between C60 and the Cu(111) surface leads to the metallization of the bottom C60 layer, while the molecular orbitals of the top C60 are essentially unaffected. Due to this substrate-induced symmetry breaking and to a tunneling transport mechanism, the system behaves as a hole-blocking layer, with a spatial dependence of the onset voltage on intra-layer coordination. Together with previous observations of strong electron-blocking character of pentacene/C60 bilayers on Cu(111), this work further demonstrates the potential of strongly hybridized, C60-coated electrodes to harness the electrical functionality of molecular components.",

author = "Smerdon, {J. A.} and P. Darancet and Guest, {J. R.}",

note = "Funding Information: Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Primary support for this work was provided by the Department of Energy Office of Basic Energy Sciences (SISGR Grant No. DE-FG02-09ER16109). We thank our anonymous referees for bringing some references to our attention, and for suggesting that static non-local correlations may explain the coordination-dependent turn-on voltage.26 Publisher Copyright: {\textcopyright} 2017 Author(s).",

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AU - Darancet, P.

AU - Guest, J. R.

N1 - Funding Information: Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Primary support for this work was provided by the Department of Energy Office of Basic Energy Sciences (SISGR Grant No. DE-FG02-09ER16109). We thank our anonymous referees for bringing some references to our attention, and for suggesting that static non-local correlations may explain the coordination-dependent turn-on voltage.26 Publisher Copyright: © 2017 Author(s).

PY - 2017/3/7

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N2 - We demonstrate rectification ratios (RR) of ≳1000 at biases of 1.3 V in bilayers of C60 deposited on copper. Using scanning tunneling spectroscopy and first-principles calculations, we show that the strong coupling between C60 and the Cu(111) surface leads to the metallization of the bottom C60 layer, while the molecular orbitals of the top C60 are essentially unaffected. Due to this substrate-induced symmetry breaking and to a tunneling transport mechanism, the system behaves as a hole-blocking layer, with a spatial dependence of the onset voltage on intra-layer coordination. Together with previous observations of strong electron-blocking character of pentacene/C60 bilayers on Cu(111), this work further demonstrates the potential of strongly hybridized, C60-coated electrodes to harness the electrical functionality of molecular components.

AB - We demonstrate rectification ratios (RR) of ≳1000 at biases of 1.3 V in bilayers of C60 deposited on copper. Using scanning tunneling spectroscopy and first-principles calculations, we show that the strong coupling between C60 and the Cu(111) surface leads to the metallization of the bottom C60 layer, while the molecular orbitals of the top C60 are essentially unaffected. Due to this substrate-induced symmetry breaking and to a tunneling transport mechanism, the system behaves as a hole-blocking layer, with a spatial dependence of the onset voltage on intra-layer coordination. Together with previous observations of strong electron-blocking character of pentacene/C60 bilayers on Cu(111), this work further demonstrates the potential of strongly hybridized, C60-coated electrodes to harness the electrical functionality of molecular components.

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