Spatially resolved, substrate-induced rectification in C60 bilayers on copper
Abstract
Here, 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.
- Authors:
-
- Univ. of Central Lancashire, Preston (United Kingdom)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1371915
- Alternate Identifier(s):
- OSTI ID: 1349344
- Grant/Contract Number:
- AC02-06CH11357; FG02-09ER16109
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 146; Journal Issue: 9; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; scanning tunneling spectroscopy; Schottky; density functional theory; fullerene; rectification
Citation Formats
Smerdon, J. A., Darancet, P., and Guest, J. R. Spatially resolved, substrate-induced rectification in C60 bilayers on copper. United States: N. p., 2017.
Web. doi:10.1063/1.4975795.
Smerdon, J. A., Darancet, P., & Guest, J. R. Spatially resolved, substrate-induced rectification in C60 bilayers on copper. United States. https://doi.org/10.1063/1.4975795
Smerdon, J. A., Darancet, P., and Guest, J. R. Wed .
"Spatially resolved, substrate-induced rectification in C60 bilayers on copper". United States. https://doi.org/10.1063/1.4975795. https://www.osti.gov/servlets/purl/1371915.
@article{osti_1371915,
title = {Spatially resolved, substrate-induced rectification in C60 bilayers on copper},
author = {Smerdon, J. A. and Darancet, P. and Guest, J. R.},
abstractNote = {Here, 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.},
doi = {10.1063/1.4975795},
journal = {Journal of Chemical Physics},
number = 9,
volume = 146,
place = {United States},
year = {Wed Feb 22 00:00:00 EST 2017},
month = {Wed Feb 22 00:00:00 EST 2017}
}
Web of Science
Works referenced in this record:
Charge transport and rectification in molecular junctions formed with carbon-based electrodes
journal, July 2014
- Kim, T.; Liu, Z. -F.; Lee, C.
- Proceedings of the National Academy of Sciences, Vol. 111, Issue 30
Modulation of nanocavity plasmonic emission by local molecular states of C_60 on Au(111)
journal, January 2012
- Geng, Feng; Zhang, Yang; Yu, Yunjie
- Optics Express, Vol. 20, Issue 24
Polarizability, Susceptibility, and Dielectric Constant of Nanometer-Scale Molecular Films: A Microscopic View
journal, May 2010
- Natan, Amir; Kuritz, Natalia; Kronik, Leeor
- Advanced Functional Materials, Vol. 20, Issue 13
The SIESTA method for ab initio order- N materials simulation
journal, March 2002
- Soler, José M.; Artacho, Emilio; Gale, Julian D.
- Journal of Physics: Condensed Matter, Vol. 14, Issue 11
Unconventional molecule-resolved current rectification in diamondoid–fullerene hybrids
journal, September 2014
- Randel, Jason C.; Niestemski, Francis C.; Botello-Mendez, Andrés R.
- Nature Communications, Vol. 5, Issue 1
Rectification and stability of a single molecular diode with controlled orientation
journal, October 2009
- Díez-Pérez, Ismael; Hihath, Joshua; Lee, Youngu
- Nature Chemistry, Vol. 1, Issue 8
Single-molecule diodes with high rectification ratios through environmental control
journal, May 2015
- Capozzi, Brian; Xia, Jianlong; Adak, Olgun
- Nature Nanotechnology, Vol. 10, Issue 6
Length-Dependent Thermopower of Highly Conducting Au–C Bonded Single Molecule Junctions
journal, May 2013
- Widawsky, J. R.; Chen, W.; Vázquez, H.
- Nano Letters, Vol. 13, Issue 6
Large Spatially Resolved Rectification in a Donor–Acceptor Molecular Heterojunction
journal, March 2016
- Smerdon, Joseph A.; Giebink, Noel C.; Guisinger, Nathan P.
- Nano Letters, Vol. 16, Issue 4
Tuning Rectification in Single-Molecular Diodes
journal, November 2013
- Batra, Arunabh; Darancet, Pierre; Chen, Qishui
- Nano Letters, Vol. 13, Issue 12
The Importance of Chemical Bonding to the Contact for Tunneling through Alkyl Chains
journal, October 2002
- Selzer, Yoram; Salomon, Adi; Cahen, David
- The Journal of Physical Chemistry B, Vol. 106, Issue 40
Band alignment in molecular devices: Influence of anchoring group and metal work function
journal, June 2008
- Wang, Jian-guo; Prodan, Emil; Car, Roberto
- Physical Review B, Vol. 77, Issue 24
Optimal Electron Doping of a Monolayer on Cu(111) via Interface Reconstruction
journal, January 2010
- Pai, Woei Wu; Jeng, H. T.; Cheng, C. -M.
- Physical Review Letters, Vol. 104, Issue 3
Molecular rectifiers
journal, November 1974
- Aviram, Arieh; Ratner, Mark A.
- Chemical Physics Letters, Vol. 29, Issue 2
A gate-tunable single-molecule diode
journal, January 2016
- Perrin, Mickael L.; Galán, Elena; Eelkema, Rienk
- Nanoscale, Vol. 8, Issue 16
Structural relaxation of adlayers in the presence of adsorbate-induced reconstruction:
journal, March 2004
- Pai, Woei Wu; Hsu, Ching-Ling; Lin, M. C.
- Physical Review B, Vol. 69, Issue 12
Rotation, translation, charge transfer, and electronic structure of on Cu(111) surface
journal, January 2004
- Wang, Lin-Lin; Cheng, Hai-Ping
- Physical Review B, Vol. 69, Issue 4
Observation of quantum interference in molecular charge transport
journal, March 2012
- Guédon, Constant M.; Valkenier, Hennie; Markussen, Troels
- Nature Nanotechnology, Vol. 7, Issue 5
Single Molecule Electronics: Increasing Dynamic Range and Switching Speed Using Cross-Conjugated Species
journal, December 2008
- Andrews, David Q.; Solomon, Gemma C.; Van Duyne, Richard P.
- Journal of the American Chemical Society, Vol. 130, Issue 51
Self-assembled molecular rectifiers
journal, March 1997
- Dhirani, A.; Lin, P. -H.; Guyot-Sionnest, P.
- The Journal of Chemical Physics, Vol. 106, Issue 12
Charge transfer and screening in individual molecules on metal substrates: A scanning tunneling spectroscopy and theoretical study
journal, September 2004
- Lu, Xinghua; Grobis, M.; Khoo, K. H.
- Physical Review B, Vol. 70, Issue 11
Spectroscopy of C 60 single molecules: the role of screening on energy level alignment
journal, April 2008
- Fernández Torrente, Isabel; Franke, Katharina J.; Ignacio Pascual, Jose
- Journal of Physics: Condensed Matter, Vol. 20, Issue 18
Metal-Molecule Contacts and Charge Transport across Monomolecular Layers: Measurement and Theory
journal, August 2002
- Kushmerick, J. G.; Holt, D. B.; Yang, J. C.
- Physical Review Letters, Vol. 89, Issue 8
Theory of Rectification in Tour Wires: The Role of Electrode Coupling
journal, September 2002
- Taylor, Jeremy; Brandbyge, Mads; Stokbro, Kurt
- Physical Review Letters, Vol. 89, Issue 13
Renormalization of Molecular Electronic Levels at Metal-Molecule Interfaces
journal, November 2006
- Neaton, J. B.; Hybertsen, Mark S.; Louie, Steven G.
- Physical Review Letters, Vol. 97, Issue 21
Tuning negative differential resistance in a molecular film
journal, May 2005
- Grobis, M.; Wachowiak, A.; Yamachika, R.
- Applied Physics Letters, Vol. 86, Issue 20
Works referencing / citing this record:
Preface: Special Topic on Frontiers in Molecular Scale Electronics
journal, March 2017
- Evers, Ferdinand; Venkataraman, Latha
- The Journal of Chemical Physics, Vol. 146, Issue 9
Preface: Special Topic on Frontiers in Molecular Scale Electronics
text, January 2017
- Evers, Ferdinand; Venkataraman, Latha
- Universität Regensburg