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Nat Commun. 2014 Sep 9;5:4877. doi: 10.1038/ncomms5877.

Unconventional molecule-resolved current rectification in diamondoid-fullerene hybrids.

Author information

1
1] SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences, Menlo Park, California 94025, USA [2] Department of Applied Physics, Stanford University, Stanford, California 94305, USA.
2
1] SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences, Menlo Park, California 94025, USA [2] Department of Physics, Stanford University, Stanford, California 94305, USA.
3
Institute of Condensed Matter and Nanosciences, Université catholique de Louvain, B-1348 Louvain-La-Neuve, Belgium.
4
Department of Electrical Engineering, Stanford University, Stanford, California 94305, USA.
5
Institute of Information and Communication Technologies, Electronics and Applied Mathematics, Université catholique de Louvain, B-1348 Louvain-La-Neuve, Belgium.
6
SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences, Menlo Park, California 94025, USA.
7
Institute of Organic Chemistry, Justus-Liebig University, Heinrich-Buff-Ring 58, 35392 Giessen, Germany.
8
1] Institute of Organic Chemistry, Justus-Liebig University, Heinrich-Buff-Ring 58, 35392 Giessen, Germany [2] Department of Organic Chemistry, Kiev Polytechnic Institute, UA-03056 Kiev, Ukraine.

Abstract

The unimolecular rectifier is a fundamental building block of molecular electronics. Rectification in single molecules can arise from electron transfer between molecular orbitals displaying asymmetric spatial charge distributions, akin to p-n junction diodes in semiconductors. Here we report a novel all-hydrocarbon molecular rectifier consisting of a diamantane-C60 conjugate. By linking both sp(3) (diamondoid) and sp(2) (fullerene) carbon allotropes, this hybrid molecule opposingly pairs negative and positive electron affinities. The single-molecule conductances of self-assembled domains on Au(111), probed by low-temperature scanning tunnelling microscopy and spectroscopy, reveal a large rectifying response of the molecular constructs. This specific electronic behaviour is postulated to originate from the electrostatic repulsion of diamantane-C60 molecules due to positively charged terminal hydrogen atoms on the diamondoid interacting with the top electrode (scanning tip) at various bias voltages. Density functional theory computations scrutinize the electronic and vibrational spectroscopic fingerprints of this unique molecular structure and corroborate the unconventional rectification mechanism.

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