Unconventional molecule-resolved current rectification in diamondoid–fullerene hybrids

Jason C. Randel, Francis C. Niestemski, Andrés R. Botello-Mendez, Warren Mar, Georges Ndabashimiye, Sorin Melinte, Jeremy E. P. Dahl, Robert M. K. Carlson, Ekaterina D. Butova, Andrey A. Fokin, Peter R. Schreiner, Jean-Christophe Charlier and Hari C. Manoharan ()
Additional contact information
Jason C. Randel: SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences
Francis C. Niestemski: SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences
Andrés R. Botello-Mendez: Institute of Condensed Matter and Nanosciences, Université catholique de Louvain
Warren Mar: Stanford University
Georges Ndabashimiye: SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences
Sorin Melinte: Institute of Information and Communication Technologies, Electronics and Applied Mathematics, Université catholique de Louvain
Jeremy E. P. Dahl: SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences
Robert M. K. Carlson: SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences
Ekaterina D. Butova: Institute of Organic Chemistry, Justus-Liebig University
Andrey A. Fokin: Institute of Organic Chemistry, Justus-Liebig University
Peter R. Schreiner: Institute of Organic Chemistry, Justus-Liebig University
Jean-Christophe Charlier: Institute of Condensed Matter and Nanosciences, Université catholique de Louvain
Hari C. Manoharan: SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences

Nature Communications, 2014, vol. 5, issue 1, 1-6

Abstract: 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 sp3 (diamondoid) and sp2 (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.

Date: 2014
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DOI: 10.1038/ncomms5877

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