Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 42, Pages 14845-14848Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b08370
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Funding
- National Science Foundation [DMR-1507440]
- Center for Precision Assembly of Superstratic and Superatomic Solids at Columbia University
- NSF MRSEC [DMR-1420634]
- NSF [DGE 16-44869]
- Molecular Foundry
- Materials Sciences and Engineering Division (Theory FWP), U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-05CH11231]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1507440] Funding Source: National Science Foundation
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We report a series of single-molecule transport measurements carried out in an ionic environment with oligophenylenediamine wires. These molecules exhibit three discrete conducting states accessed by electrochemically modifying the contacts. Transport in these junctions is defined by the oligophenylene backbone, but the conductance is increased by factors of similar to 20 and when compared to traditional dative junctions. We propose that the higher-conducting states arise from in situ electrochemical conversion of the dative Au <- N bond into a new type of Au-N contact. Density functional theory based transport calculations establish that the new contacts dramatically increase the electronic coupling of the oligophenylene backbone to the Au electrodes, consistent with experimental transport data. The resulting contact resistance is the lowest reported to date; more generally, our work demonstrates a facile method for creating electronically transparent metal-organic interfaces.
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