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In situ formation of N-heterocyclic carbene-bound single-molecule junctions
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SYSNO ASEP 0492829 Document Type J - Journal Article R&D Document Type Journal Article Subsidiary J Článek ve WOS Title In situ formation of N-heterocyclic carbene-bound single-molecule junctions Author(s) Doud, E.A. (US)
Inkpen, M.S. (US)
Lovat, G. (US)
Montes Muñoz, Enrique (FZU-D) ORCID
Paley, D.W. (US)
Steigerwald, M.L. (US)
Vázquez, Héctor (FZU-D) ORCID
Venkataraman, L. (US)
Roy, X. (US)Number of authors 9 Source Title Journal of the American Chemical Society. - : American Chemical Society - ISSN 0002-7863
Roč. 140, č. 28 (2018), s. 8944-8949Number of pages 6 s. Language eng - English Country US - United States Keywords self-assembled monolayers ; gold surfaces ; conductance ; chemisorption Subject RIV BM - Solid Matter Physics ; Magnetism OECD category Condensed matter physics (including formerly solid state physics, supercond.) R&D Projects GA15-19672S GA ČR - Czech Science Foundation (CSF) Institutional support FZU-D - RVO:68378271 UT WOS 000439532000045 EID SCOPUS 85050088888 DOI 10.1021/jacs.8b05184 Annotation Self-assembled monolayers (SAMs) formed using N-heterocyclic carbenes (NHCs) have recently emerged as thermally and chemically ultrastable alternatives to those formed from thiols. The rich chemistry and strong sigma-donating ability of NHCs offer unique prospects for applications in nanoelectronics, sensing, and electrochemistry. Although stable in SAMs, free carbenes are notoriously reactive, making their electronic characterization challenging. Here we report the first investigation of electron transport across single NHC-bound molecules using the scanning tunneling microscope-based break junction (STM-BJ) technique. We develop a series of air-stable metal NHC complexes that can be electrochemically reduced in situ to form NHC electrode contacts, enabling reliable single molecule conductance measurements of NHCs under ambient conditions. Using this approach, we show that the conductance of an NHC depends on the identity of the single metal atom to which it is coordinated in the junction. Our observations are supported by density functional theory (DFT) calculations, which also firmly establish the contributions of the NHC linker to the junction transport characteristics. Our work demonstrates a powerful method to probe electron transfer across NHC electrode interfaces, more generally, it opens the door to the exploitation of surface-bound NHCs in constructing novel, functionalized electrodes and/or nanoelectronic devices. Workplace Institute of Physics Contact Kristina Potocká, potocka@fzu.cz, Tel.: 220 318 579 Year of Publishing 2019
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