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In situ formation of N-heterocyclic carbene-bound single-molecule junctions

Identifikátory výsledku

  • Kód výsledku v IS VaVaI

    <a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F68378271%3A_____%2F18%3A00492829" target="_blank" >RIV/68378271:_____/18:00492829 - isvavai.cz</a>

  • Výsledek na webu

    <a href="http://dx.doi.org/10.1021/jacs.8b05184" target="_blank" >http://dx.doi.org/10.1021/jacs.8b05184</a>

  • DOI - Digital Object Identifier

    <a href="http://dx.doi.org/10.1021/jacs.8b05184" target="_blank" >10.1021/jacs.8b05184</a>

Alternativní jazyky

  • Jazyk výsledku

    angličtina

  • Název v původním jazyce

    In situ formation of N-heterocyclic carbene-bound single-molecule junctions

  • Popis výsledku v původním jazyce

    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.

  • Název v anglickém jazyce

    In situ formation of N-heterocyclic carbene-bound single-molecule junctions

  • Popis výsledku anglicky

    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.

Klasifikace

  • Druh

    J<sub>imp</sub> - Článek v periodiku v databázi Web of Science

  • CEP obor

  • OECD FORD obor

    10302 - Condensed matter physics (including formerly solid state physics, supercond.)

Návaznosti výsledku

  • Projekt

    <a href="/cs/project/GA15-19672S" target="_blank" >GA15-19672S: Síly a vodivost v molekulárních kontaktech</a><br>

  • Návaznosti

    P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Ostatní

  • Rok uplatnění

    2018

  • Kód důvěrnosti údajů

    S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Údaje specifické pro druh výsledku

  • Název periodika

    Journal of the American Chemical Society

  • ISSN

    0002-7863

  • e-ISSN

  • Svazek periodika

    140

  • Číslo periodika v rámci svazku

    28

  • Stát vydavatele periodika

    US - Spojené státy americké

  • Počet stran výsledku

    6

  • Strana od-do

    8944-8949

  • Kód UT WoS článku

    000439532000045

  • EID výsledku v databázi Scopus

    2-s2.0-85050088888