High Molecular Conductance and Inverted Conductance Decay over 3 nm in Aminium-Terminated Carbon-Bridged Oligophenylene-Vinylenes

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2024-12-20 DOI:10.1021/jacs.4c13901
Luisa K. I. Rieger, Susanne Leitherer, William Bro-Jo̷rgensen, Gemma C. Solomon, Rainer F. Winter
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Abstract

With the progressing miniaturization of electronic device components to improve circuit density while retaining or even reducing spatial requirements, single molecules employed as electric components define the lower limit of accessible structural width. To circumvent the typical exponential conductance decay for increasing length in molecule-based wires, topological states, which describe the occurrence of discontinuities of a bulk material’s electronic structure confined to its surface, can be realized for molecules by the introduction of unpaired spins at the molecular termini. The resulting high conductance and reversed conductance decay are typically only observed for shorter molecules, as the terminal spins must be within the electronic coupling range to produce the desired effects. We expand the realm of long and exceptionally conductive molecular wires by employing highly conjugated, planarized carbon-bridged oligo(phenylene-vinylene)s as conduits between readily oxidizable diarylamine termini. This yields molecular wires of already decent conductance values and small conductance decay in the neutral state. Upon the introduction of topological states, the conductance can be increased by a factor of up to 1800 for a 3 nm long molecule, and the conductance decay becomes inverted, together with an excellent signal intensity at concentrations as low as 0.01 mM.

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氨基端碳桥接的聚苯乙烯-乙烯基聚合物在3nm范围内的高分子电导和反向电导衰减
随着电子器件元件的不断小型化,在保持甚至减少空间要求的同时提高电路密度,作为电子元件的单分子定义了可访问结构宽度的下限。为了避免典型的指数电导衰减在分子基导线中增加长度,拓扑状态,描述限制在其表面的大块材料的电子结构的不连续的发生,可以通过在分子末端引入不成对的自旋来实现分子。所产生的高电导和反向电导衰减通常只在较短的分子中观察到,因为终端自旋必须在电子耦合范围内才能产生所需的效果。我们通过采用高度共轭、平面化的碳桥接低聚物(苯乙烯-乙烯)作为易氧化二芳胺末端之间的导管,扩展了长而导电异常的分子线领域。这就产生了在中性状态下具有良好电导值和小电导衰减的分子线。在引入拓扑状态后,对于3nm长的分子,电导可以增加到1800倍,并且电导衰减变为反转,同时在低至0.01 mM的浓度下具有优异的信号强度。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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