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含3-噻吩基接触基团的有机金属配合物的单分子电导研究

Single-Molecule Conductance Studies of Organometallic Complexes Bearing 3-Thienyl Contacting Groups.

作者信息

Bock Sören, Al-Owaedi Oday A, Eaves Samantha G, Milan David C, Lemmer Mario, Skelton Brian W, Osorio Henrry M, Nichols Richard J, Higgins Simon J, Cea Pilar, Long Nicholas J, Albrecht Tim, Martín Santiago, Lambert Colin J, Low Paul J

机构信息

School of Chemistry and Biochemistry, University of Western Australia, 35 Stirling Highway, Crawley, 6009, WA, Australia.

Department of Physics, Lancaster University, Lancaster, LA1 4YB, UK.

出版信息

Chemistry. 2017 Feb 10;23(9):2133-2143. doi: 10.1002/chem.201604565. Epub 2017 Jan 16.

DOI:10.1002/chem.201604565
PMID:27897344
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC5396322/
Abstract

The compounds and complexes 1,4-C H (C≡C-cyclo-3-C H S) (2), trans-[Pt(C≡C-cyclo-3-C H S) (PEt ) ] (3), trans-[Ru(C≡C-cyclo-3-C H S) (dppe) ] (4; dppe=1,2-bis(diphenylphosphino)ethane) and trans-[Ru(C≡C-cyclo-3-C H S) {P(OEt) } ] (5) featuring the 3-thienyl moiety as a surface contacting group for gold electrodes have been prepared, crystallographically characterised in the case of 3-5 and studied in metal|molecule|metal junctions by using both scanning tunnelling microscope break-junction (STM-BJ) and STM-I(s) methods (measuring the tunnelling current (I) as a function of distance (s)). The compounds exhibit similar conductance profiles, with a low conductance feature being more readily identified by STM-I(s) methods, and a higher feature by the STM-BJ method. The lower conductance feature was further characterised by analysis using an unsupervised, automated multi-parameter vector classification (MPVC) of the conductance traces. The combination of similarly structured HOMOs and non-resonant tunnelling mechanism accounts for the remarkably similar conductance values across the chemically distinct members of the family 2-5.

摘要

已制备出化合物和配合物1,4-C₆H₄(C≡C-cyclo-3-C₄H₃S)₂ (2)、反式-[Pt(C≡C-cyclo-3-C₄H₃S)₂(PEt₃)₂] (3)、反式-[Ru(C≡C-cyclo-3-C₄H₃S)₂(dppe)₂] (4；dppe = 1,2-双(二苯基膦基)乙烷) 和反式-[Ru(C≡C-cyclo-3-C₄H₃S)₂{P(OEt)₃}₂] (5)，它们以3-噻吩基部分作为金电极的表面接触基团，对3-5进行了晶体学表征，并通过扫描隧道显微镜断接结 (STM-BJ) 和STM-I(s) 方法（测量隧穿电流 (I) 作为距离 (s) 的函数）在金属|分子|金属结中进行了研究。这些化合物表现出相似的电导曲线，STM-I(s) 方法更容易识别低电导特征，而STM-BJ方法更容易识别高电导特征。通过使用电导迹线的无监督自动多参数向量分类 (MPVC) 分析进一步表征了较低的电导特征。结构相似的最高占据分子轨道 (HOMO) 和非共振隧穿机制的结合解释了家族2-5中化学性质不同的成员之间电导值的显著相似性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/03b4/5396322/3d501a37c3f2/CHEM-23-2133-g011.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/03b4/5396322/f478f09da73f/CHEM-23-2133-g012.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/03b4/5396322/f439af07b6f7/CHEM-23-2133-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/03b4/5396322/f052adf188c0/CHEM-23-2133-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/03b4/5396322/1072bb6d21bc/CHEM-23-2133-g005.jpg
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