Influence of the donor unit on the rectification ratio in tunnel junctions based on donor–acceptor SAMs using PTM units as acceptors†,Physical Chemistry Chemical Physics

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Influence of the donor unit on the rectification ratio in tunnel junctions based on donor–acceptor SAMs using PTM units as acceptors†
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2018-09-25 00:00:00 , DOI: 10.1039/c8cp05488f
Manuel Souto _{1,

2,

3,

4} , Valentin Díez-Cabanes _{5,

6,

7,

8} , Li Yuan _{9,

10,

11,

12} , Adriana R. Kyvik _{1,

2,

3,

4} , Imma Ratera _{1,

2,

3,

4} , Christian A. Nijhuis _{9,

10,

11,

12,

13} , Jerome Cornil _{5,

6,

7,

8} , Jaume Veciana _{1,

2,

3,

4}

Affiliation

Dyads formed by an electron donor unit (D) covalently linked to an electron acceptor (A) by an organic bridge are promising materials as molecular rectifiers. Very recently, we have reported the charge transport measurements across self-assembled monolayers (SAMs) of two D–A systems consisting of the ferrocene (Fc) electron-donor linked to a polychlorotriphenylmethane (PTM) electron-acceptor in its non-radical (SAM 1) and radical (SAM 2) forms. Interestingly, we observed that the non-radical SAM 1 showed rectification behavior of 2 orders of magnitude higher than its radical analogue dyad 2. In order to study the influence of the donor unit on the transport properties, we report herein the synthesis and characterization of two new D–A SAMs in which the electron-donor Fc unit is replaced by a tetrathiafulvalene (TTF) moiety linked to the PTM unit in its non-radical (SAM 3) and radical (SAM 4) forms. The observed decrease in the rectification ratio and increased current density for TTF-PTM based SAMs 3 and 4 in comparison to Fc-PTM based SAMs 1 and 2 are explained, supported by theoretical calculations, by significant changes in the electronic and supramolecular structures.

中文翻译：

基于PTM单元作为受体的施主-受主SAM，施主单元对隧道结整流比的影响†

由通过有机桥与电子受体（A）共价连接的电子供体单元（D）形成的二元化合物是有前途的作为分子整流器的材料。最近，我们已经报道了两个D–A系统自组装单层（SAM）上的电荷传输测量，该系统由二茂铁（Fc）电子给体与非氯原子上的聚氯三苯甲烷（PTM）电子受体连接而成。 SAM 1）和自由基（SAM 2）的形式。有趣的是，我们观察到非自由基SAM 1的整流行为比其自由基类似物dyad 2高2个数量级。。为了研究供体单元对传输性质的影响，我们在此报告了两种新的D–A SAM的合成和表征，其中电子供体Fc单元被连接至PTM的四硫富瓦烯（TTF）部分取代非自由基（SAM 3）和自由基（SAM 4）形式的单元。与基于Fc-PTM的SAMs 1和2相比，基于TTF-PTM的SAMs 3和4观察到的整流比的降低和电流密度的增加得到了理论计算的支持，其中电子和超分子结构发生了显着变化。

更新日期：2018-09-25

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