Transport through Redox-Active Ru-Terpyridine Complexes Integrated in Single Nanoparticle Devices
Transport through Redox-Active Ru-Terpyridine Complexes Integrated in Single Nanoparticle Devices
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DOI：
10.1021/acs.jpcc.9b11716
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发表时间：
2020-02-27
影响因子：
3.7
通讯作者：
Karthaeuser, Silvia
中科院分区：
文献类型：
--
作者：
Mennicken, Max;Peter, Sophia K.;Karthaeuser, Silvia
过渡金属配合物由于其高导电性和涉及金属到配体电荷转移的固有开关能力而成为电功能分子。在这里，提出了一种方法，以可靠地接触几个单一的氧化还原活性钌三联吡啶复合物在CMOS兼容的纳米器件，并保持其电功能。使用来自14 nm金纳米颗粒（AuNP）和双-{4 '44-（巯基苯基）-2，2'：6 '，2“-三联吡啶]}-钌（II）络合物的杂化材料，实现了包括30（2）nm（2）的纳米电极的器件尺寸。此外，这种方法有机会进一步缩小规模。Ru络合物AuNP器件在两个很好分离的电导范围内显示出对称和不对称的电流-电压曲线，具有滞后特性。通过基于单沟道Landauer模型的理论近似，深入分析了双势垒隧道结中的电荷输运，揭示了其对分子/金属接触的敏感性。结果表明，通过HOMO的隧穿输运是主要的输运机制，而退相干跳跃输运在一定程度上是次要的。
Transition metal complexes are electrofunctional molecules due to their high conductivity and their intrinsic switching ability involving a metal-to-ligand charge transfer. Here, a method is presented to contact reliably a few to single redox-active Ru-terpyridine complexes in a CMOS compatible nanodevice and preserve their electrical functionality. Using hybrid materials from 14 nm gold nanoparticles (AuNP) and bis-{4'44-(mercaptopheny1)-2,2':6',2 ''-terpyridine]}-ruthenium(II) complexes a device size of 30(2) nm(2) inclusive nanoelectrodes is achieved. Moreover, this method bears the opportunity for further downscaling. The Ru-complex AuNP devices show symmetric and asymmetric current versus voltage curves with a hysteretic characteristic in two well separated conductance ranges. By theoretical approximations based on the single-channel Landauer model, the charge transport through the formed double-barrier tunnel junction is thoroughly analyzed and its sensibility to the molecule/metal contact is revealed. It can be verified that tunneling transport through the HOMO is the main transport mechanism while decoherent hopping transport is present to a minor extent.