Carlotti Marco, Soni Saurabh, Kumar Sumit, Ai Yong, Sauter Eric, Zharnikov Michael, Chiechi Ryan C
Stratingh Institute for Chemistry, University of Groningen, Nijenborgh 4, 9747 AG, Groningen, The Netherlands.
Zernike Institute for Advanced Materials, Nijenborgh 4, 9747 AG, Groningen, The Netherlands.
Angew Chem Int Ed Engl. 2018 Nov 26;57(48):15681-15685. doi: 10.1002/anie.201807879. Epub 2018 Oct 30.
Large-area molecular tunneling junctions comprising self-assembled monolayers of redox-active molecules are described that exhibit two-terminal bias switching. The as-prepared monolayers undergo partial charge transfer to the underlying metal substrate (Au, Pt, or Ag), which converts their cores from a quinoid to a hydroquinoid form. The resulting rearomatization converts the bond topology from a cross-conjugated to a linearly conjugated π system. The cross-conjugated form correlates to the appearance of an interference feature in the transmission spectrum that vanishes for the linearly conjugated form. Owing to the presence of electron-withdrawing nitrile groups, the reduction potential and the interference feature lie close to the work function and Fermi level of the metallic substrate. We exploited the relationship between conjugation patterns and quantum interference to create nonvolatile memory in proto-devices using eutectic Ga-In as the top contact.
描述了由氧化还原活性分子的自组装单分子层组成的大面积分子隧道结,其具有两端偏置开关特性。所制备的单分子层会发生部分电荷转移至下层金属基底(金、铂或银),这会将其核心从醌型转变为对苯二酚型。由此产生的再芳构化将键拓扑结构从交叉共轭转变为线性共轭π体系。交叉共轭形式与透射光谱中一种干涉特征的出现相关,而对于线性共轭形式,该干涉特征消失。由于存在吸电子腈基,还原电位和干涉特征接近于金属基底的功函数和费米能级。我们利用共轭模式与量子干涉之间的关系,以共晶镓铟作为顶部接触,在原型器件中创建了非易失性存储器。