Jaroš Adam, Bonab Esmaeil Farajpour, Straka Michal, Foroutan-Nejad Cina
Institute of Organic Chemistry and Biochemistry of the Czech Academy of Sciences , Flemingovo nám. 2 , CZ-16610 Prague , Czech Republic.
Faculty of Science , Charles University , Albertov 2038/6 , CZ-12843 Prague 2 , Czech Republic.
J Am Chem Soc. 2019 Dec 18;141(50):19644-19654. doi: 10.1021/jacs.9b07215. Epub 2019 Dec 4.
Employing multiscale in silico modeling, we propose switching molecular diodes on the basis of endohedral fullerenes (fullerene switching diode, FSD), encapsulated with polar molecules of general type MX (M: metal, X: nonmetal) to be used for data storage and processing. Here, we demonstrate for MX@C systems that the relative orientation of enclosed MX with respect to a set of electrodes connected to the system can be controlled by application of oriented external electric field(s). We suggest systems with two- and four-terminal electrodes, in which the source and drain electrodes help the current to pass through the device and help the switching between the conductive states of FSD via applied voltage. The gate electrodes then assist the switching by effectively lowering the energy barrier between local minima via stabilizing the transition state of switching process if the applied voltage between the source and drain is insufficient to switch the MX inside the fullerene. Using nonequilibrium Green's function combined with density functional theory (DFT-NEGF) computations, we further show that conductivity of the studied MX@C systems depends on the relative orientation of MX inside the cage with respect to the electrodes. Therefore, the orientation of the MX inside C can be both enforced ("written") and retrieved ("read") by applied voltage. The studied systems thus behave like voltage-sensitive switching molecular diodes, which is reminiscent of a molecular memristor.
利用多尺度计算机模拟，我们提出基于内嵌富勒烯（富勒烯开关二极管，FSD）的分子二极管切换，该富勒烯由通用类型MX（M：金属，X：非金属）的极性分子封装，用于数据存储和处理。在此，我们针对MX@C系统证明，通过施加定向外部电场，可以控制封闭的MX相对于连接到该系统的一组电极的相对取向。我们提出了具有两终端和四终端电极的系统，其中源电极和漏电极有助于电流通过器件，并通过施加电压帮助FSD在导电状态之间切换。如果源电极和漏电极之间施加的电压不足以切换富勒烯内部的MX，则栅电极通过稳定开关过程的过渡态有效降低局部极小值之间的能垒来辅助切换。结合非平衡格林函数与密度泛函理论（DFT-NEGF）计算，我们进一步表明，所研究的MX@C系统的电导率取决于笼内MX相对于电极的相对取向。因此，C内MX的取向可以通过施加电压来强制（“写入”）和恢复（“读取”）。所研究的系统因此表现得像电压敏感型开关分子二极管，这让人联想到分子忆阻器。
