Univ Rennes, CNRS, Institut des Sciences Chimiques de Rennes (ISCR) - UMR 6226, F-35000 Rennes, France.
Inorg Chem. 2020 Nov 2;59(21):15772-15779. doi: 10.1021/acs.inorgchem.0c02207. Epub 2020 Oct 19.
Mixed-valence compounds can be used for the design of molecular quantum-dot cellular automata (QCA). Here, we investigate the QCA properties of a three-dot "Y"-shaped functionalized zwitterionic neutral -carborane model 1-(3,5-{Cp(dHpe)Fe-C≡C-}(CH))-10-Cp(dHpe)Fe-C≡C--1-CBH () (Cp = cyclopentadienyl (η-CH) and dHpe = 1,2-bis(phosphino)ethane (HPCHCHPH)) as a neutral clocked molecular half-cell. DFT results clearly demonstrate that can display simultaneously the two most basic properties necessary for clocked QCA operation, i.e., bistable switching behavior and clocked control. This is possible due to the three stable states (two active and one null) of , corresponding to occupation of each of the three iron-ethynyl groups by the positive charge. In addition, the proximal electronic bias effects can be overcome by the zwitterionic nature of , which could be imposed by external counterions, rendering these effects more predictable.
混合价态化合物可用于设计分子量子点细胞自动机 (QCA)。在这里，我们研究了三点点状“Y”形功能化两性离子中性 -卡硼烷模型 1-(3,5-{Cp(dHpe)Fe-C≡C-}(CH))-10-Cp(dHpe)Fe-C≡C--1-CBH()（Cp=环戊二烯基（η-CH），dHpe=1,2-双(膦基)乙烷（HPCHCHPH））作为中性时钟分子半电池的 QCA 性质。DFT 结果清楚地表明， 可以同时显示出时钟 QCA 操作所需的两个最基本的性质，即双稳开关行为和时钟控制。这是可能的，因为 的三个稳定状态（两个活性和一个空），对应于每个铁-乙炔基基团被正电荷占据。此外，由于 的两性离子性质，可以克服近端电子偏置效应，这可以通过外部抗衡离子施加，使这些效应更可预测。
