State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemical and Biochemical Engineering, College of Chemistry and Chemical Engineering, Graphene Industry and Engineering Research Institute, iChEM, Xiamen University, Xiamen, 361005, China.
Department of Chemistry, Durham University, Durham, DH1 3LE, UK.
Angew Chem Int Ed Engl. 2017 Oct 9;56(42):13061-13065. doi: 10.1002/anie.201707710. Epub 2017 Sep 12.
We studied the single-molecule conductance through an acid oxidant triggered phenothiazine (PTZ-) based radical junction using the mechanically controllable break junction technique. The electrical conductance of the radical state was enhanced by up to 200 times compared to the neutral state, with high stability lasting for at least two months and high junction formation probability at room-temperature. Theoretical studies revealed that the conductance increase is due to a significant decrease of the HOMO-LUMO gap and also the enhanced transmission close to the HOMO orbital when the radical forms. The large conductance enhancement induced by the formation of the stable PTZ radical molecule will lead to promising applications in single-molecule electronics and spintronics.
我们使用机械可控断键技术研究了单分子电导通过酸氧化剂触发的吩噻嗪（PTZ-）基自由基结。与中性状态相比，自由基状态的电导增强了高达 200 倍，具有至少两个月的高稳定性和室温下高的结形成概率。理论研究表明，电导的增加是由于自由基形成时 HOMO-LUMO 能隙显著减小，以及 HOMO 轨道附近的传输增强。稳定的 PTZ 自由基分子形成引起的大电导增强将导致在单分子电子学和自旋电子学中有很有前景的应用。
