论文标题
非原子操纵产生的非苯甲酸高自旋多环烃
Non-benzenoid high-spin polycyclic hydrocarbons generated by atom manipulation
论文作者
论文摘要
我们通过三核酸（C27H18）在造币金属和绝缘体表面上脱氢（C27H18）的脱氢作用来报告非苯甲醇三片的地面合成。通过组合扫描隧道显微镜/原子力显微镜的尖端施加的电压脉冲用于在三税中裂解单个C-H键。最终产物Truxene-5,10,15-三酰基（1）在单分子尺度上使用原子力显微镜，扫描隧道显微镜和扫描隧道光谱的组合进行表征。我们的分析表明，1保留其在Cu（111）表面上的两个单层厚的NaCl层上，由密度功能理论预测的开放壳四重奏基态预测。我们对1的边缘轨道密度进行成像，并确认它们对应于单单占单独占据的分子轨道。通过我们的合成策略，我们还分离了两个反应性中间体，分别将氟苯基自由基和indeno [1,2-a]氟的1-衍生物分别分离出，分别具有预测的自旋 - doublet和自旋 - 三个基态。我们的结果应该具有与Lieb定理外的磁性的非双苯并且高自旋多环形框架合成的轴承。
We report the on-surface synthesis of a non-benzenoid triradical through dehydrogenation of truxene (C27H18) on coinage metal and insulator surfaces. Voltage pulses applied via the tip of a combined scanning tunneling microscope/atomic force microscope were used to cleave individual C-H bonds in truxene. The resultant final product truxene-5,10,15-triyl (1) was characterized at the single-molecule scale using a combination of atomic force microscopy, scanning tunneling microscopy and scanning tunneling spectroscopy. Our analyses show that 1 retains its open-shell quartet ground state, predicted by density functional theory, on a two monolayer-thick NaCl layer on a Cu(111) surface. We image the frontier orbital densities of 1 and confirm that they correspond to spin-split singly occupied molecular orbitals. Through our synthetic strategy, we also isolate two reactive intermediates toward the synthesis of 1 - derivatives of fluorenyl radical and indeno[1,2-a]fluorene, with predicted spin-doublet and spin-triplet ground states, respectively. Our results should have bearings on the synthesis of non-benzenoid high-spin polycyclic frameworks with magnetism beyond Lieb's theorem.
