原子操纵生成的非苯型高自旋多环烃
Non-benzenoid high-spin polycyclic hydrocarbons generated by atom manipulation
摘要：
我们报道了在钴金属和绝缘体表面上通过三聚氧乙烯（C27H18）脱氢合成非苯型三自由基。通过扫描隧道显微镜/原子力显微镜的尖端施加的电压脉冲被用来切割truxene中的单个C-H键。采用原子力显微镜、扫描隧道显微镜和扫描隧道光谱的组合在单分子尺度上表征了最终产物truxene-5，10，15-triyl（1）。我们的分析表明，在Cu（111）表面的两个单层厚的NaCl层上，1保留了密度泛函理论预测的开壳层四重态基态。我们的图像前线轨道密度1，并确认它们对应于自旋分裂单占据分子轨道。通过我们的合成策略，我们还分离了两个反应中间体，分别用于合成芴基自由基和茚并[1，2-a]芴的1-衍生物，具有预测的自旋二重态和自旋三重态基态。我们的研究结果应该有轴承的非苯型高自旋多环框架的磁性超出Lieb定理的合成。
英文摘要：
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.
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