Nonbenzenoid High-Spin Polycyclic Hydrocarbons Generated by Atom Manipulation
| Autor: | Shantanu Mishra, Shadi Fatayer, Saleta Fernández, Katharina Kaiser, Diego Peña, Leo Gross |
|---|---|
| Rok vydání: | 2022 |
| Předmět: | |
| Zdroj: | ACS Nano |
| ISSN: | 1936-086X |
| Popis: | 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. 8 pages, 5 figures and supporting information containing additional data |
| Databáze: | OpenAIRE |
| Externí odkaz: |
|