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<p>As a renowned class of open-shell molecules characterized by triangular nanographenic structures and novel magnetic properties with high-spin ground states, triangulenes are attractive targets to both synthetic chemists and molecular magnet researchers. Here, a highly stable aza-derivative of [4]triangulene triradical (<b>1</b>) is achieved, with a quartet ground state (<i>S</i> = 3/2). By virtue of the stability under ambient conditions (<i>τ</i><sub>1/2</sub> ~ 9 days in the solid state and 28 h in an air-saturated solution), thorough structural and magnetic characterizations are performed. Crystallographic analysis confirms that <b>1</b> has&#xa0;a planar triangular polycyclic aromatic skeleton embedded with delocalized spins. Concurrently, continuous-wave and pulsed EPR spectroscopies provide unambiguous evidence supporting its high-spin ground state. SQUID measurements reveal impressively large doublet-quartet energy gap (Δ<i>E</i><sub>D-Q</sub> = 3.18 kcal/mol), indicating very strong intramolecular ferromagnetic spin-spin exchanges (<i>J</i>/<i>k</i><sub>B</sub> = +534 K) rendered by the triangulene structure.</p>

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Solution-synthesized stable triaza[4]triangulene triradical with a quartet ground state

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月3日

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  • Xudong Bai,
  • Di Zhang,
  • Yushuang Zhang,
  • Yihan Wang,
  • Yanning Cheng,
  • Yi Xie,
  • Ziqi Zhu,
  • Shang-Da Jiang,
  • Dahui Zhao

摘要

As a renowned class of open-shell molecules characterized by triangular nanographenic structures and novel magnetic properties with high-spin ground states, triangulenes are attractive targets to both synthetic chemists and molecular magnet researchers. Here, a highly stable aza-derivative of [4]triangulene triradical (1) is achieved, with a quartet ground state (S = 3/2). By virtue of the stability under ambient conditions (τ1/2 ~ 9 days in the solid state and 28 h in an air-saturated solution), thorough structural and magnetic characterizations are performed. Crystallographic analysis confirms that 1 has a planar triangular polycyclic aromatic skeleton embedded with delocalized spins. Concurrently, continuous-wave and pulsed EPR spectroscopies provide unambiguous evidence supporting its high-spin ground state. SQUID measurements reveal impressively large doublet-quartet energy gap (ΔED-Q = 3.18 kcal/mol), indicating very strong intramolecular ferromagnetic spin-spin exchanges (J/kB = +534 K) rendered by the triangulene structure.