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Solution-Synthesized, Crystallographically Characterized [3]Triangulene Dimer Tetraradical with an Open-Shell Singlet
Yiming Yang1, Qi Xiong2, Yeda Ding1
1State Key Laboratory of Petroleum Molecular & Process Engineering, Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai200062, China.
Solution synthesis of a stable triangulene dimer (TRI-d) was achieved. This breakthrough enables new possibilities for quantum spin functionalities and higher-order triangulene structures.
Area of Science:
- Organic Chemistry
- Materials Science
- Quantum Physics
Background:
- Triangulene, a non-Kekulé hydrocarbon, has been studied extensively, but solution-phase dimers were inaccessible.
- Previous studies focused on surface-bound triangulene dimers, limiting their characterization in solution.
Purpose of the Study:
- To synthesize and characterize a stable triangulene dimer in solution.
- To investigate the magnetic and spin properties of the triangulene dimer.
- To explore potential applications in quantum spin technologies.
Main Methods:
- Solution synthesis and single-crystal structural characterization of a β-β-linked triangulene dimer (TRI-d).
- Pulsed Electron Paramagnetic Resonance (EPR) and magnetic measurements.
- Continuous-wave (cw) EPR spectroscopy.
Main Results:
- Kinetically stabilized TRI-d was synthesized and structurally characterized, exhibiting a twisted geometry.
- Weak antiferromagnetic coupling (J = -3.47 meV) was observed, leading to a singlet ground state.
- TRI-d shows millisecond spin-lattice relaxation and microsecond coherence, with the S = 2 state detectable by cw-EPR.
Conclusions:
- The successful synthesis of TRI-d overcomes previous experimental limitations for solution-phase triangulene dimers.
- TRI-d's stability and spin properties make it a promising building block for advanced materials.
- This work opens avenues for constructing higher-order triangulene oligomers and exploring quantum spin functionalities.
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