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2. Dimerization of indenocorannulene radicals: imposing stability through increasing strain and curvature

   https://doi.org/10.1039/D0QO00686F  

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   null (Ed.)

   One-electron reduction of bowl-shaped indenocorannulene, C 26 H 12 , with Rb metal in THF affords [{Rb + (18-crown-6)} 2 (C 26 H 12 –C 26 H 12 ) 2− ]·4THF, as confirmed by single-crystal X-ray diffraction. The product consists of a dimeric σ-bonded dianion (C–C, 1.568(7) Å) having two endo -η 6 coordinated {Rb + (18-crown-6)} moieties (Rb–C, 3.272(4)–3.561(4) Å). The (C 26 H 12 –C 26 H 12 ) 2− dimer represents the first crystallographically confirmed example of spontaneous coupling for indenocorannulene monoanion radicals, C 26 H 12 ˙ − . Comprehensive theoretical investigation of the new dimer confirms the single σ-bond character of the linker and reveals a significant increase of both thermodynamic and kinetic stability of [σ-(C 26 H 12 ) 2 ] 2− in comparison with analogues formed by such π-bowls as corannulene and its dibenzo-derivative. The in-depth computational analysis and direct comparison of the series demonstrates the effect of curvature on radical coupling processes, allowing control over stability and reactivity of bowl-shaped π-radicals. 

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5. Temperature-Dependent Spin-Driven Dimerization Determines the Ultrafast Dynamics of a Copper(II)-Bound Tripyrrindione Radical

   https://doi.org/10.1021/acs.jpclett.3c02726  

   Kumar, Anshu ; Thompson, Benjamin ; Gautam, Ritika ; Tomat, Elisa ; Huxter, Vanessa ( December 2023 , The Journal of Physical Chemistry Letters)

   Radicals and other open-shell molecules play a central role in chemical transformations and redox chemistry. While radicals are often highly reactive, stable radical systems are desirable for a range of potential applications, ranging from materials chemistry and catalysis to spintronics and quantum information. Here we investigate the ultrafast properties of a stable radical system with temperature-dependent spin-tunable properties. This radical complex, Cu(II) hexaethyl tripyrrin-1,14-dione, accommodates unpaired electrons localized on both the copper metal center and the tripyrrolic ligand. The unusual combination of two unpaired electrons and high stability in this radical molecule enable switchable temperature-dependent spin coupling. Two-dimensional electronic spectroscopy measurements of Cu(II) hexaethyl tripyrrin-1,14-dione were collected at room temperature and at 77 K. At room temperature, the molecules are present as monomers and have short picosecond lifetimes. At 77 K, the molecules are present in a dimer form mediated by ferromagnetic and antiferromagnetic coupling. This reversible spin-driven dimerization changes the optical properties of the system, generating long-lived excitonic states. 

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