Near-infrared luminescent open-shell π-conjugated systems with a bright lowest-energy zwitterionic singlet excited state.

Autor: Yu CP; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK.; Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK., Chowdhury R; Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK., Fu Y; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK., Ghosh P; Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK., Zeng W; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK., Mustafa TBE; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK.; Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK., Grüne J; Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK., Walker LE; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK., Congrave DG; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK., Chua XW; Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK., Murto P; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK.; Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK., Rao A; Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK., Sirringhaus H; Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK., Plasser F; Department of Chemistry, Loughborough University, Loughborough, LE11 3TU, UK., Grey CP; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK., Friend RH; Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK., Bronstein H; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK.; Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK.
Jazyk: angličtina
Zdroj: Science advances [Sci Adv] 2024 Jul 26; Vol. 10 (30), pp. eado3476. Date of Electronic Publication: 2024 Jul 24.
DOI: 10.1126/sciadv.ado3476
Abstrakt: Open-shell systems with extensive π-conjugation have fascinating properties due to their narrow bandgaps and spin interactions. In this work, we report neutral open-shell di- and polyradical conjugated materials exhibiting intriguing optical and magnetic properties. Our key design advance is the planarized geometry allowing for greater interaction between adjacent spins. This results in absorption and emission in the near infrared at 803 and 1050 nanometers, respectively, and we demonstrate a unique electronic structure where a bright zwitterionic excited state is the lowest-accessible electronic transition. Electron paramagnetic resonance spectroscopy and superconducting quantum interference device measurements reveal that our materials are open-shell singlets with different degrees of spin interactions, dynamics, and antiferromagnetic properties, which likely contributed to the formation of their emissive zwitterionic singlet excited state and near-infrared emission. In addition, our materials show reversible and stable electrochromic switching with more than 500 cycles, indicating their potential for optoelectronic and electrochemical energy storage applications.
Databáze: MEDLINE
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