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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.<\/jats:p>","DOI":"10.1126\/sciadv.ado3476","type":"journal-article","created":{"date-parts":[[2024,7,24]],"date-time":"2024-07-24T17:59:07Z","timestamp":1721843947000},"update-policy":"https:\/\/doi.org\/10.34133\/aaas_crossmark","source":"Crossref","is-referenced-by-count":41,"title":["Near-infrared luminescent open-shell \u03c0-conjugated systems with a bright lowest-energy zwitterionic singlet excited state"],"prefix":"10.1126","volume":"10","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1423-5244","authenticated-orcid":true,"given":"Craig P.","family":"Yu","sequence":"first","affiliation":[{"name":"Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK."},{"name":"Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rituparno","family":"Chowdhury","sequence":"additional","affiliation":[{"name":"Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4103-0065","authenticated-orcid":true,"given":"Yao","family":"Fu","sequence":"additional","affiliation":[{"name":"Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5780-3718","authenticated-orcid":true,"given":"Pratyush","family":"Ghosh","sequence":"additional","affiliation":[{"name":"Department of Physics, Cavendish Laboratory, Cambridge University, Cambridge CB3 0HF, UK."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1577-9021","authenticated-orcid":true,"given":"Weixuan","family":"Zeng","sequence":"additional","affiliation":[{"name":"Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3656-9293","authenticated-orcid":true,"given":"Tarig B. 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