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Extending LMCT absorption into the visible region utilizing strongly donating ligands often leads to ligand dissociation and further decomposition, which highlights the intrinsic trade\u2010off between spectral response and structural robustness in homogeneous systems. In this context, we reconfigure LMCT chemistry within heterogeneous single\u2010atom catalysts, where rigid coordination environments that decouple electronic excitation from (photo)stability. Low\u2010energy LMCT excited states are implemented into single\u2010atom photocatalysts through incorporating site\u2010specific Co\n                    <jats:sub>1<\/jats:sub>\n                    \u2010C\n                    <jats:sub>2<\/jats:sub>\n                    N\n                    <jats:sub>1<\/jats:sub>\n                    moiety. Multimodal synchrotron x\u2010ray spectroscopies reveal that the pseudo square\u2010planar geometry fosters a low spin Co(II) state (\n                    <jats:italic>s<\/jats:italic>\n                    = 1\/2) with pronounced Jahn\u2010Teller distortion. Crucially, enhanced d\n                    <jats:sub>z<\/jats:sub>\n                    <jats:sup>2<\/jats:sup>\n                    \u2010p\n                    <jats:sub>z<\/jats:sub>\n                    orbital coupling gives access to visible\u2010light responsive LMCT states, fundamentally different from the predominant metal\u2010to\u2010ligand charge transfer excitations in conventional Co\n                    <jats:sub>1<\/jats:sub>\n                    \u2010N\n                    <jats:sub>2<\/jats:sub>\n                    counterpart. Electron localization at Co\u2500C pairs creates photoreduction centers in close proximity, facilitating selective benzyl alcohol oxidation via a singlet oxygen (\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    )\u2010mediated pathway. This work establishes single\u2010atom frontier\u2010orbital engineering for exploring visible\u2010light photochemistry in heterogeneous photocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.7984934","type":"journal-article","created":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T07:45:12Z","timestamp":1790754312000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Spin Crossover\u2010Mediated Low\u2010Energy Charge Transfer Excited States in a Heterogeneous Cobalt Photocatalyst"],"prefix":"10.1002","author":[{"given":"Tianna","family":"Liu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Fine Chemicals, School of Chemistry, Frontier Science Center for Smart Materials Dalian University of Technology  Dalian China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenzhe","family":"Shang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Fine Chemicals, School of Chemistry, Frontier Science Center for Smart Materials Dalian University of Technology  Dalian China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-1502-5118","authenticated-orcid":false,"given":"Wei","family":"Che","sequence":"additional","affiliation":[{"name":"School of Energy and Chemical Engineering\/Center for Dimension Controllable Organic Frameworks Ulsan National Institute of Science and Technology (UNIST)  Ulsan Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wentao","family":"Peng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Fine Chemicals, School of Chemistry, Frontier Science Center for Smart Materials Dalian University of Technology  Dalian 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