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Catholique de Louvain","doi-asserted-by":"publisher","award":["NA"],"award-info":[{"award-number":["NA"]}],"id":[{"id":"10.13039\/501100005041","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,10,14]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>The cage escape yield (\u03a6CE), i.e., the separation of the geminate radical pair formed upon bimolecular excited-state electron transfer, is a key parameter that governs the efficiency of photoredox transformations. For Fe(III) photosensitizers featuring doublet ligand-to-metal charge transfer excited states, \u03a6CE are notoriously small in polar solvents such as acetonitrile yet increase markedly in dichloromethane, an empirical observation that has long remained unexplained. Herein, excited-state quenching and \u03a6CE were quantified for the reaction between the prototypical [Fe(phtmeimb)2]+ photosensitizer and a curated series of 17 nitrogen-based aromatic electron donors whose one-electron oxidation potentials span a potential window of \u223c0.8 eV. We show that \u03a6CE is dictated by the position of the geminate charge recombination on the Marcus parabola: as the driving force for charge recombination becomes more negative, \u03a6CE increases from below 5% to 63% in acetonitrile. Because dichloromethane exhibits a smaller reorganization energy than acetonitrile, its inverted region is reached at less negative driving forces, which quantitatively accounts for the systematically larger \u03a6CE measured in this solvent, even reaching unity. The complete data sets are reproduced by a single nonadiabatic Marcus model, providing a predictive framework for cage escape based solely on driving force and reorganization energy. These results establish that cage escape in open-shell Fe(III) photosensitizers obeys Marcus theory and deliver rational design guidelines for earth-abundant photoredox catalysis.<\/jats:p>","DOI":"10.1021\/jacs.6c16361","type":"journal-article","created":{"date-parts":[[2026,9,29]],"date-time":"2026-09-29T03:02:23Z","timestamp":1790650943000},"page":"43847-43853","source":"Crossref","is-referenced-by-count":0,"title":["Resolving Anomalous\nCage Escape in Fe(III) Photosensitizers:\nA Marcus Theory Framework"],"prefix":"10.1021","volume":"148","author":[{"given":"Sven","family":"Lempereur","sequence":"first","affiliation":[{"name":"Molecular Chemistry, Materials and Catalysis (MOST) , , Place Louis Pasteur 1\/L4.01.02 , ,","place":["Louvain-la-Neuve, Belgium, B-1348"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6717-916X","authenticated-orcid":true,"given":"Felix","family":"Glaser","sequence":"additional","affiliation":[{"name":"Molecular Chemistry, Materials and Catalysis (MOST) , , Place Louis Pasteur 1\/L4.01.02 , ,","place":["Louvain-la-Neuve, Belgium, B-1348"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2193-1536","authenticated-orcid":true,"given":"Yoann","family":"Olivier","sequence":"additional","affiliation":[{"name":"Namur Institute of Structured Matter, University of Namur , , Rue de Bruxelles 61 , ,","place":["Namur, Belgium, 5000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5037-3313","authenticated-orcid":true,"given":"Benjamin","family":"Elias","sequence":"additional","affiliation":[{"name":"Molecular Chemistry, Materials and Catalysis (MOST) , , Place Louis Pasteur 1\/L4.01.02 , ,","place":["Louvain-la-Neuve, Belgium, B-1348"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7690-1361","authenticated-orcid":true,"given":"Ludovic","family":"Troian-Gautier","sequence":"additional","affiliation":[{"name":"Molecular Chemistry, Materials and Catalysis (MOST) , , Place Louis Pasteur 1\/L4.01.02 , ,","place":["Louvain-la-Neuve, Belgium, B-1348"]},{"name":"Wel Research Institute , Avenue Pasteur 6 , ,","place":["Wavre, Belgium, 1300"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,28]]},"reference":[{"key":"2026101414072940700_cit1","doi-asserted-by":"publisher","first-page":"5803","DOI":"10.1039\/C6CS00526H","article-title":"The Photophysics of Photoredox Catalysis: A Roadmap\nfor Catalyst Design","volume":"45","author":"Arias-Rotondo","year":"2016","journal-title":"Chem. Soc. Rev."},{"key":"2026101414072940700_cit2","doi-asserted-by":"publisher","first-page":"102","DOI":"10.1039\/B913880N","article-title":"Visible\nLight Photoredox Catalysis:\nApplications in Organic Synthesis","volume":"40","author":"Narayanam","year":"2011","journal-title":"Chem. Soc.\nRev."},{"key":"2026101414072940700_cit3","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2023.215522","article-title":"The Great\nStrides of Iron Photosensitizers for Contemporary Organic Photoredox\nCatalysis: On Our Way to the Holy Grail?","volume":"500","author":"Glaser","year":"2024","journal-title":"Coord.\nChem. Rev."},{"key":"2026101414072940700_cit4","doi-asserted-by":"publisher","first-page":"746","DOI":"10.1038\/s41557-022-00911-6","article-title":"Ion-Pair Reorganization\nRegulates Reactivity in Photoredox Catalysts","volume":"14","author":"Earley","year":"2022","journal-title":"Nat. Chem."},{"key":"2026101414072940700_cit5","doi-asserted-by":"publisher","first-page":"191","DOI":"10.1126\/science.adj0612","article-title":"Exploiting\nthe Marcus Inverted Region for First-Row Transition Metal\u2013Based\nPhotoredox Catalysis","volume":"382","author":"Chan","year":"2023","journal-title":"Science"},{"key":"2026101414072940700_cit6","doi-asserted-by":"publisher","first-page":"77","DOI":"10.1126\/science.1161976","article-title":"Merging\nPhotoredox Catalysis with Organocatalysis:\nThe Direct Asymmetric Alkylation of Aldehydes","volume":"322","author":"Nicewicz","year":"2008","journal-title":"Science"},{"key":"2026101414072940700_cit7","doi-asserted-by":"publisher","first-page":"5322","DOI":"10.1021\/cr300503r","article-title":"Visible Light Photoredox Catalysis\nwith Transition Metal Complexes: Applications in Organic Synthesis","volume":"113","author":"Prier","year":"2013","journal-title":"Chem. 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Soc."},{"key":"2026101414072940700_cit16","doi-asserted-by":"publisher","DOI":"10.1002\/cptc.202400134","article-title":"A Compendium\nof Methodically Determined Ground- and Excited-State Properties of\nHomoleptic Ruthenium(Ii) and Osmium(Ii) Photosensitizers","volume":"8","author":"Glaser","year":"2024","journal-title":"ChemPhotoChem"},{"key":"2026101414072940700_cit17","doi-asserted-by":"publisher","first-page":"217","DOI":"10.1002\/cptc.202000255","article-title":"A Roadmap\nTowards Visible Light Mediated Electron Transfer Chemistry with Iridium(Iii)\nComplexes","volume":"5","author":"Bevernaegie","year":"2021","journal-title":"ChemPhotoChem"},{"key":"2026101414072940700_cit18","doi-asserted-by":"publisher","first-page":"9540","DOI":"10.1039\/D1CS00311A","article-title":"Recent Advances\nin Visible Light-Activated Radical\nCoupling Reactions Triggered by (I) Ruthenium, (Ii) Iridium and (Iii)\nOrganic Photoredox Agents","volume":"50","author":"Bell","year":"2021","journal-title":"Chem. 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Rev."},{"key":"2026101414072940700_cit22","doi-asserted-by":"publisher","first-page":"5627","DOI":"10.1039\/D5SC07843A","article-title":"Highly-Destabilized\nLigand Field Excited States of Iron Carbene Complexes and Their Relation\nto Charge Transfer State Lifetimes","volume":"17","author":"Hooper","year":"2026","journal-title":"Chem. Sci."},{"key":"2026101414072940700_cit23","doi-asserted-by":"publisher","first-page":"4461","DOI":"10.1021\/acs.inorgchem.3c03972","article-title":"How Rigidity\nand Conjugation of Bidentate Ligands Affect\nthe Geometry and Photophysics of Iron N-Heterocyclic Complexes: A\nComparative Study","volume":"63","author":"Prakash","year":"2024","journal-title":"Inorg. Chem."},{"key":"2026101414072940700_cit24","doi-asserted-by":"publisher","first-page":"26878","DOI":"10.1021\/jacs.6c08685","article-title":"Optimized\nOctahedral Geometry and Hidden Rigidity of a Mer-Tridentate N-Heterocyclic\nCarbene Ligand Enhance Luminescence of an Fe(Iii) Complex","volume":"148","author":"Mochimaru","year":"2026","journal-title":"J. Am. Chem. Soc."},{"key":"2026101414072940700_cit25","doi-asserted-by":"publisher","first-page":"10129","DOI":"10.1039\/D3SC02806B","article-title":"Ferrous and Ferric Complexes with\nCyclometalating N-Heterocyclic Carbene Ligands: A Case of Dual Emission\nRevisited","volume":"14","author":"Johnson","year":"2023","journal-title":"Chem. Sci."},{"key":"2026101414072940700_cit26","doi-asserted-by":"publisher","DOI":"10.1016\/j.checat.2024.101110","article-title":"From Photons\nto Reactions: Key Concepts in Photoredox Catalysis","volume":"4","author":"De Kreijger","year":"2024","journal-title":"Chem. Catal."},{"key":"2026101414072940700_cit27","doi-asserted-by":"publisher","first-page":"7379","DOI":"10.1021\/acs.chemrev.3c00930","article-title":"Factors That\nImpact Photochemical\nCage Escape Yields","volume":"124","author":"Goodwin","year":"2024","journal-title":"Chem. Rev."},{"key":"2026101414072940700_cit28","doi-asserted-by":"publisher","first-page":"8037","DOI":"10.1039\/D1CY01771C","article-title":"Mechanistic\nInvestigation of a Visible Light Mediated Dehalogenation\/Cyclisation\nReaction Using Iron(Iii), Iridium(Iii) and Ruthenium(Ii) Photosensitizers","volume":"11","author":"Aydogan","year":"2021","journal-title":"Catal. Sci. Technol."},{"key":"2026101414072940700_cit29","doi-asserted-by":"publisher","first-page":"15661","DOI":"10.1021\/jacs.1c06081","article-title":"Accessing\nPhotoredox Transformations with an Iron(Iii) Photosensitizer and Green\nLight","volume":"143","author":"Aydogan","year":"2021","journal-title":"J. Am. Chem. Soc."},{"key":"2026101414072940700_cit30","doi-asserted-by":"publisher","first-page":"1151","DOI":"10.1038\/s41557-024-01482-4","article-title":"Cage Escape Governs\nPhotoredox Reaction Rates and Quantum Yields","volume":"16","author":"Wang","year":"2024","journal-title":"Nat. Chem."},{"key":"2026101414072940700_cit31","doi-asserted-by":"publisher","first-page":"22818","DOI":"10.1021\/jacs.4c08158","article-title":"Factors Controlling\nCage Escape Yields of Closed- and Open-Shell Metal Complexes in Bimolecular\nPhotoinduced Electron Transfer","volume":"146","author":"Ripak","year":"2024","journal-title":"J. Am. Chem.\nSoc."},{"key":"2026101414072940700_cit32","doi-asserted-by":"publisher","first-page":"10286","DOI":"10.1021\/jacs.4c02808","article-title":"Investigation\nof the Excited-State Electron Transfer and Cage Escape Yields between\nHalides and a Fe(Iii) Photosensitizer","volume":"146","author":"De Kreijger","year":"2024","journal-title":"J. Am.\nChem. Soc."},{"key":"2026101414072940700_cit33","doi-asserted-by":"publisher","first-page":"8559","DOI":"10.1021\/jacs.4c17167","article-title":"Two Birds, One Stone: Microsecond\nDark Excited-State Lifetime and Large Cage Escape Yield Afforded by\nan Iron\u2013Anthracene Molecular Dyad","volume":"147","author":"Glaser","year":"2025","journal-title":"J.\nAm. Chem. Soc."},{"key":"2026101414072940700_cit34","doi-asserted-by":"publisher","first-page":"3569","DOI":"10.1039\/D2SC05357H","article-title":"Competing Dynamics\nof Intramolecular Deactivation and Bimolecular Charge Transfer Processes\nin Luminescent Fe(Iii) N-Heterocyclic Carbene Complexes","volume":"14","author":"Rosemann","year":"2023","journal-title":"Chem. Sci."},{"key":"2026101414072940700_cit35","doi-asserted-by":"publisher","first-page":"31509","DOI":"10.1021\/jacs.5c04296","article-title":"Understanding Anomalous Cage-Escape\nDynamics in Photoredox Processes Driven by a Fe(Iii) N-Heterocyclic\nCarbene Complex","volume":"147","author":"Losada","year":"2025","journal-title":"J. Am. Chem. Soc."},{"key":"2026101414072940700_cit36","doi-asserted-by":"publisher","first-page":"889","DOI":"10.1039\/C8CY02336K","article-title":"Photoredox Catalysts Based on Earth-Abundant\nMetal Complexes","volume":"9","author":"Hockin","year":"2019","journal-title":"Catal. Sci. Technol."},{"key":"2026101414072940700_cit37","doi-asserted-by":"publisher","first-page":"24619","DOI":"10.1021\/jacs.4c08588","article-title":"Enter Mniv\u2013Nhc:\nA Dark Photooxidant with a Long-Lived\nCharge-Transfer Excited State","volume":"146","author":"Kaul","year":"2024","journal-title":"J. Am. Chem.\nSoc."},{"key":"2026101414072940700_cit38","doi-asserted-by":"publisher","DOI":"10.1002\/chem.202502668","article-title":"Decoupling Redox Potentials and Excited\nState Energies in Substituted Chromium(Iii) Chromophores","volume":"32","author":"Sittel","year":"2026","journal-title":"Chem. - Eur. J."},{"key":"2026101414072940700_cit39","doi-asserted-by":"publisher","first-page":"13244","DOI":"10.1021\/jacs.9b06524","article-title":"Chiral Molecular Ruby [Cr(Dqp)2]3+\nwith Long-Lived Circularly Polarized Luminescence","volume":"141","author":"Jime\u0301nez","year":"2019","journal-title":"J. Am. Chem. 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Res."},{"key":"2026101414072940700_cit43","doi-asserted-by":"publisher","first-page":"8565","DOI":"10.1021\/jacs.0c00755","article-title":"Tracing the Full Bimolecular\nPhotocycle\nof Iron(Iii)\u2013Carbene Light Harvesters in Electron-Donating\nSolvents","volume":"142","author":"Rosemann","year":"2020","journal-title":"J. Am. Chem. Soc."},{"key":"2026101414072940700_cit44","doi-asserted-by":"publisher","first-page":"834","DOI":"10.1002\/bbpc.19690730818","article-title":"Kinetik Und Mechanismus\nDer Elektronu\u0308bertragung\nBei Der Fluoreszenzlo\u0308schung in Acetonitril","volume":"73","author":"Rehm","year":"1969","journal-title":"Berich. Bunsen-Ges. Phys. Chem."},{"key":"2026101414072940700_cit45","doi-asserted-by":"publisher","first-page":"10337","DOI":"10.1021\/jp953110e","article-title":"Dipole Solvation\nin Nondipolar Solvents: Experimental Studies of Reorganization Energies\nand Solvation Dynamics","volume":"100","author":"Reynolds","year":"1996","journal-title":"J. Phys. Chem. A"},{"key":"2026101414072940700_cit46","doi-asserted-by":"publisher","first-page":"176","DOI":"10.1524\/zpch.1954.1.3_4.176","article-title":"U\u0308ber\nDie Kinetik Sehr Schnell Verlaufender Ionenreaktionen in Wa\u0308sseriger\nLo\u0308sung.*","volume":"1","author":"Eigen","year":"1954","journal-title":"Z. Phys. Chem."},{"key":"2026101414072940700_cit47","doi-asserted-by":"publisher","first-page":"115","DOI":"10.1016\/1010-6030(94)03922-H","article-title":"Solvent\nEffects on the Photoinduced Electron Transfer Reaction between Excited\nSinglet Pyrene and Indole","volume":"86","author":"Montejano","year":"1995","journal-title":"J. Photochem. Photobiol.,\nA"},{"key":"2026101414072940700_cit48","doi-asserted-by":"publisher","first-page":"966","DOI":"10.1063\/1.1742723","article-title":"On the\nTheory of Oxidation-Reduction Reactions Involving Electron Transfer.\nI","volume":"24","author":"Marcus","year":"1956","journal-title":"J. Chem. 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