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Metal\u2013organic frameworks (MOFs) are a promising architecture to leverage such opportunities since they offer control over spin placement, tunable porosity and large internal surface areas for efficient integration with sensing targets, and a richly tunable chemical space. However, optical spin readout has not been demonstrated in a MOF. Here, we report the first successful optical detection of spins in a MOF. We use a porphyrin-based aluminum MOF (Al-PMOF), which supports efficient triplet generation on the porphyrin chromophore ligands. Using electron paramagnetic resonance, we demonstrate that these triplet states support a spin coherence time (T2) on the order of a few microseconds at 50 K. Importantly, we successfully detect optically detected magnetic resonance of these triplets using near-infrared ODMR at 77 K. Optical spin readout in a MOF paves the way for next-generation quantum sensing applications that leverage bottom-up assembly.<\/jats:p>","DOI":"10.1021\/jacs.6c12867","type":"journal-article","created":{"date-parts":[[2026,10,9]],"date-time":"2026-10-09T06:01:55Z","timestamp":1791525715000},"page":"44541-44548","source":"Crossref","is-referenced-by-count":0,"title":["Optically Addressable Spins in a Metal\u2013Organic\nFramework"],"prefix":"10.1021","volume":"148","author":[{"given":"Miku","family":"Inoue","sequence":"first","affiliation":[{"name":"The University of Tokyo , , ,","place":["Tokyo, Japan, 113-0033"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wataru","family":"Ishii","sequence":"additional","affiliation":[{"name":"The University of Tokyo , , ,","place":["Tokyo, Japan, 113-0033"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Thomas W.","family":"Bradbury","sequence":"additional","affiliation":[{"name":"University of Sheffield , , ,","place":["Sheffield, U.K., S3 7RT"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hiroki","family":"Nagashima","sequence":"additional","affiliation":[{"name":"Saitama University , , 255 Shimo-Okubo, Sakura-ku , ,","place":["Saitama, Japan, 338-8570"]},{"name":"National Institutes for Quantum Science and Technology (QST) , , 4-9-1 Anagawa, Inage-ku , ,","place":["Chiba, Japan, 263-8555"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6371-6047","authenticated-orcid":true,"given":"Alistair","family":"Inglis","sequence":"additional","affiliation":[{"name":"University of Glasgow , , ,","place":["Glasgow, U.K., G12 8QQ"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yoshitaka","family":"Aoyama","sequence":"additional","affiliation":[{"name":"JEOL Ltd. , 3-1-2 Musashino , , ,","place":["Akishima, Tokyo, Japan, 196-8558"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7136-1127","authenticated-orcid":true,"given":"Yusuke","family":"Nishiyama","sequence":"additional","affiliation":[{"name":"JEOL Ltd. , 3-1-2 Musashino , , ,","place":["Akishima, Tokyo, Japan, 196-8558"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mizue","family":"Asada","sequence":"additional","affiliation":[{"name":"Institute for Molecular Science , Nishigonaka 38, Myodaiji , , ,","place":["Okazaki, Aichi, Japan, 444-8585"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8672-0946","authenticated-orcid":true,"given":"Toshikazu","family":"Nakamura","sequence":"additional","affiliation":[{"name":"Institute for Molecular Science , Nishigonaka 38, Myodaiji , , ,","place":["Okazaki, Aichi, Japan, 444-8585"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7419-343X","authenticated-orcid":true,"given":"Kiminori","family":"Maeda","sequence":"additional","affiliation":[{"name":"Saitama University , , 255 Shimo-Okubo, Sakura-ku , ,","place":["Saitama, Japan, 338-8570"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yasuhiro","family":"Kobori","sequence":"additional","affiliation":[{"name":"Kobe University , , 1-1 Rokkodaicho Nada-ku , ,","place":["Kobe, Japan, 657-8501"]},{"name":"Kobe University , , 1-1, Rokkodai-Cho, Nada-ku , ,","place":["Kobe, Japan, 657-8501"]},{"name":"JST , , Honcho 4-1-8 , , ,","place":["Kawaguchi, Saitama, Japan, 332-0012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9664-967X","authenticated-orcid":true,"given":"Jenny","family":"Clark","sequence":"additional","affiliation":[{"name":"University of Sheffield , , ,","place":["Sheffield, U.K., S3 7RT"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1156-7243","authenticated-orcid":true,"given":"Sam L.","family":"Bayliss","sequence":"additional","affiliation":[{"name":"University of Glasgow , , ,","place":["Glasgow, U.K., G12 8QQ"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0297-6544","authenticated-orcid":true,"given":"Nobuhiro","family":"Yanai","sequence":"additional","affiliation":[{"name":"The University of Tokyo , , ,","place":["Tokyo, Japan, 113-0033"]},{"name":"JST , , Honcho 4-1-8 , , ,","place":["Kawaguchi, Saitama, Japan, 332-0012"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,9]]},"reference":[{"key":"2026102111092980000_cit1","doi-asserted-by":"publisher","first-page":"644","DOI":"10.1038\/nature07279","article-title":"Nanoscale magnetic sensing\nwith an individual electronic spin in 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X"},{"key":"2026102111092980000_cit6","doi-asserted-by":"publisher","first-page":"383","DOI":"10.1038\/nmat2420","article-title":"Ultralong spin coherence time in isotopically engineered\ndiamond","volume":"8","author":"Balasubramanian","year":"2009","journal-title":"Nat. Mater."},{"key":"2026102111092980000_cit7","doi-asserted-by":"publisher","first-page":"74","DOI":"10.1038\/s41586-025-09524-8","article-title":"Spin squeezing in an ensemble of nitrogen-vacancy centres\nin diamond","volume":"646","author":"Wu","year":"2025","journal-title":"Nature"},{"key":"2026102111092980000_cit8","doi-asserted-by":"publisher","first-page":"1646","DOI":"10.1016\/j.jlumin.2009.12.028","article-title":"Fabrication of single\noptical centres in diamond\u2500a review","volume":"130","author":"Orwa","year":"2010","journal-title":"J. Lumin."},{"key":"2026102111092980000_cit9","doi-asserted-by":"publisher","first-page":"9803","DOI":"10.1038\/s41467-025-64758-4","article-title":"Scalable nanoscale positioning of highly coherent color\ncenters in prefabricated diamond nanostructures","volume":"16","author":"Kim","year":"2025","journal-title":"Nat. Commun."},{"key":"2026102111092980000_cit10","doi-asserted-by":"publisher","first-page":"557","DOI":"10.1126\/science.1231540","article-title":"Nanoscale Nuclear Magnetic Resonance with a Nitrogen-Vacancy Spin\nSensor","volume":"339","author":"Mamin","year":"2013","journal-title":"Science"},{"key":"2026102111092980000_cit11","doi-asserted-by":"publisher","first-page":"195422","DOI":"10.1103\/PhysRevB.86.195422","article-title":"Detecting external electron spins\nusing nitrogen-vacancy centers","volume":"86","author":"Mamin","year":"2012","journal-title":"Phys. Rev. B"},{"key":"2026102111092980000_cit12","doi-asserted-by":"publisher","first-page":"1309","DOI":"10.1126\/science.abb9352","article-title":"Optically addressable molecular spins for quantum information\nprocessing","volume":"370","author":"Bayliss","year":"2020","journal-title":"Science"},{"key":"2026102111092980000_cit13","doi-asserted-by":"publisher","first-page":"538","DOI":"10.1038\/s41586-023-06222-1","article-title":"Reversible spin-optical interface in luminescent organic\nradicals","volume":"620","author":"Gorgon","year":"2023","journal-title":"Nature"},{"key":"2026102111092980000_cit14","doi-asserted-by":"publisher","first-page":"27935","DOI":"10.1021\/jacs.4c11116","article-title":"Luminescent Organic Triplet Diradicals\nas Optically Addressable Molecular Qubits","volume":"146","author":"Kopp","year":"2024","journal-title":"J.\nAm. Chem. Soc."},{"key":"2026102111092980000_cit15","doi-asserted-by":"publisher","first-page":"120801","DOI":"10.1103\/PhysRevLett.133.120801","article-title":"Room-Temperature\nOptically Detected Coherent Control of Molecular Spins","volume":"133","author":"Mena","year":"2024","journal-title":"Phys. Rev. Lett."},{"key":"2026102111092980000_cit16","doi-asserted-by":"publisher","first-page":"10530","DOI":"10.1038\/s41467-025-65508-2","article-title":"High sensitivity\npressure and temperature quantum sensing in pentacene-doped p-terphenyl\nsingle crystals","volume":"16","author":"Singh","year":"2025","journal-title":"Nat. Commun."},{"key":"2026102111092980000_cit17","doi-asserted-by":"publisher","first-page":"312","DOI":"10.1557\/s43577-026-01071-5","article-title":"Optically addressable molecular spin qubits","volume":"51","author":"Mann","year":"2026","journal-title":"MRS Bull."},{"key":"2026102111092980000_cit18","doi-asserted-by":"publisher","first-page":"1410","DOI":"10.1038\/s41557-025-01875-z","article-title":"Bright triplet and bright charge-separated\nsinglet excitons in organic diradicals enable optical read-out and\nwriting of spin states","volume":"17","author":"Chowdhury","year":"2025","journal-title":"Nat. Chem."},{"key":"2026102111092980000_cit19","doi-asserted-by":"publisher","first-page":"36383","DOI":"10.1021\/jacs.5c10272","article-title":"Optically Detected Magnetic\nResonance on Carbene Molecular Qubits","volume":"147","author":"Roggors","year":"2025","journal-title":"J. Am.\nChem. Soc."},{"key":"2026102111092980000_cit20","doi-asserted-by":"publisher","first-page":"7089","DOI":"10.1021\/jacs.7b03123","article-title":"A Porous Array of\nClock Qubits","volume":"139","author":"Zadrozny","year":"2017","journal-title":"J. Am. Chem. Soc."},{"key":"2026102111092980000_cit21","doi-asserted-by":"publisher","first-page":"12090","DOI":"10.1021\/jacs.8b06733","article-title":"Scaling Up Electronic Spin Qubits into a Three-Dimensional\nMetal-Organic Framework","volume":"140","author":"Yamabayashi","year":"2018","journal-title":"J. Am. Chem. Soc."},{"key":"2026102111092980000_cit22","doi-asserted-by":"publisher","first-page":"15485","DOI":"10.1021\/jacs.5c17789","article-title":"Quantum Coherence in\na Perylene-Based Metal-Organic Framework for Potential Solid-State\nQubits","volume":"148","author":"Rani","year":"2026","journal-title":"J. Am. Chem. Soc."},{"key":"2026102111092980000_cit23","doi-asserted-by":"publisher","first-page":"2963","DOI":"10.1021\/acs.accounts.4c00333","article-title":"Toward Quantum Noses: Quantum Chemosensing Based on Molecular Qubits\nin Metal-Organic Frameworks","volume":"57","author":"Yamauchi","year":"2024","journal-title":"Acc. Chem. Res."},{"key":"2026102111092980000_cit24","doi-asserted-by":"publisher","first-page":"31930","DOI":"10.1021\/jacs.5c09638","article-title":"Ultralong Room-Temperature Qubit Lifetimes of Covalent Organic Frameworks","volume":"147","author":"Sun","year":"2025","journal-title":"J. Am. Chem. Soc."},{"key":"2026102111092980000_cit25","doi-asserted-by":"publisher","first-page":"10684","DOI":"10.1021\/jacs.5c20171","article-title":"Advancing Room-Temperature\nSpin Qubits with Naphthalene Diimide-Based Chiral Covalent Organic\nFrameworks","volume":"148","author":"Tang","year":"2026","journal-title":"J. Am. Chem. Soc."},{"key":"2026102111092980000_cit26","doi-asserted-by":"publisher","first-page":"7622","DOI":"10.1038\/s41467-024-51715-w","article-title":"Modulation\nof triplet quantum coherence by guest-induced structural changes in\na flexible metal-organic framework","volume":"15","author":"Yamauchi","year":"2024","journal-title":"Nat. Commun."},{"key":"2026102111092980000_cit27","doi-asserted-by":"publisher","first-page":"6130","DOI":"10.1039\/D4CC01564A","article-title":"Guest-responsive coherence\ntime of radical qubits in a metal-organic framework","volume":"60","author":"Inoue","year":"2024","journal-title":"Chem. Commun."},{"key":"2026102111092980000_cit28","doi-asserted-by":"publisher","DOI":"10.26434\/chemrxiv-2025-xt8h4","article-title":"Sublevel-Selective Electron Spin Hyerpolarization\nof Triplet Radical Pairs in Metal\u2013Organic Frameworks","author":"Hamachi","year":"2025","journal-title":"ChemRxiv"},{"key":"2026102111092980000_cit29","doi-asserted-by":"publisher","first-page":"553","DOI":"10.1021\/acssensors.4c03229","article-title":"Employing Triphenylene-Based, Layered,\nConductive Metal-Organic Framework Materials as Electrochemical Sensors\nfor Nitric Oxide in Aqueous Media","volume":"10","author":"Ambrogi","year":"2025","journal-title":"ACS Sens."},{"key":"2026102111092980000_cit30","doi-asserted-by":"publisher","first-page":"5815","DOI":"10.1039\/C4CS00010B","article-title":"Luminescent metal-organic frameworks\nfor chemical sensing and explosive detection","volume":"43","author":"Hu","year":"2014","journal-title":"Chem. Soc. Rev."},{"key":"2026102111092980000_cit31","doi-asserted-by":"publisher","first-page":"3242","DOI":"10.1039\/C6CS00930A","article-title":"Metal-organic frameworks: functional luminescent and\nphotonic materials for sensing applications","volume":"46","author":"Lustig","year":"2017","journal-title":"Chem. Soc. Rev."},{"key":"2026102111092980000_cit32","doi-asserted-by":"publisher","first-page":"28","DOI":"10.1016\/j.ccr.2017.06.007","article-title":"Luminescent sensors based on metal-organic frameworks","volume":"354","author":"Zhang","year":"2018","journal-title":"Coord. Chem. Rev."},{"key":"2026102111092980000_cit33","doi-asserted-by":"publisher","first-page":"6737","DOI":"10.1021\/acs.jpclett.2c01429","article-title":"Atomic-Scale Quantum Sensing of Ensembles\nof Guest Molecules in a Metal\u2013Organic Framework with Intrinsic\nElectron Spin Centers","volume":"13","author":"Kultaeva","year":"2022","journal-title":"J. Phys. Chem. Lett."},{"key":"2026102111092980000_cit34","doi-asserted-by":"publisher","first-page":"19008","DOI":"10.1021\/jacs.2c07692","article-title":"Room-Temperature Quantitative Quantum Sensing\nof Lithium Ions with a Radical-Embedded Metal-Organic Framework","volume":"144","author":"Sun","year":"2022","journal-title":"J. Am. Chem. Soc."},{"issue":"20","key":"2026102111092980000_cit35","doi-asserted-by":"publisher","first-page":"4334","DOI":"10.1021\/acs.jpca.1c01839","article-title":"Design Guidelines to\nElongate Spin-Lattice Relaxation Times of Porphyrins with Large Triplet\nElectron Polarization","volume":"125","author":"Yamauchi","year":"2021","journal-title":"J. Phys. Chem. A"},{"key":"2026102111092980000_cit36","doi-asserted-by":"publisher","first-page":"1509","DOI":"10.1021\/acsinfecdis.2c00131","article-title":"Antibacterial Photodynamic\nTherapy in the Near-Infrared Region with a Targeting Antimicrobial\nPeptide Connected to a \u03c0-Extended Porphyrin","volume":"8","author":"Gourlot","year":"2022","journal-title":"ACS Infect. Dis."},{"key":"2026102111092980000_cit37","doi-asserted-by":"publisher","first-page":"403","DOI":"10.1007\/s11120-009-9407-5","article-title":"Optically\nDetected Magnetic Resonance (ODMR) of photoexcited triplet states","volume":"102","author":"Carbonera","year":"2009","journal-title":"Photosynth. Res."},{"key":"2026102111092980000_cit38","doi-asserted-by":"publisher","first-page":"4073","DOI":"10.1063\/1.1677817","article-title":"Zero-Field Splitting of the Triplet\nState in Zinc Etioporphyrin","volume":"56","author":"Gouterman","year":"1972","journal-title":"J. Chem. Phys."},{"key":"2026102111092980000_cit39","doi-asserted-by":"publisher","first-page":"221","DOI":"10.1016\/0009-2614(73)80123-X","article-title":"Investigation of the lowest triplet state of free base\nporphin by microwave induced changes in its fluorescence","volume":"21","author":"Van Dorp","year":"1973","journal-title":"Chem. Phys. Lett."},{"key":"2026102111092980000_cit40","doi-asserted-by":"publisher","first-page":"169","DOI":"10.1063\/1.430249","article-title":"Zero field\nsplitting of the triplet state of porphyrins. II","volume":"62","author":"Langhoff","year":"1975","journal-title":"J. Chem. Phys."},{"key":"2026102111092980000_cit41","doi-asserted-by":"publisher","first-page":"3535","DOI":"10.1063\/1.438743","article-title":"Optically detected magnetic resonance\nof the \u03bc-oxo bridged porphyrin dimer","volume":"71","author":"Leenstra","year":"1979","journal-title":"J. Chem. Phys."},{"key":"2026102111092980000_cit42","doi-asserted-by":"publisher","first-page":"161","DOI":"10.1016\/0301-0104(84)85164-2","article-title":"ODMR of triplet states of cofacial dimeric zinc porphyrins","volume":"86","author":"Gu\u0308ckel","year":"1984","journal-title":"Chem. Phys."},{"key":"2026102111092980000_cit43","doi-asserted-by":"publisher","first-page":"17047","DOI":"10.1021\/jp0580569","article-title":"Spectroscopy and Photophysics\nof Self-Organized Zinc Porphyrin Nanolayers. 3. Fluorescence Detected\nMagnetic Resonance of Triplet States","volume":"109","author":"Schaafsma","year":"2005","journal-title":"J. Phys.\nChem. B"},{"key":"2026102111092980000_cit44","doi-asserted-by":"publisher","first-page":"220","DOI":"10.1515\/znc-1983-3-411","article-title":"Optically Detected Magnetic Resonance\nof Porphyrin Complexes in the Bacterium Rhodopseudomonas sphaeroides","volume":"38c","author":"Beck","year":"1983","journal-title":"Z. Naturforsch."},{"key":"2026102111092980000_cit45","doi-asserted-by":"publisher","first-page":"7440","DOI":"10.1002\/anie.201202471","article-title":"A water-stable\nporphyrin-based metal-organic framework active for visible-light photocatalysis","volume":"51","author":"Fateeva","year":"2012","journal-title":"Angew. Chem. Int. 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