{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,22]],"date-time":"2026-10-22T08:40:43Z","timestamp":1792658443331,"version":"4.5.0"},"reference-count":66,"publisher":"American Chemical Society (ACS)","license":[{"start":{"date-parts":[[2026,10,22]],"date-time":"2026-10-22T00:00:00Z","timestamp":1792627200000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,10,22]],"date-time":"2026-10-22T00:00:00Z","timestamp":1792627200000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,10,22]],"date-time":"2026-10-22T00:00:00Z","timestamp":1792627200000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"DOI":"10.13039\/100016755","name":"International Institute for Nanotechnology, Northwestern University","doi-asserted-by":"publisher","id":[{"id":"10.13039\/100016755","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100000183","name":"Army Research Office","doi-asserted-by":"publisher","award":["W911NF-23-1-0306"],"award-info":[{"award-number":["W911NF-23-1-0306"]}],"id":[{"id":"10.13039\/100000183","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100000082","name":"Division of Graduate Education","doi-asserted-by":"publisher","award":["DGE-2234667"],"award-info":[{"award-number":["DGE-2234667"]}],"id":[{"id":"10.13039\/100000082","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Molecular electron spin qubits are an emerging platform for quantum technologies due to their atomic-scale synthetic tunability. Supramolecular structures can also place these qubits at precise positions within ordered arrays, allowing the scale-up of qubit architectures through a bottom-up approach. Here, we introduce the first three-dimensional paired-ion framework (PIF), VO-3D-PIF-1, which is composed of a concentrated array of S = 1\/2 vanadyl porphyrin spin qubits arranged by ionic lattice interactions. The PIF was characterized using electron paramagnetic resonance spectroscopy to demonstrate the impact of framework structure and spin density on spin\u2013lattice relaxation (T1) and spin decoherence (Tm). The high vanadyl porphyrin spin density within the framework (0.125 spins\/nm3) promotes dipolar-driven decoherence, with Tm = 200\u2013400 ns over a temperature range of 140\u20135 K. Spin\u2013lattice relaxation mirrors that of vanadyl porphyrins in dilute solution, suggesting that the weak ionic interactions assembling the porphyrins within the secondary coordination sphere do not adversely affect phonon-induced T1 relaxation.<\/jats:p>","DOI":"10.1021\/acs.jpclett.6c02513","type":"journal-article","created":{"date-parts":[[2026,10,22]],"date-time":"2026-10-22T01:01:38Z","timestamp":1792630898000},"source":"Crossref","is-referenced-by-count":0,"title":["Spin-Phonon\nRelaxation and Decoherence in a Three-Dimensional\nPaired-Ion Framework Composed of Vanadyl Porphyrin Qubits"],"prefix":"10.1021","author":[{"given":"Christian A.","family":"Epure","sequence":"first","affiliation":[{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0146-0610","authenticated-orcid":true,"given":"Georgia C.","family":"Mantel","sequence":"additional","affiliation":[{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]},{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]},{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8760-9991","authenticated-orcid":true,"given":"Casandra M.","family":"Moisanu","sequence":"additional","affiliation":[{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4010-8967","authenticated-orcid":true,"given":"Jonathan R.","family":"Palmer","sequence":"additional","affiliation":[{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]},{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]},{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8655-6947","authenticated-orcid":true,"given":"Madison I.","family":"Bardot","sequence":"additional","affiliation":[{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2920-5440","authenticated-orcid":true,"given":"Michael R.","family":"Wasielewski","sequence":"additional","affiliation":[{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]},{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]},{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3635-6119","authenticated-orcid":true,"given":"William R.","family":"Dichtel","sequence":"additional","affiliation":[{"name":"Northwestern University , , 2145 Sheridan Road , , ,","place":["Evanston, Illinois, United States, 60208"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,22]]},"reference":[{"key":"2026102121012977200_cit1","doi-asserted-by":"publisher","first-page":"202","DOI":"10.1016\/S0304-8853(99)00315-7","article-title":"Quantum computers and quantum coherence","volume":"200","author":"DiVincenzo","year":"1999","journal-title":"J.\nMagn. 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Lett."},{"key":"2026102121012977200_cit26","doi-asserted-by":"publisher","first-page":"28088","DOI":"10.1021\/jacs.4c07288","article-title":"A Paired-Ion Framework Composed of Vanadyl Porphyrin\nMolecular Qubits Extends Spin Coherence Times","volume":"146","author":"Moisanu","year":"2024","journal-title":"J. Am. Chem. Soc."},{"key":"2026102121012977200_cit27","doi-asserted-by":"publisher","first-page":"18447","DOI":"10.1021\/jacs.3c04786","article-title":"Crystalline Arrays of Copper Porphyrin Qubits Based\non Ion-Paired Frameworks","volume":"145","author":"Moisanu","year":"2023","journal-title":"J. Am. Chem. Soc."},{"key":"2026102121012977200_cit28","doi-asserted-by":"publisher","first-page":"709","DOI":"10.1016\/j.chempr.2022.12.010","article-title":"Dissipative crystallization\nof ion-pair receptors","volume":"9","author":"Skala","year":"2023","journal-title":"Chem."},{"key":"2026102121012977200_cit29","doi-asserted-by":"publisher","first-page":"1208","DOI":"10.1016\/j.chempr.2023.01.011","article-title":"A modular platform\nfor the precise assembly of molecular\nframeworks composed of ion pairs","volume":"9","author":"Skala","year":"2023","journal-title":"Chem."},{"key":"2026102121012977200_cit30","doi-asserted-by":"publisher","first-page":"5140","DOI":"10.1021\/ja960307r","article-title":"Calix[4]pyrroles: Old\nYet New Anion-Binding Agents","volume":"118","author":"Gale","year":"1996","journal-title":"J. Am. Chem. Soc."},{"key":"2026102121012977200_cit31","doi-asserted-by":"publisher","first-page":"2537","DOI":"10.1002\/anie.200462945","article-title":"Calix[4]pyrrole:\nAn Old yet New Ion-Pair Receptor","volume":"44","author":"Custelcean","year":"2005","journal-title":"Angew. Chem.,\nInt. Ed."},{"key":"2026102121012977200_cit32","doi-asserted-by":"publisher","first-page":"2525","DOI":"10.1021\/ar500157a","article-title":"Calix[4]pyrrole-Based\nIon Pair Receptors","volume":"47","author":"Kim","year":"2014","journal-title":"Acc. Chem. Res."},{"key":"2026102121012977200_cit33","doi-asserted-by":"publisher","first-page":"12281","DOI":"10.1021\/ja064012h","article-title":"Calix[4]pyrrole\nas a Chloride Anion Receptor: Solvent and Countercation Effects","volume":"128","author":"Sessler","year":"2006","journal-title":"J. Am. Chem. Soc."},{"key":"2026102121012977200_cit34","doi-asserted-by":"publisher","first-page":"2514","DOI":"10.1002\/chem.201103239","article-title":"Oligoether-Strapped Calix[4]pyrrole: An Ion-Pair Receptor Displaying\nCation-Dependent Chloride Anion Transport","volume":"18","author":"Park","year":"2012","journal-title":"Chem.\nA Eur. J."},{"key":"2026102121012977200_cit35","doi-asserted-by":"publisher","first-page":"2911","DOI":"10.1002\/ejoc.201100359","article-title":"Salt (LiF)\nRegulated Fluorescence Switching","volume":"2011","author":"Sokkalingam","year":"2011","journal-title":"Eur. J. Org.\nChem."},{"key":"2026102121012977200_cit36","doi-asserted-by":"publisher","first-page":"8324","DOI":"10.1021\/ja4021793","article-title":"Quantification of Nitrate\u2212\u03c0\nInteractions and Selective Transport of Nitrate Using Calix[4]pyrroles\nwith Two Aromatic Walls","volume":"135","author":"Adriaenssens","year":"2013","journal-title":"J. Am. Chem. Soc."},{"key":"2026102121012977200_cit37","doi-asserted-by":"publisher","first-page":"1089","DOI":"10.1021\/jacs.3c12277","article-title":"Oriented\nTriplet Excitons as Long-Lived Electron Spin Qutrits in a Molecular\nDonor\u2013Acceptor Single Cocrystal","volume":"146","author":"Palmer","year":"2024","journal-title":"J. Am.\nChem. Soc."},{"key":"2026102121012977200_cit38","doi-asserted-by":"publisher","first-page":"47985","DOI":"10.1021\/jacs.5c12570","article-title":"Telecom-Luminescent\nand Room Temperature Coherent Tetrathiafulvalene-Based Qubits in Spin-Rich\nSolids","volume":"147","author":"McNamara","year":"2025","journal-title":"J. Am. Chem. Soc."},{"key":"2026102121012977200_cit39","doi-asserted-by":"crossref","DOI":"10.1007\/b111467","volume-title":"Distance Measurements in Biological Systems by\nEPR","author":"Berliner","year":"2002"},{"key":"2026102121012977200_cit40","doi-asserted-by":"publisher","first-page":"14678","DOI":"10.1021\/jacs.6b08467","article-title":"Long Coherence Times\nin Nuclear Spin-Free Vanadyl Qubits","volume":"138","author":"Yu","year":"2016","journal-title":"J. Am.\nChem. Soc."},{"key":"2026102121012977200_cit41","doi-asserted-by":"publisher","first-page":"165","DOI":"10.1006\/jmre.1999.1763","article-title":"Electron Spin Lattice\nRelaxation Rates for S = 12 Molecular Species in Glassy Matrices or\nMagnetically Dilute Solids at Temperatures between 10 and 300 K","volume":"139","author":"Zhou","year":"1999","journal-title":"J. Magn. Reson."},{"key":"2026102121012977200_cit42","doi-asserted-by":"publisher","first-page":"4237","DOI":"10.1021\/acs.energyfuels.9b00867","article-title":"Vanadyl Porphyrin Speciation Based on Submegahertz Ligand Proton\nHyperfine Couplings","volume":"33","author":"Mannikko","year":"2019","journal-title":"Energy Fuels"},{"key":"2026102121012977200_cit43","doi-asserted-by":"publisher","first-page":"299","DOI":"10.1016\/j.chempr.2023.09.013","article-title":"Enhanced\ncoherence by\ncoupling spins through a delocalized \u03c0-system: Vanadyl porphyrin\ndimers","volume":"10","author":"Pozo","year":"2024","journal-title":"Chem."},{"key":"2026102121012977200_cit44","doi-asserted-by":"publisher","first-page":"AB4","DOI":"10.1103\/PhysRev.138.AB4.3","article-title":"Electron-Spin-Echo\nEnvelope Modulation","volume":"138","author":"Rowan","year":"1965","journal-title":"Phys. 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Commun."},{"key":"2026102121012977200_cit48","doi-asserted-by":"publisher","first-page":"7603","DOI":"10.1021\/acs.inorgchem.5c04870","article-title":"Enlarging\nQuantum Coherence of Vanadyl Spin Qubits in Zirconium Porphyrinic\nMOFs","volume":"65","author":"Vujevic\u0301","year":"2026","journal-title":"Inorg. Chem."},{"key":"2026102121012977200_cit49","doi-asserted-by":"publisher","first-page":"370","DOI":"10.1103\/PhysRev.168.370","article-title":"Phase Memory\nin Electron Spin Echoes, Lattice Relaxation Effects in CaWO4: Er,\nCe, Mn","volume":"168","author":"Mims","year":"1968","journal-title":"Phys. Rev."},{"key":"2026102121012977200_cit50","doi-asserted-by":"publisher","first-page":"7658","DOI":"10.1021\/acs.jpclett.3c01964","article-title":"T1 Anisotropy Elucidates\nSpin Relaxation Mechanisms in an S = 1 Cr(IV) Optically Addressable\nMolecular Qubit","volume":"14","author":"Kazmierczak","year":"2023","journal-title":"J. Phys. Chem. Lett."},{"key":"2026102121012977200_cit51","doi-asserted-by":"publisher","first-page":"2353","DOI":"10.1021\/acscentsci.4c01177","article-title":"Spectroscopic\nSignatures of Phonon\nCharacter in Molecular Electron Spin Relaxation","volume":"10","author":"Kazmierczak","year":"2024","journal-title":"ACS Cent. Sci."},{"key":"2026102121012977200_cit52","doi-asserted-by":"publisher","first-page":"14036","DOI":"10.1021\/jacs.5c00803","article-title":"Slow Electron\nSpin Relaxation at\nAmbient Temperatures with Copper Coordinated by a Rigid Macrocyclic\nLigand","volume":"147","author":"Espinosa","year":"2025","journal-title":"J. Am. Chem. Soc."},{"key":"2026102121012977200_cit53","doi-asserted-by":"publisher","first-page":"20804","DOI":"10.1021\/jacs.2c08729","article-title":"Illuminating Ligand\nField Contributions to Molecular\nQubit Spin Relaxation via T1 Anisotropy","volume":"144","author":"Kazmierczak","year":"2022","journal-title":"J.\nAm. Chem. Soc."},{"key":"2026102121012977200_cit54","doi-asserted-by":"publisher","first-page":"67","DOI":"10.1006\/jmra.1995.9971","article-title":"Temperature and Orientation Dependence\nof Electron-Spin Relaxation Rates for Bis(diethyldithiocarbamato)copper(II)","volume":"117","author":"Du","year":"1995","journal-title":"Journal of Magnetic Resonance, Series A"},{"key":"2026102121012977200_cit55","doi-asserted-by":"publisher","first-page":"13815","DOI":"10.1021\/jacs.5c01962","article-title":"Anisotropy of Spin\u2013Lattice\nRelaxation Time (T1)\nfor Oxo-Vanadium(IV) and Nitrido Chromium(V) Porphyrins","volume":"147","author":"Eaton","year":"2025","journal-title":"J. Am. Chem. Soc."},{"key":"2026102121012977200_cit56","doi-asserted-by":"publisher","first-page":"17305","DOI":"10.1021\/jacs.1c04605","article-title":"The Impact of Ligand Field Symmetry\non Molecular Qubit Coherence","volume":"143","author":"Kazmierczak","year":"2021","journal-title":"J. Am. Chem. 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