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Ultrasmall iron oxide nanoparticles (USIOs)-based CAs have emerged as promising alternatives, offering adjustable MRI T1 relaxivity, favorable pharmacokinetics, and high biocompatibility; however, their performance is critically hampered by inefficient atomic utilization for MR T1 relaxivity enhancement. Herein, we report Mg-doped USIOs MRI CAs with high atomic utilization efficiency, where incorporating a biocompatible Mg dopant into surface octahedral-site Fe vacancies substantially boosts the T1 relaxivity, enabling accurate detection of SSPE-associated structural and perfusion abnormalities. The Mg0.03-USIOs exhibit a 261-fold enhancement of T1 relaxivity contribution by the Mg dopant, achieving an exceptionally high T1 relaxivity of 12.6 mM\u22121 s\u22121. Such a high atomic utilization efficiency could stem from the promoted spin polarization and ferromagnetic spin alignment through the surface Mg doping, which considerably boosts the magnetic moment and outer-sphere relaxation contribution. Further in vivo MRI studies in a pig SSPE model demonstrated that the Mg0.03-USIOs enabled visualization of structural and perfusion abnormalities in SSPE, far surpassing the capabilities of Gd-based CAs. In vivo biosafety assessment in the pig model confirmed the high biocompatibility of Mg0.03-USIOs. Our findings provide a highly efficient doping strategy to construct high-performance USIOs-based T1 CAs for sensitive MRI of microvascular structural and functional abnormalities.<\/jats:p>","DOI":"10.1021\/acsnano.6c09779","type":"journal-article","created":{"date-parts":[[2026,8,19]],"date-time":"2026-08-19T06:02:06Z","timestamp":1787119326000},"page":"24040-24056","source":"Crossref","is-referenced-by-count":0,"title":["Trace Mg-Doped Ultrasmall\nIron Oxide Nanoparticles\nwith Boosted\n                    <i>T<\/i>\n                    1 Relaxivity for Highly\nSensitive MRI of Subsegmental Pulmonary Embolism"],"prefix":"10.1021","volume":"20","author":[{"given":"Huan","family":"Zhang","sequence":"first","affiliation":[{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Minrui","family":"Liu","sequence":"additional","affiliation":[{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhongqin","family":"Zhou","sequence":"additional","affiliation":[{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pengfei","family":"Ye","sequence":"additional","affiliation":[{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lingyi","family":"Wen","sequence":"additional","affiliation":[{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Quanqing","family":"Feng","sequence":"additional","affiliation":[{"name":"Northwest University , , , ,","place":["Xi\u2019an, Shaanxi, China, 710127"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0114-1759","authenticated-orcid":true,"given":"Ningning","family":"Song","sequence":"additional","affiliation":[{"name":"Beijing University of Chemical Technology , , ,","place":["Beijing, China, 100029"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanyun","family":"Wang","sequence":"additional","affiliation":[{"name":"Northwest University , , , ,","place":["Xi\u2019an, Shaanxi, China, 710127"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guohang","family":"Ma","sequence":"additional","affiliation":[{"name":"Northwest University , , , ,","place":["Xi\u2019an, Shaanxi, China, 710127"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ran","family":"Sun","sequence":"additional","affiliation":[{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kun","family":"Zhang","sequence":"additional","affiliation":[{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qihong","family":"Wu","sequence":"additional","affiliation":[{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Meng","family":"Zhang","sequence":"additional","affiliation":[{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yining","family":"Wang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Medical Sciences and Peking Union Medical College , , ,","place":["Beijing, China, 100730"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yingkun","family":"Guo","sequence":"additional","affiliation":[{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0091-772X","authenticated-orcid":true,"given":"Haiming","family":"Fan","sequence":"additional","affiliation":[{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Sichuan University , , , ,","place":["Chengdu, Sichuan, China, 610041"]},{"name":"Northwest University , , , ,","place":["Xi\u2019an, Shaanxi, China, 710127"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,19]]},"reference":[{"key":"2026090306593562600_cit1","doi-asserted-by":"publisher","first-page":"30","DOI":"10.5320\/wjr.v9.i3.30","article-title":"Diagnosis and Treatment\nof Subsegmental Pulmonary Embolism","volume":"9","author":"Newnham","year":"2019","journal-title":"World J.\nRespirol."},{"key":"2026090306593562600_cit2","doi-asserted-by":"publisher","first-page":"248","DOI":"10.1038\/s41569-022-00787-6","article-title":"Epidemiology and Prevention of Venous 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Diagn.\nTher."},{"key":"2026090306593562600_cit6","doi-asserted-by":"publisher","first-page":"784","DOI":"10.1002\/jmri.28912","article-title":"International Workshop for Pulmonary\nFunctional, I.,\nMagnetic Resonance Imaging of Lung Perfusion","volume":"59","author":"Triphan","year":"2024","journal-title":"J. Magn. Reson. Imaging."},{"key":"2026090306593562600_cit7","doi-asserted-by":"publisher","first-page":"957","DOI":"10.1021\/acs.chemrev.8b00363","article-title":"Chemistry of MRI Contrast\nAgents: Current Challenges and New Frontiers","volume":"119","author":"Wahsner","year":"2019","journal-title":"Chem. Rev."},{"key":"2026090306593562600_cit8","doi-asserted-by":"publisher","first-page":"117668","DOI":"10.1016\/j.ejmech.2025.117668","article-title":"Molecular and Supramolecular\nRoutes to Enhance Gadolinium-Based Contrast Agents Relaxivity: How\nFar Are We From the Theoretical Optimal Value?","volume":"292","author":"Palagi","year":"2025","journal-title":"Eur. J. Med. Chem."},{"key":"2026090306593562600_cit9","doi-asserted-by":"publisher","first-page":"1104","DOI":"10.1093\/ndt\/gfk062","article-title":"Gadolinium\u2212a\nSpecific Trigger for the Development of Nephrogenic Fbrosing Dermopathy\nand Nephrogenic Systemic Fibrosis?","volume":"21","author":"Grobner","year":"2006","journal-title":"Nephrol.\nDial. Trans."},{"key":"2026090306593562600_cit10","doi-asserted-by":"publisher","first-page":"2359","DOI":"10.1681\/ASN.2006060601","article-title":"Nephrogenic Systemic Fibrosis: Suspected\nCausative Role of Gadodiamide Used for Contrast-Enhanced Magnetic\nResonance Imaging","volume":"17","author":"Marckmann","year":"2006","journal-title":"J. Am. Soc. Nephrol."},{"key":"2026090306593562600_cit11","doi-asserted-by":"publisher","first-page":"1906539","DOI":"10.1002\/adma.201906539","article-title":"Iron Oxide Nanoparticles\nas T1 Contrast Agents for Magnetic Resonance Imaging: Fundamentals,\nChallenges, Applications, and Prospectives","volume":"33","author":"Jeon","year":"2021","journal-title":"Adv. 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Eng."},{"key":"2026090306593562600_cit15","doi-asserted-by":"publisher","first-page":"17014","DOI":"10.1038\/natrevmats.2017.14","article-title":"Towards\nClinically Translatable in Vivo Nanodiagnostics","volume":"2","author":"Park","year":"2017","journal-title":"Nat. Rev. Mater."},{"key":"2026090306593562600_cit16","doi-asserted-by":"publisher","first-page":"10992","DOI":"10.1021\/acsnano.7b04924","article-title":"Multifunctional Theranostic\nNanoparticles\nBased on Exceedingly Small Magnetic Iron Oxide Nanoparticles for T1-Weighted Magnetic Resonance Imaging and Chemotherapy","volume":"11","author":"Shen","year":"2017","journal-title":"ACS Nano"},{"key":"2026090306593562600_cit17","doi-asserted-by":"publisher","first-page":"637","DOI":"10.1038\/s41551-017-0116-7","article-title":"Iron Oxide Nanoclusters for T1 Magnetic Resonance Imaging of Non-Human Primates","volume":"1","author":"Lu","year":"2017","journal-title":"Nat. Biomed. 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Am. Chem. Soc."},{"key":"2026090306593562600_cit31","doi-asserted-by":"publisher","first-page":"3795","DOI":"10.1021\/jp411481p","article-title":"Magnetic Iron\nOxide Nanoparticles: Reproducible Tuning of the Size and Nanosized-Dependent\nComposition, Defects, and Spin Canting","volume":"118","author":"Baaziz","year":"2014","journal-title":"J. Phys.\nChem. C"},{"key":"2026090306593562600_cit32","doi-asserted-by":"publisher","first-page":"2401133","DOI":"10.1002\/adma.202401133","article-title":"Synergizing Fe2O3 Nanoparticles on Single Atom\nFe-N-C for Nitrate Reduction to Ammonia at Industrial Current Densities","volume":"36","author":"Murphy","year":"2024","journal-title":"Adv. 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