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Nanostructured materials with high nitroxide densities, where each individual nitroxide within a macromolecular construct contributes to the image contrast, could address this limitation, but the synthesis of such materials remains challenging. Here, we report a modular and scalable synthetic approach to nitroxide-based brush-arm star polymer (BASP) organic radical CAs (ORCAs) with high nitroxide loadings. The optimized \u223c30 nm diameter \u201cBASP-ORCA3\u201d displays outstanding T2 sensitivity with a very high molecular transverse relaxivity (r2 &amp;gt; 1000 mM\u20131 s\u20131). BASP-ORCA3 further exhibits excellent stability in vivo, no acute toxicity, and highly desirable pharmacokinetic and biodistribution profiles for longitudinal detection of tumors by MRI. When injected intravenously into mice bearing subcutaneous plasmacytomas, BASP-ORCA3 affords distinct in vivo visualization of tumors on translationally relevant time scales. Leveraging its high sensitivity, BASP-ORCA3 enables efficient mapping of tumor necrosis, which is an important biomarker to predict therapeutic outcomes. Moreover, BASP-ORCA3 allows for detection of millimetric tumor implants in a disseminated murine model of advanced-stage human ovarian cancer that possess genetic, histological, and vascular characteristics that are similar to those seen in patients. This work establishes BASP-ORCA3 as a promising metal-free spin contrast agent for MRI.<\/jats:p>","DOI":"10.1021\/acsnano.8b06160","type":"journal-article","created":{"date-parts":[[2018,11,2]],"date-time":"2018-11-02T15:31:16Z","timestamp":1541172676000},"page":"11343-11354","source":"Crossref","is-referenced-by-count":79,"title":["Triply\nLoaded Nitroxide Brush-Arm Star Polymers Enable\nMetal-Free Millimetric Tumor Detection by Magnetic Resonance Imaging"],"prefix":"10.1021","volume":"12","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-6945-4057","authenticated-orcid":true,"given":"Hung V.-T.","family":"Nguyen","sequence":"first","affiliation":[{"name":"Massachusetts Institute of Technology , , 77 Massachusetts Avenue , , ,","place":["Cambridge, Massachusetts, United States, 02139"]},{"name":"Dana-Farber Cancer Institute , , 450 Brookline Avenue , , ,","place":["Boston, Massachusetts, United States, 02215"]},{"name":"Harvard Medical School , 25 Shattuck Street , , 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02139"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hui","family":"Zhang","sequence":"additional","affiliation":[{"name":"University of Nebraska , , , ,","place":["Lincoln, Nebraska, United States, 68588"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peter","family":"Harvey","sequence":"additional","affiliation":[{"name":"Massachusetts Institute of Technology , , 77 Massachusetts Avenue , , ,","place":["Cambridge, Massachusetts, United States, 02139"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Changcun","family":"Yan","sequence":"additional","affiliation":[{"name":"University of Nebraska , , , ,","place":["Lincoln, Nebraska, United States, 68588"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Clelia","family":"Mathieu","sequence":"additional","affiliation":[{"name":"Dana-Farber Cancer Institute , , 450 Brookline Avenue , , ,","place":["Boston, Massachusetts, United States, 02215"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5848-7366","authenticated-orcid":true,"given":"Matthew R.","family":"Golder","sequence":"additional","affiliation":[{"name":"Massachusetts Institute of Technology , , 77 Massachusetts Avenue , , ,","place":["Cambridge, Massachusetts, United States, 02139"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yivan","family":"Jiang","sequence":"additional","affiliation":[{"name":"Massachusetts Institute of Technology , , 77 Massachusetts Avenue , , ,","place":["Cambridge, Massachusetts, United States, 02139"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4681-4718","authenticated-orcid":true,"given":"Maria Francesca","family":"Ottaviani","sequence":"additional","affiliation":[{"name":"University of Urbino , , ,","place":["Urbino, Italy, 61029"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Alan","family":"Jasanoff","sequence":"additional","affiliation":[{"name":"Massachusetts Institute of Technology , , 77 Massachusetts Avenue , , ,","place":["Cambridge, Massachusetts, United States, 02139"]},{"name":"Massachusetts Institute of Technology , , 77 Massachusetts Avenue , , ,","place":["Cambridge, Massachusetts, United States, 02139"]},{"name":"Massachusetts Institute of Technology , , 77 Massachusetts Avenue , , ,","place":["Cambridge, Massachusetts, United States, 02139"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8856-1536","authenticated-orcid":true,"given":"Andrzej","family":"Rajca","sequence":"additional","affiliation":[{"name":"University of Nebraska , , , ,","place":["Lincoln, Nebraska, United States, 68588"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Irene","family":"Ghobrial","sequence":"additional","affiliation":[{"name":"Dana-Farber Cancer Institute , , 450 Brookline Avenue , , ,","place":["Boston, Massachusetts, United States, 02215"]},{"name":"Harvard Medical School , 25 Shattuck Street , , ,","place":["Boston, Massachusetts, United States, 02115"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2564-1950","authenticated-orcid":true,"given":"P. 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Surg."},{"key":"2026081801133544300_cit20","doi-asserted-by":"publisher","first-page":"173","DOI":"10.1007\/s00247-013-2795-x","article-title":"Pediatric Nephrogenic Systemic Fibrosis\nis Rarely Reported: a RADAR Report","volume":"44","author":"Nardone","year":"2014","journal-title":"Pediatr.\nRadiol."},{"key":"2026081801133544300_cit21","doi-asserted-by":"publisher","first-page":"13400","DOI":"10.3748\/wjg.v21.i47.13400","article-title":"Current\nStatus of Superparamagnetic Iron Oxide Contrast Agents for Liver Magnetic\nResonance Imaging","volume":"21","author":"Wang","year":"2015","journal-title":"World J. Gastroenterol."},{"key":"2026081801133544300_cit22","doi-asserted-by":"publisher","first-page":"461","DOI":"10.2215\/CJN.06011108","article-title":"Current\nStatus of Gadolinium Toxicity in Patients with Kidney Disease","volume":"4","author":"Perazella","year":"2009","journal-title":"Clin. J. Am. Soc. 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Pharmacol."},{"key":"2026081801133544300_cit42","doi-asserted-by":"publisher","first-page":"9921","DOI":"10.1158\/0008-5472.CAN-06-0879","article-title":"Probing\nthe Intracellular Redox Status of Tumors with Magnetic Resonance Imaging\nand Redox-Sensitive Contrast Agents","volume":"66","author":"Hyodo","year":"2006","journal-title":"Cancer\nRes."},{"key":"2026081801133544300_cit43","doi-asserted-by":"publisher","first-page":"504","DOI":"10.1021\/mp800175k","article-title":"Nitroxyl Radicals for\nLabeling of Conventional Therapeutics and Noninvasive Magnetic Resonance\nImaging of Their Permeability for Blood\u2013Brain Barrier: Relationship\nbetween Structure, Blood Clearance, and MRI Signal Dynamic in the\nBrain","volume":"6","author":"Zhelev","year":"2009","journal-title":"Mol. 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