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Elucidation of the mechanism of the reaction of NO with DNA regulatory proteins that contain Fe\u2010S clusters has been hampered by a lack of information about the nature of the iron\u2010nitrosyl products formed. Herein, we report nuclear resonance vibrational spectroscopy (NRVS) and density functional theory (DFT) calculations that identify NO reaction products in WhiD and NsrR, regulatory proteins that use a [4Fe\u20104S] cluster to sense NO. This work reveals that nitrosylation yields multiple products structurally related to Roussin's Red Ester (RRE, [Fe<jats:sub>2<\/jats:sub>(NO)<jats:sub>4<\/jats:sub>(Cys)<jats:sub>2<\/jats:sub>]) and Roussin's Black Salt (RBS, [Fe<jats:sub>4<\/jats:sub>(NO)<jats:sub>7<\/jats:sub>S<jats:sub>3<\/jats:sub>]. In the latter case, the absence of <jats:sup>32<\/jats:sup>S\/<jats:sup>34<\/jats:sup>S shifts in the Fe\u2212S region of the NRVS spectra suggest that a new species, Roussin's Black Ester (RBE), may be formed, in which one or more of the sulfide ligands is replaced by Cys thiolates.<\/jats:p>","DOI":"10.1002\/anie.201607033","type":"journal-article","created":{"date-parts":[[2016,10,25]],"date-time":"2016-10-25T07:32:47Z","timestamp":1477380767000},"page":"14575-14579","source":"Crossref","is-referenced-by-count":42,"title":["Nitrosylation of Nitric\u2010Oxide\u2010Sensing Regulatory Proteins Containing [4Fe\u20104S] Clusters Gives Rise to Multiple Iron\u2013Nitrosyl Complexes"],"prefix":"10.1002","volume":"55","author":[{"given":"Pauline N.","family":"Serrano","sequence":"first","affiliation":[{"name":"Department of Chemistry University of California  Davis CA 95616 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hongxin","family":"Wang","sequence":"additional","affiliation":[{"name":"Department of Chemistry University of California  Davis CA 95616 USA"},{"name":"Physical Biosciences Division Lawrence Berkeley National Laboratory  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jason C.","family":"Crack","sequence":"additional","affiliation":[{"name":"Centre for Molecular and Structural Biochemistry School of Chemistry University of East Anglia  Norwich Research Park Norwich NR4 7TJ UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Christopher","family":"Prior","sequence":"additional","affiliation":[{"name":"Centre for Molecular and Structural Biochemistry School of Chemistry University of East Anglia  Norwich Research Park Norwich NR4 7TJ UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Matthew I.","family":"Hutchings","sequence":"additional","affiliation":[{"name":"School of Biological Sciences University of East Anglia  Norwich NR4 7TJ UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Andrew J.","family":"Thomson","sequence":"additional","affiliation":[{"name":"Centre for Molecular and Structural Biochemistry School of Chemistry University of East Anglia  Norwich Research Park Norwich NR4 7TJ UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Saeed","family":"Kamali","sequence":"additional","affiliation":[{"name":"University of Tennessee Space Institute  Tullahome TN 37388-9700 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yoshitaka","family":"Yoda","sequence":"additional","affiliation":[{"name":"Research and Utilization Division SPring-8\/JASRI  1-1-1 Kouto, Sayo Hyogo 679-5198 Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiyong","family":"Zhao","sequence":"additional","affiliation":[{"name":"Advanced Photon Source Argonne National Laboratory  Argonne IL 60439 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Michael Y.","family":"Hu","sequence":"additional","affiliation":[{"name":"Advanced Photon Source Argonne National Laboratory  Argonne IL 60439 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ercan E.","family":"Alp","sequence":"additional","affiliation":[{"name":"Advanced Photon Source Argonne National Laboratory  Argonne IL 60439 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Vasily S.","family":"Oganesyan","sequence":"additional","affiliation":[{"name":"Centre for Molecular and Structural Biochemistry School of Chemistry University of East Anglia  Norwich Research Park Norwich NR4 7TJ UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nick E.","family":"Le\u2005Brun","sequence":"additional","affiliation":[{"name":"Centre for Molecular and Structural Biochemistry School of Chemistry University of East Anglia  Norwich Research Park Norwich NR4 7TJ UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Stephen P.","family":"Cramer","sequence":"additional","affiliation":[{"name":"Department of Chemistry University of California  Davis CA 95616 USA"},{"name":"Physical Biosciences Division Lawrence Berkeley National Laboratory  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2016,10,25]]},"reference":[{"key":"e_1_2_2_1_1","doi-asserted-by":"publisher","DOI":"10.1146\/annurev.biochem.74.082803.133518"},{"key":"e_1_2_2_2_1","unstructured":"\u00a0"},{"key":"e_1_2_2_3_2","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.97.10.5146"},{"key":"e_1_2_2_4_2","doi-asserted-by":"publisher","DOI":"10.1006\/meth.1996.0426"},{"key":"e_1_2_2_5_2","doi-asserted-by":"publisher","DOI":"10.1021\/ar5002507"},{"key":"e_1_2_2_6_1","unstructured":"\u00a0"},{"key":"e_1_2_2_7_2","doi-asserted-by":"publisher","DOI":"10.1021\/cr020623q"},{"key":"e_1_2_2_8_2","volume-title":"Nitric Oxide: Biology and Pathobiology","author":"Ignarro L. 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