Real-time tracking of CO migration and binding in the ? and ? subunits of human hemoglobin via 150-ps time-resolved Laue crystallography

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dc.citation.firstpage98en_US
dc.citation.journalTitleChemical Physicsen_US
dc.citation.lastpage106en_US
dc.citation.volumeNumber422en_US
dc.contributor.authorSchotte, Friedrichen_US
dc.contributor.authorCho, Hyun Sunen_US
dc.contributor.authorSoman, Jayashreeen_US
dc.contributor.authorWulff, Michaelen_US
dc.contributor.authorOlson, John S.en_US
dc.contributor.authorAnfinrud, Philip A.en_US
dc.contributor.orgW.M. Keck Center for Computational Biologyen_US
dc.date.accessioned2014-10-08T21:25:35Zen_US
dc.date.available2014-10-08T21:25:35Zen_US
dc.date.issued2013en_US
dc.description.abstractWe have developed the method of picosecond Laue crystallography and used this capability to probe ligand dynamics in tetrameric R-state hemoglobin (Hb). Time-resolved, 2 Å-resolution electron density maps of photolyzed HbCO reveal the time-dependent population of CO in the binding (A) and primary docking (B) sites of both α and β subunits from 100 ps to 10 μs. The proximity of the B site in the β subunit is about 0.25 Å closer to its A binding site, and its kBA rebinding rate (∼300 μs−1) is six times faster, suggesting distal control of the rebinding dynamics. Geminate rebinding in the β subunit exhibits both prompt and delayed geminate phases. We developed a microscopic model to quantitatively explain the observed kinetics, with three states for the α subunit and four states for the β subunit. This model provides a consistent framework for interpreting rebinding kinetics reported in prior studies of both HbCO and HbO2.en_US
dc.identifier.citationSchotte, Friedrich, Cho, Hyun Sun, Soman, Jayashree, et al.. "Real-time tracking of CO migration and binding in the ? and ? subunits of human hemoglobin via 150-ps time-resolved Laue crystallography." <i>Chemical Physics,</i> 422, (2013) Elsevier: 98-106. http://dx.doi.org/10.1016/j.chemphys.2012.12.030.en_US
dc.identifier.doihttp://dx.doi.org/10.1016/j.chemphys.2012.12.030en_US
dc.identifier.urihttps://hdl.handle.net/1911/77453en_US
dc.language.isoengen_US
dc.publisherElsevieren_US
dc.rightsThis is an author's peer-reviewed final manuscript, as accepted by the publisher. The published article is copyrighted by Elsevier.en_US
dc.subject.keywordhemoglobinen_US
dc.subject.keywordgeminate rebindingen_US
dc.subject.keywordligand migrationen_US
dc.subject.keywordtime-resolved Laue crystallographyen_US
dc.titleReal-time tracking of CO migration and binding in the ? and ? subunits of human hemoglobin via 150-ps time-resolved Laue crystallographyen_US
dc.typeJournal articleen_US
dc.type.dcmiTexten_US
dc.type.publicationpost-printen_US
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