Structural Evolution of Photoexcited Methylcobalamin Towards a CarH-like Metastable State: Evidence from Time-Resolved X-ray Absorption and X-ray Emission
dc.contributor.author | Sension, Roseanne J | |
dc.contributor.author | McClain, Taylor P. | |
dc.contributor.author | Michocki, Lindsay B. | |
dc.contributor.author | Miller, Nicholas A. | |
dc.contributor.author | Alonso-Mori, Roberto | |
dc.contributor.author | Lima, Frederico Alves | |
dc.contributor.author | Ardana-Lamas, Fernando | |
dc.contributor.author | Biednov, Mykola | |
dc.contributor.author | Chung, Taewon | |
dc.contributor.author | Deb, Aniruddha | |
dc.contributor.author | Jiang, Yifeng | |
dc.contributor.author | Kaneshiro, April K. | |
dc.contributor.author | Khakhu, Dmitry | |
dc.contributor.author | Kubarych, Kevin J. | |
dc.contributor.author | Lamb, Ryan M. | |
dc.contributor.author | Meadows, Joseph H. | |
dc.contributor.author | Otte, Florian | |
dc.contributor.author | Sofferman, Danielle L. | |
dc.contributor.author | Song, Sanghoon | |
dc.contributor.author | Uemura, Yohei | |
dc.contributor.author | van Driel, Tim B. | |
dc.contributor.author | Penner-Hah, James E. | |
dc.date.accessioned | 2024-08-26T15:13:46Z | |
dc.date.available | 2024-08-26T15:13:46Z | |
dc.date.issued | 2024-07-24 | |
dc.identifier.citation | Journal of Physical Chemistry B https://pubs.acs.org/doi/10.1021/acs.jpcb.4c03729 | en_US |
dc.identifier.uri | https://hdl.handle.net/2027.42/194115 | en |
dc.description | Data associated with this manuscript can be found at https://doi.org/10.7302/9ycc-t185 | en_US |
dc.description.abstract | CarH is a protein photoreceptor that uses a form of B12, adenosylcobalamin (AdoCbl), to sense light via formation of a metastable excited state. Aside from AdoCbl bound to CarH, methylcobalamin (MeCbl) is the only other example – to date – of photoexcited cobalamins forming metastable excited states with lifetimes of nanoseconds or longer. The UV-visible spectra of the excited states of MeCbl and AdoCbl bound to CarH are similar. We have used transient Co K-edge X-ray absorption and X-ray emission spectroscopies in conjunction with transient absorption spectroscopy in the UV−visible region to characterize the excited states of MeCbl. These data show that the metastable excited state of MeCbl has a slightly expanded corrin ring and increased electron density on the cobalt, but only small changes in the axial bond lengths. This is similar to changes seen previously for CarH, suggesting that MeCbl may be a good model for AdoCbl in CarH. | en_US |
dc.description.sponsorship | National Science Foundation NSF-CHE 1836435, NSF-CHE 2154157 NIH grant P41GM139687 U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences Contract No. DE-AC02-76SF00515 | en_US |
dc.language.iso | en_US | en_US |
dc.publisher | American Chemical Society | en_US |
dc.rights | Attribution-NonCommercial-ShareAlike 4.0 International | * |
dc.rights.uri | http://creativecommons.org/licenses/by-nc-sa/4.0/ | * |
dc.subject | Ultrafast | en_US |
dc.subject | X-ray | en_US |
dc.subject | Transient absorption | en_US |
dc.subject | cobalamin | en_US |
dc.subject | vitamin B12 | en_US |
dc.subject | XAS | en_US |
dc.subject | XANES | en_US |
dc.subject | XES | en_US |
dc.title | Structural Evolution of Photoexcited Methylcobalamin Towards a CarH-like Metastable State: Evidence from Time-Resolved X-ray Absorption and X-ray Emission | en_US |
dc.type | Article | en_US |
dc.subject.hlbsecondlevel | Chemistry | |
dc.subject.hlbtoplevel | Science | |
dc.description.peerreviewed | Peer Reviewed | en_US |
dc.contributor.affiliationum | Department of Chemistry | en_US |
dc.contributor.affiliationum | Department of Physics | en_US |
dc.contributor.affiliationum | Department of Biophysics | en_US |
dc.contributor.affiliationum | Department of Biological Chemistry | en_US |
dc.contributor.affiliationum | Program in Applied Physics | en_US |
dc.contributor.affiliationother | Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, U.S.A | en_US |
dc.contributor.affiliationother | Femtosecond X-ray Experiments Group, European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany | en_US |
dc.contributor.affiliationumcampus | Ann Arbor | en_US |
dc.description.bitstreamurl | http://deepblue.lib.umich.edu/bitstream/2027.42/194115/1/jpcb.4c03729 as accepted.pdf | |
dc.identifier.doi | https://dx.doi.org/10.7302/23559 | |
dc.identifier.source | Journal of Physical Chemistry B | en_US |
dc.identifier.orcid | 0000-0002-5357-0934;0000-0001-9028-5051;0000-0003-2219-155X;0000-0002-9629-890X;0000-0002-0331-9709;0000-0002-4884-171X;0000-0003-0685-0498;0000-0002-7560-9895;0000-0003-1152-4734;0000-0001-6458-3653;0000-0001-8106-2892;0009-0009-3077-0966;0000-0002-0154-9906; 0000-0002-9146-5414;0000-0002-2431-4464;0000-0003-0314-1274;0000-0001-7155-2011;0000-0001-6758-0132;0000-0001-7386-4019;0000-0003-3164-7168;0000-0003-4070-3168 | en_US |
dc.description.filedescription | Description of jpcb.4c03729 as accepted.pdf : This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry B, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/articlesonrequest/AOR-NUFZPAJFUTPSIMBX494N | |
dc.description.depositor | SELF | en_US |
dc.working.doi | 10.7302/23559 | en_US |
dc.owningcollname | Chemistry, Department of |
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