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DOI	10.1073/pnas.2018966118
	Interplays of electron and nuclear motions along co dissociation trajectory in myoglobin revealed by ultrafast x-rays and quantum dynamics calculations
	Shelby M.L.; Wildman A.; Hayes D.; Mara M.W.; Lestrange P.J.; Cammarata M.; Balducci L.; Artamonov M.; Lemke H.T.; Zhu D.; Seideman T.; Hoffman B.M.; Li X.; Chen L.X.
发表日期	2021
ISSN	00278424
卷号	118 期号:14
英文摘要	Ultrafast structural dynamics with different spatial and temporal scales were investigated during photodissociation of carbon monoxide (CO) from iron(II)-heme in bovine myoglobin during the first 3 ps following laser excitation. We used simultaneous X-ray transient absorption (XTA) spectroscopy and X-ray transient solution scattering (XSS) at an X-ray free electron laser source with a time resolution of 80 fs. Kinetic traces at different characteristic X-ray energies were collected to give a global picture of the multistep pathway in the photodissociation of CO from heme. In order to extract the reaction coordinates along different directions of the CO departure, XTA data were collected with parallel and perpendicular relative polarizations of the laser pump and X-ray probe pulse to isolate the contributions of electronic spin state transition, bond breaking, and heme macrocycle nuclear relaxation. The time evolution of the iron K-edge X-ray absorption near edge structure (XANES) features along the two major photochemical reaction coordinates, i.e., the iron(II)-CO bond elongation and the heme macrocycle doming relaxation were modeled by time-dependent density functional theory calculations. Combined results from the experiments and computations reveal insight into interplays between the nuclear and electronic structural dynamics along the CO photodissociation trajectory. Time-resolved small-angle X-ray scattering data during the same process are also simultaneously collected, which show that the local CO dissociation causes a protein quake propagating on different spatial and temporal scales. These studies are important for understanding gas transport and protein deligation processes and shed light on the interplay of active site conformational changes and large-scale protein reorganization. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	Myoglobin; Protein structural dynamics; Quantum dynamics calculation; Time-resolved solution X-ray scattering; X-ray transient absorption
语种	英语
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/179969
作者单位	Department of Chemistry, Northwestern University, Evanston, IL 60208, United States; Department of Chemistry, University of Washington, Seattle, WA 98195, United States; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL 60437, United States; Institut de Physique de Rennes, Université de Rennes, Rennes CEDEX, 35042, France; Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, United States
推荐引用方式 GB/T 7714	Shelby M.L.,Wildman A.,Hayes D.,et al. Interplays of electron and nuclear motions along co dissociation trajectory in myoglobin revealed by ultrafast x-rays and quantum dynamics calculations[J],2021,118(14).
APA	Shelby M.L..,Wildman A..,Hayes D..,Mara M.W..,Lestrange P.J..,...&Chen L.X..(2021).Interplays of electron and nuclear motions along co dissociation trajectory in myoglobin revealed by ultrafast x-rays and quantum dynamics calculations.Proceedings of the National Academy of Sciences of the United States of America,118(14).
MLA	Shelby M.L.,et al."Interplays of electron and nuclear motions along co dissociation trajectory in myoglobin revealed by ultrafast x-rays and quantum dynamics calculations".Proceedings of the National Academy of Sciences of the United States of America 118.14(2021).