title: Direct observation of ultrafast collective motions in CO myoglobin upon ligand dissociation.
abstract: The hemoprotein myoglobin is a model system for the study of protein dynamics. We used time-resolved serial femtosecond crystallography at an x-ray free-electron laser to resolve the ultrafast structural changes in the carbonmonoxy myoglobin complex upon photolysis of the Fe-CO bond. Structural changes appear throughout the protein within 500 femtoseconds, with the C, F, and H helices moving away from the heme cofactor and the E and A helices moving toward it. These collective movements are predicted by hybrid quantum mechanics/molecular mechanics simulations. Together with the observed oscillations of residues contacting the heme, our calculations support the prediction that an immediate collective response of the protein occurs upon ligand dissociation, as a result of heme vibrational modes coupling to global modes of the protein.
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany. thomas.barends@mpimf-heidelberg.mpg.de ilme.schlichting@mpimf-heidelberg.mpg.de.
authors.forename: Thomas R M
authors.initials: TR
authors.lastname: Barends
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany.
authors.forename: Lutz
authors.initials: L
authors.lastname: Foucar
authors.affiliation: Max-Planck-Institut für Biophysik, Max-von-Laue-Straße 3, 60438 Frankfurt am Main, Germany.
authors.forename: Albert
authors.initials: A
authors.lastname: Ardevol
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany.
authors.forename: Karol
authors.initials: K
authors.lastname: Nass
authors.affiliation: European XFEL GmbH, Albert-Einstein-Ring 19, 22761 Hamburg, Germany.
authors.forename: Andrew
authors.initials: A
authors.lastname: Aquila
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany.
authors.forename: Sabine
authors.initials: S
authors.lastname: Botha
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany.
authors.forename: R Bruce
authors.initials: RB
authors.lastname: Doak
authors.affiliation: Institut für Physikalische und Theoretische Chemie, Goethe-Universität, Max-von-Laue-Straße 7, 60438 Frankfurt am Main, Germany.
authors.forename: Konstantin
authors.initials: K
authors.lastname: Falahati
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany.
authors.forename: Elisabeth
authors.initials: E
authors.lastname: Hartmann
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany.
authors.forename: Mario
authors.initials: M
authors.lastname: Hilpert
authors.affiliation: Max-Planck-Institut für Biophysik, Max-von-Laue-Straße 3, 60438 Frankfurt am Main, Germany. Institut für Physikalische und Theoretische Chemie, Goethe-Universität, Max-von-Laue-Straße 7, 60438 Frankfurt am Main, Germany.
authors.forename: Marcel
authors.initials: M
authors.lastname: Heinz
authors.affiliation: Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.
authors.forename: Matthias C
authors.initials: MC
authors.lastname: Hoffmann
authors.affiliation: Max-Planck-Institut für Biophysik, Max-von-Laue-Straße 3, 60438 Frankfurt am Main, Germany.
authors.forename: Jürgen
authors.initials: J
authors.lastname: Köfinger
authors.affiliation: Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.
authors.forename: Jason E
authors.initials: JE
authors.lastname: Koglin
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany.
authors.forename: Gabriela
authors.initials: G
authors.lastname: Kovacsova
authors.affiliation: Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.
authors.forename: Mengning
authors.initials: M
authors.lastname: Liang
authors.affiliation: Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.
authors.forename: Despina
authors.initials: D
authors.lastname: Milathianaki
authors.affiliation: Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.
authors.forename: Henrik T
authors.initials: HT
authors.lastname: Lemke
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany.
authors.forename: Jochen
authors.initials: J
authors.lastname: Reinstein
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany.
authors.forename: Christopher M
authors.initials: CM
authors.lastname: Roome
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany.
authors.forename: Robert L
authors.initials: RL
authors.lastname: Shoeman
authors.affiliation: Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.
authors.forename: Garth J
authors.initials: GJ
authors.lastname: Williams
authors.affiliation: Institut für Physikalische und Theoretische Chemie, Goethe-Universität, Max-von-Laue-Straße 7, 60438 Frankfurt am Main, Germany.
authors.forename: Irene
authors.initials: I
authors.lastname: Burghardt
authors.affiliation: Max-Planck-Institut für Biophysik, Max-von-Laue-Straße 3, 60438 Frankfurt am Main, Germany.
authors.forename: Gerhard
authors.initials: G
authors.lastname: Hummer
authors.affiliation: Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.
authors.forename: Sébastien
authors.initials: S
authors.lastname: Boutet
authors.affiliation: Max-Planck-Institut für Medizinische Forschung, Jahnstraße 29, 69120 Heidelberg, Germany. thomas.barends@mpimf-heidelberg.mpg.de ilme.schlichting@mpimf-heidelberg.mpg.de.
authors.forename: Ilme
authors.initials: I
authors.lastname: Schlichting
mesh_terms: D000818:Animals; D002248:Carbon Monoxide / Q000737:chemistry; D018360:Crystallography, X-Ray; D006418:Heme / Q000737:chemistry; D006736:Horses; D007501:Iron / Q000737:chemistry; D008024:Ligands; D056004:Molecular Dynamics Simulation; D009038:Motion; D009211:Myoglobin / Q000737:chemistry*; D010782:Photolysis; D017433:Protein Structure, Secondary
chemical_list: D008024:Ligands; D009211:Myoglobin; C018013:carboxymyoglobin; D006418:Heme; D002248:Carbon Monoxide; D007501:Iron