title: Molecular structure and free energy landscape for electron transport in the decahaem cytochrome MtrF.
abstract: The free energy profile for electron flow through the bacterial decahaem cytochrome MtrF has been computed using thermodynamic integration and classical molecular dynamics. The extensive calculations on two versions of the structure help to validate the method and results, because differences in the profiles can be related to differences in the charged amino acids local to specific haem groups. First estimates of reorganization free energies λ yield a range consistent with expectations for partially solvent-exposed cofactors, and reveal an activation energy range surmountable for electron flow. Future work will aim at increasing the accuracy of λ with polarizable forcefield dynamics and quantum chemical energy gap calculations, as well as quantum chemical computation of electronic coupling matrix elements.
authors.affiliation: Condensed Matter and Materials Physics, Department of Physics and Astronomy, Faculty of Mathematical and Physical Sciences, University College London, Gower Street, London WC1E 6BT, UK.
authors.forename: Marian
authors.initials: M
authors.lastname: Breuer
authors.forename: Piotr
authors.initials: P
authors.lastname: Zarzycki
authors.forename: Liang
authors.initials: L
authors.lastname: Shi
authors.forename: Thomas A
authors.initials: TA
authors.lastname: Clarke
authors.forename: Marcus J
authors.initials: MJ
authors.lastname: Edwards
authors.forename: Julea N
authors.initials: JN
authors.lastname: Butt
authors.forename: David J
authors.initials: DJ
authors.lastname: Richardson
authors.forename: James K
authors.initials: JK
authors.lastname: Fredrickson
authors.forename: John M
authors.initials: JM
authors.lastname: Zachara
authors.forename: Jochen
authors.initials: J
authors.lastname: Blumberger
authors.forename: Kevin M
authors.initials: KM
authors.lastname: Rosso
mesh_terms: D001425:Bacterial Outer Membrane Proteins / Q000737:chemistry*; D003580:Cytochromes / Q000737:chemistry*; D004579:Electron Transport; D006418:Heme / Q000737:chemistry; D056004:Molecular Dynamics Simulation; D020836:Protein Structure, Quaternary; D017433:Protein Structure, Secondary; D020592:Shewanella / Q000378:metabolism*; D013816:Thermodynamics
chemical_list: D001425:Bacterial Outer Membrane Proteins; D003580:Cytochromes; D006418:Heme