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Importance of many-body effects in the kernel of hemoglobin for ligand binding
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Weber, Cedric, O'Regan, David D., Hine, Nicholas, Littlewood, Peter B., Kotliar, Gabriel and Payne, Mike C. (2013) Importance of many-body effects in the kernel of hemoglobin for ligand binding. Physical Review Letters, 110 (10). 106402. doi:10.1103/PhysRevLett.110.106402
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Official URL: http://dx.doi.org/10.1103/PhysRevLett.110.106402
Abstract
We propose a mechanism for binding of diatomic ligands to heme based on a dynamical orbital selection process. This scenario may be described as bonding determined by local valence fluctuations. We support this model using linear-scaling first-principles calculations, in combination with dynamical mean-field theory, applied to heme, the kernel of the hemoglobin metalloprotein central to human respiration. We find that variations in Hund’s exchange coupling induce a reduction of the iron 3d density, with a concomitant increase of valence fluctuations. We discuss the comparison between our computed optical absorption spectra and experimental data, our picture accounting for the observation of optical transitions in the infrared regime, and how the Hund’s coupling reduces, by a factor of 5, the strong imbalance in the binding energies of heme with CO and O2 ligands.
| Item Type: | Journal Article | ||||
|---|---|---|---|---|---|
| Subjects: | Q Science > QD Chemistry | ||||
| Divisions: | Faculty of Science > Physics | ||||
| Library of Congress Subject Headings (LCSH): | Ligand binding (Biochemistry) | ||||
| Journal or Publication Title: | Physical Review Letters | ||||
| Publisher: | American Physical Society | ||||
| ISSN: | 0031-9007 | ||||
| Official Date: | March 2013 | ||||
| Dates: |
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| Date of first compliant deposit: | 1 April 2016 | ||||
| Volume: | 110 | ||||
| Number: | 10 | ||||
| Number of Pages: | 6 | ||||
| Article Number: | 106402 | ||||
| DOI: | 10.1103/PhysRevLett.110.106402 | ||||
| Status: | Peer Reviewed | ||||
| Publication Status: | Published | ||||
| Access rights to Published version: | Restricted or Subscription Access | ||||
| Funder: | Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung [Swiss National Science Foundation] (SNSF), Engineering and Physical Sciences Research Council (EPSRC), United States. Department of Energy | ||||
| Grant number: | EP/G055882/1 (EPSRC), FWP 70069 (DOE), EP/F032773/1 (EPSRC) |
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