Skip to Content
Merck
  • Renormalization of myoglobin-ligand binding energetics by quantum many-body effects.

Renormalization of myoglobin-ligand binding energetics by quantum many-body effects.

Proceedings of the National Academy of Sciences of the United States of America (2014-04-11)
Cédric Weber, Daniel J Cole, David D O'Regan, Mike C Payne
ABSTRACT

We carry out a first-principles atomistic study of the electronic mechanisms of ligand binding and discrimination in the myoglobin protein. Electronic correlation effects are taken into account using one of the most advanced methods currently available, namely a linear-scaling density functional theory (DFT) approach wherein the treatment of localized iron 3d electrons is further refined using dynamical mean-field theory. This combination of methods explicitly accounts for dynamical and multireference quantum physics, such as valence and spin fluctuations, of the 3d electrons, while treating a significant proportion of the protein (more than 1,000 atoms) with DFT. The computed electronic structure of the myoglobin complexes and the nature of the Fe-O2 bonding are validated against experimental spectroscopic observables. We elucidate and solve a long-standing problem related to the quantum-mechanical description of the respiration process, namely that DFT calculations predict a strong imbalance between O2 and CO binding, favoring the latter to an unphysically large extent. We show that the explicit inclusion of the many-body effects induced by the Hund's coupling mechanism results in the correct prediction of similar binding energies for oxy- and carbonmonoxymyoglobin.

MATERIALS
Product Number
Brand
Product Description

Sigma-Aldrich
Titanium, foil, thickness 0.5 mm, 99.99% trace metals basis
Sigma-Aldrich
Titanium, foil, thickness 0.25 mm, 99.99% trace metals basis
Sigma-Aldrich
Titanium(IV) oxide, anatase, powder, 99.8% trace metals basis
Sigma-Aldrich
Titanium, foil, thickness 0.25 mm, 99.7% trace metals basis
Sigma-Aldrich
Titanium(IV) oxide, contains 1% Mn as dopant, nanopowder, <100 nm particle size (BET), ≥97%
Sigma-Aldrich
Titanium, powder, <45 μm avg. part. size, 99.98% trace metals basis
Sigma-Aldrich
Titanium, wire, diam. 0.5 mm, 99.99% trace metals basis
Sigma-Aldrich
Titanium, sponge, 1-20 mm, 99.5% trace metals basis
Sigma-Aldrich
Titanium, powder, −100 mesh, 99.7% trace metals basis
Sigma-Aldrich
Titanium, evaporation slug, diam. × L 6.3 mm × 6.3 mm, ≥99.99% trace metals basis
Sigma-Aldrich
Titanium, foil, thickness 0.127 mm, ≥99.99% trace metals basis
Titanium, IRMM®, certified reference material, 0.1 mm foil
Sigma-Aldrich
Titanium(IV) oxide, nanowires, diam. × L ~10 nm × 10 μm
Sigma-Aldrich
Titanium(IV) oxide, nanowires, diam. × L ~100 nm × 10 μm
Sigma-Aldrich
Titanium(IV) oxide, anatase, powder, −325 mesh, ≥99% trace metals basis
Sigma-Aldrich
Titanium(IV) oxide, nanopowder, 21 nm primary particle size (TEM), ≥99.5% trace metals basis
Sigma-Aldrich
Titanium(IV) oxide, anatase, nanopowder, <25 nm particle size, 99.7% trace metals basis
Titanium, mesh, 100x100mm, nominal aperture 4.3mm, wire diameter 1.5mm, 4.4x4.4 wires/inch, open area 94%, platinized diamond mesh
Titanium, rod, 200mm, diameter 20mm, annealed, 99.6+%
Titanium, rod, 100mm, diameter 1.5mm, annealed, 99.6+%
Titanium, rod, 100mm, diameter 16mm, annealed, 99.6+%
Titanium, rod, 50mm, diameter 9.5mm, annealed, 99.99+%
Titanium, microfoil, disks, 25mm, thinness 1.0μm, specific density 429μg/cm2, permanent mylar 3.5μm support, 99.6+%
Titanium, tube, 200mm, outside diameter 6.1mm, inside diameter 5.1mm, wall thickness 0.5mm, annealed, 99.6+%
Titanium, tube, 100mm, outside diameter 3.0mm, inside diameter 1.5mm, wall thickness 0.75mm, annealed, 99.6+%
Titanium, rod, 500mm, diameter 3.0mm, annealed, 99.6+%
Titanium, tube, 200mm, outside diameter 0.81mm, inside diameter 0.61mm, wall thickness 0.1mm, as drawn, 99.6+%
Titanium, tube, 100mm, outside diameter 0.81mm, inside diameter 0.61mm, wall thickness 0.1mm, as drawn, 99.6+%
Titanium, rod, 1000mm, diameter 2mm, annealed, 99.6+%
Titanium, rod, 100mm, diameter 20mm, as drawn, 99.99+%