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(IV) oxide, mixture of rutile and anatase, nanoparticles, <150 nm particle size (volume distribution, DLS), dispersion, 40 wt. % in H2O, 99.5% trace metals basis
Sigma-Aldrich
Titanium(IV) oxide, rutile, nanopowder, <100 nm particle size, 99.5% trace metals basis
Sigma-Aldrich
Titanium(IV) oxide, mixture of rutile and anatase, nanopowder, <100 nm particle size (BET), 99.5% trace metals basis
Sigma-Aldrich
Titanium(IV) oxide, rutile, <001>, (single crystal substrate), ≥99.9% trace metals basis, L × W × thickness 10 mm × 10 mm × 0.5 mm
Titanium, IRMM®, certified reference material, 0.5 mm wire
Titanium, IRMM®, certified reference material, 0.5 mm foil
Sigma-Aldrich
Titanium(IV) oxide, rutile, 99.995% trace metals basis
Sigma-Aldrich
Titanium, wire, diam. 0.81 mm, 99.7% trace metals basis
Sigma-Aldrich
Titanium, 5-10 mm, ≥99.99% trace metals basis (purity exclusive of Na and K content)
Sigma-Aldrich
Titanium, foil, thickness 0.025 mm, 99.98% trace metals basis
Sigma-Aldrich
Titanium, wire, diam. 1.0 mm, 99.99% trace metals basis
Sigma-Aldrich
Titanium, foil, thickness 2.0 mm, 99.7% trace metals basis
Sigma-Aldrich
Titanium, wire, diam. 0.25 mm, 99.7% trace metals basis
Sigma-Aldrich
Titanium(IV) oxide, rutile, ≥99.98% trace metals basis
Sigma-Aldrich
Titanium, foil, thickness 0.127 mm, 99.7% trace metals basis
Sigma-Aldrich
Titanium(IV) oxide, rutile, powder, <5 μm, ≥99.9% trace metals basis
Titanium, microfoil, disks, 25mm, thinness 0.25μm, specific density 112.6μg/cm2, permanent mylar 3.5μm support, 99.6+%
Titanium, rod, 200mm, diameter 3.0mm, annealed, 99.6+%
Titanium, rod, 200mm, diameter 9.5mm, annealed, 99.99+%
Titanium, tube, 100mm, outside diameter 1.6mm, inside diameter 1.2mm, wall thickness 0.2mm, hard, 99.6+%
Titanium, tube, 100mm, outside diameter 10.3mm, inside diameter 8.7mm, wall thickness 0.8mm, annealed, 99.6+%
Titanium, tube, 200mm, outside diameter 25.4mm, inside diameter 23.62mm, wall thickness 0.89mm, annealed, 99.6+%
Titanium, rod, 1000mm, diameter 3.0mm, annealed, 99.6+%
Titanium, mesh, 100x100mm, nominal aperture 0.19mm, wire diameter 0.23mm, 60x60 wires/inch, open area 20%, twill weave
Titanium, rod, 100mm, diameter 2mm, annealed, 99.6+%
Titanium, microfoil, disks, 25mm, thinness 0.5μm, specific density 225.4μg/cm2, permanent mylar 3.5μm support, 99.6+%
Titanium, rod, 100mm, diameter 9.5mm, annealed, 99.99+%
Titanium, rod, 100mm, diameter 2mm, as drawn, 99.99+%
Titanium, rod, 10mm, diameter 50mm, 99.99+%
Titanium, rod, 200mm, diameter 4mm, annealed, 99.6+%