Ultrafast Dynamics of Carboxy-Hemoglobin: Two-Dimensional Infrared Spectroscopy Experiments and Simulations

Cyril Falvo 1 Louis Daniault 2 Thibault Vieille 2 Vincent Kemlin 2 Jean-Christophe Lambry 2 Christoph Meier 3 Marten H. Vos 2 Adeline Bonvalet 2 Manuel Joffre 2
1 ISMO - Institut des Sciences Moléculaires d'Orsay
2 LOB - Laboratoire d'Optique et Biosciences
3 Théorie (LCAR)
LCAR - Laboratoire Collisions Agregats Reactivite
Abstract : This Letter presents a comparison between experimental and simulated 2D mid-infrared spectra of carboxy-hemoglobin in the spectral region of the carbon monoxide stretching mode. The simulations rely on a fluctuating potential energy surface that includes both the effect of heme and the protein surroundings computed from molecular dynamics simulations. A very good agreement between theory and experiment is obtained with no adjustable parameters. The simulations show that the effect of the distal histidine through the hydrogen bond is strong and is directly responsible for the slow decay of the frequency–frequency correlation function on a 10 ps time scale. This study confirms that fluctuations in carboxy-hemoglobin are more inhomogeneous than those in the more frequently studied carboxy-myoglobin. The comparison between simulations and experiments brings valuable information on the complex relation between protein structure and spectral diffusion.
Document type :
Journal articles
Complete list of metadatas
https://hal-polytechnique.archives-ouvertes.fr/hal-01165610
Contributor : Denis Roura <>
Submitted on : Friday, June 19, 2015 - 3:22:28 PM
Last modification on : Monday, April 29, 2019 - 3:48:41 PM

Identifiers

Collections

X | LCAR | X-LOB | JYB-LAB | PARISTECH | IRSAMC | LCAR_THE | UNIV-PARIS-SACLAY | X-DEP-BIO | UNIV-TLSE3

Citation

Cyril Falvo, Louis Daniault, Thibault Vieille, Vincent Kemlin, Jean-Christophe Lambry, et al.. Ultrafast Dynamics of Carboxy-Hemoglobin: Two-Dimensional Infrared Spectroscopy Experiments and Simulations. Journal of Physical Chemistry Letters, American Chemical Society, 2015, 6 (12), pp.2216-2222. ⟨10.1021/acs.jpclett.5b00811⟩. ⟨hal-01165610⟩

Export

BibTeX TEI DC DCterms EndNote

Share

Metrics

Record views

362

Contact

support.ccsd.cnrs.fr
hal.support@ccsd.cnrs.fr
Logo CCSD