Ultrafast Structural Fluctuations of Myoglobin-Bound Thiocyanate and Selenocyanate Ions Measured with Two-Dimensional Infrared Photon Echo Spectroscopy

Chemphyschem. 2015 Nov 16;16(16):3468-76. doi: 10.1002/cphc.201500606. Epub 2015 Sep 11.

Abstract

Structural dynamics within the distal cavity of myoglobin protein is investigated using 2D-IR and IR pump-probe spectroscopy of the N≡C stretch modes of heme-bound thiocyanate and selenocyanate ions. Although myoglobin-bound thiocyanate group shows a doublet in its IR absorption spectrum, no cross peaks originating from chemical exchange between the two components are observed in the time-resolved 2D IR spectra within the experimental time window. Frequency-frequency correlation functions of the two studied anionic ligands are obtained by means of a few different analysis approaches; these functions were then used to elucidate the differences in structural fluctuation around ligand, ligand-protein interactions, and the degree of structural heterogeneity within the hydrophobic pocket of these myoglobin complexes.

Keywords: IR spectroscopy; myoglobin; protein dynamics; ultrafast vibrational dynamics; vibrational spectroscopy.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Cyanates / chemistry*
  • Cyanates / metabolism
  • Horses
  • Ions / chemistry
  • Myoglobin / chemistry*
  • Myoglobin / metabolism
  • Selenium Compounds / chemistry*
  • Selenium Compounds / metabolism
  • Spectroscopy, Fourier Transform Infrared
  • Thiocyanates / chemistry*
  • Thiocyanates / metabolism

Substances

  • Cyanates
  • Ions
  • Myoglobin
  • Selenium Compounds
  • Thiocyanates
  • carboxymyoglobin
  • myoglobin nitroxide
  • selenocyanic acid
  • thiocyanate