Reaction coordinates and rates from transition paths

Proc Natl Acad Sci U S A. 2005 May 10;102(19):6732-7. doi: 10.1073/pnas.0408098102. Epub 2005 Apr 6.

Abstract

The molecular mechanism of a reaction in solution is reflected in its transition-state ensemble and transition paths. We use a Bayesian formula relating the equilibrium and transition-path ensembles to identify transition states, rank reaction coordinates, and estimate rate coefficients. We also introduce a variational procedure to optimize reaction coordinates. The theory is illustrated with applications to protein folding and the dipole reorientation of an ordered water chain inside a carbon nanotube. To describe the folding of a simple model of a three-helix bundle protein, we variationally optimize the weights of a projection onto the matrix of native and nonnative amino acid contacts. The resulting one-dimensional reaction coordinate captures the folding transition state, with formation and packing of helix 2 and 3 constituting the bottleneck for folding.

MeSH terms

  • Adenosine Triphosphate / chemistry
  • Algorithms
  • Bayes Theorem
  • Biophysics / methods*
  • Hydrogen Bonding
  • Models, Molecular
  • Models, Statistical
  • Nanotechnology / methods
  • Nanotubes, Carbon / chemistry
  • Phase Transition
  • Probability
  • Protein Conformation
  • Protein Folding*
  • Protein Structure, Secondary
  • Software
  • Water / chemistry

Substances

  • Nanotubes, Carbon
  • Water
  • Adenosine Triphosphate