Analysis of cooperativity and localization for atomic rearrangements.
We propose measures of localization and cooperativity for the analysis of atomic rearrangements. We show that for both clusters and bulk material cooperative rearrangements usually have significantly lower barriers than uncooperative ones, irrespective of the degree of localization. We also find that previous methods used to sample stationary points are biased towards rearrangements of particular types. Linear interpolation between local minima in double-ended transition state searches tends to produce cooperative rearrangements, while random perturbations of all the coordinates, as sometimes used in single-ended searches, have the opposite effect.
University Chemical Laboratories, Lensfield Road, Cambridge CB21EW, United Kingdom. sat39@cam.ac.uk
Semen A
SA
Trygubenko
David J
DJ
Wales