Collective Motion and Structural Order in Adsorbate Vibrational Dynamics

M. V. Pykhtin; Steven P. Lewis; E. J. Mele; Andrew M. Rappe

doi:10.1103/PhysRevLett.81.5940

Collective Motion and Structural Order in Adsorbate Vibrational Dynamics

M. V. Pykhtin, Steven P. Lewis, E. J. Mele, and Andrew M. Rappe

Phys. Rev. Lett. 81, 5940 – Published 28 December 1998

Abstract

A simple, broadly applicable theory is developed to describe resonant vibrational coupling between adsorbates and a substrate lattice. This is one of the principal mechanisms governing the relaxation of adsorbate vibrations. This theory can be applied to widely varying surface coverages and arbitrary overlayer structures, and it correctly incorporates collective adsorbate motion, which has been shown to have a critical impact on the relaxation dynamics. Vibrational lifetimes predicted by this theory are in excellent quantitative agreement with experiments on adsorbate systems ranging from a diffuse, disordered overlayer to a dense, periodic overlayer.

Received 10 August 1998

DOI:https://doi.org/10.1103/PhysRevLett.81.5940

Authors & Affiliations

M. V. Pykhtin¹, Steven P. Lewis^2,*, E. J. Mele¹, and Andrew M. Rappe²

¹Department of Physics and Laboratory for Research on the Structure of Matter, University of Pennsylvania, Philadelphia, Pennsylvania 19104
²Department of Chemistry and Laboratory for Research on the Structure of Matter, University of Pennsylvania, Philadelphia, Pennsylvania 19104