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Continuum Elastic Theory of Adsorbate Vibrational Relaxation | | Steven P. Lewis
; M. V. Pykhtin
; E. J. Mele
; Andrew M. Rappe
; | | Date: |
30 Sep 1997 | | Subject: | Materials Science | cond-mat.mtrl-sci | | Abstract: | An analytical theory is presented for the damping of low-frequency adsorbate vibrations via resonant coupling to the substrate phonons. The system is treated classically, with the substrate modeled as a semi-infinite elastic continuum and the adsorbate overlayer modeled as an array of point masses connected to the surface by harmonic springs. The theory provides a simple expression for the relaxation rate in terms of fundamental parameters of the system: $gamma = mar{omega}_0^2/A_c
ho c_T$, where $m$ is the adsorbate mass, $ar{omega}_0$ is the measured frequency, $A_c$ is the overlayer unit-cell area, and $
ho$ and $c_T$ are the substrate mass density and transverse speed of sound, respectively. This expression is strongly coverage dependent, and predicts relaxation rates in excellent quantitative agreement with available experiments. For a half-monolayer of carbon monoxide on the copper (100) surface, the predicted damping rate of in-plane frustrated translations is $0.50 imes 10^{12}$~s$^{-1}$, as compared to the experimental value of $(0.43pm0.07) imes 10^{12}$ s$^{-1}$. Furthermore it is shown that, for all coverages presently accessible to experiment, adsorbate motions exhibit collective effects which cannot be treated as stemming from isolated oscillators. | | Source: | arXiv, cond-mat/9709346 | | Services: | Forum | Review | PDF | Favorites | |
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