Effects of electronic relaxation processes on vibrational linewidths of adsorbates on surfaces: The case of CO/Cu(100)

Article

关键词: GENERALIZED GRADIENT APPROXIMATION;    PHONON SELF-ENERGY;    METAL-SURFACES;    RAMAN-SCATTERING;    SUPERCONDUCTING OXIDES;    OPTICAL-PROPERTIES;    CO;    CU(100);    SPECTROSCOPY;    IMPURITIES;   

DOI  :  10.1103/PhysRevB.94.224306

来源: SCIE

【 摘 要 】

We investigate nonadiabatic effects for the vibrational stretch mode of the CO molecule adsorbed on the top site of theCu(100) surface. By studying the long-wavelength (q approximate to 0) imaginary and real parts of the density functional theory based phonon self-energy due to the electron-phonon coupling Pi(lambda). we obtain the phonon linewidth and the frequency renormalization of the CO stretch mode, respectively. To simulate electronic scattering processes that lead to further damping of the phonon modes we include a phenomenological damping in the phonon self-energy, as well as in the single-electron spectral function that enters Pi(lambda), through the momentum distribution function. For the specific case of electron-impurity scattering we explicitly show how this process opens the indirect intraband channel and broadens the linewidth of the CO stretch mode. To emphasize the importance of accounting for electronic scattering processes we compare the phonon linewidths in the clean noninteracting limit (infinite electron lifetime) and when electronic scattering processes are phenomenologically included (finite electron lifetime) with available experimental data. We find that the agreement with experiments is improved in the latter case.

【 授权许可】

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