Abstract

A systematic investigation of various (NO+O) coadsorbate layers on Ru(001) is presented. By using infrared absorption spectroscopy, fundamental and overtone bands were studied in a wide temperature range to extract dynamical information on lifetime broadening (low-temperature limit) and dephasing behavior (thermal broadening and line shifts). The layers studied were (1) 3NO-(2×2)/Ru(001), (2) (2NO+O)(2×2)/Ru(001) and (3) (NO+2O)(2×2)/Ru(001). It is found that replacing hollow-site NO by oxygen atoms causes characteristic frequency shifts of ν Ru–NO and ν N–O of linearly bond on-top NO which is present for all three layers. In agreement with earlier results on CO/Ru(001) and with theoretical prediction, the ν N–O″ overtone band displays rapid broadening with increasing temperature (about four times faster than the respective localized ν N–O fundamental band) while the temperature-dependent line shift and the 0 K linewidth is twice as high as observed for ν N–O. An unusually large bandwidth close to 100 cm −1 is found for the ν N–O mode of the row-like (NO+O)(2×1)/Ru(001) overlayer.

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