“…Typically, the type of surface reconstruction determines the characteristic features of the corresponding RA spectra, but a number of different parameters such as atomic order, purity, and sample temperature are decisive for the position and intensity of the observed peaks [9,16,17,24]. Beyond that, major signal contributions can arise from bulk-related anisotropies (such as ordering [25]) or from mesoscopic 3D-structures on the surface such as facets, steps, terraces or islands [26,27]. Various origins of the RAS signal have already been modeled by empirical [26] and semiempirical [28] methods, some even by ab initio computational techniques [18], but still experimental RA spectra can generally not be predicted reliably by theoretical calculations.…”