“…The addition of acetonitrile to the Si(100)‐2×1 surface was first reported by Xu in 2001 2. Since the initial study, the addition of acetonitrile to the Si(100)‐2×1 surface has been examined at various temperatures, including room temperature, and the adducts have been identified using a variety of techniques, including temperature‐programmed desorption (TPD),2 high‐resolution electron energy loss spectroscopy (HREELS),2 conventional X‐ray photoelectron spectroscopy (XPS),2, 3 synchrotron radiation XPS,4, 5 near‐edge X‐ray absorption fine structures (NEXAFS),4, 5 resonant Auger electron spectroscopy (RAES),6 and multiple internal reflection Fourier transform infrared (MIR‐FTIR) spectroscopy 3. Current theoretical2, 5, 7–10 and experimental3, 5, 6 evidence supports the formation of three types of nitrile adducts in equal amounts on the Si surface at room temperature: an α‐CH insertion adduct ( 1 ), a cycloadduct involving the CN bond ( 2 a , b ), and a twisted ketenimine product ( 3 a , b ) (Figure 1).…”