Complex of Silylene with Nitrogen: A Combined Matrix‐Spectroscopic and Density Functional Theory Study

The quest for a new and productive route to matrix‐isolated silylene 1 has led to the observation that the presence of nitrogen is favorable, as under such conditions 1 is stabilized by formation of a donor–acceptor complex 1 ⋅N 2 . Either matrix photolysis of diazidosilane or pulsed high‐vacuum flash pyrolysis of 1,1,1‐trimethyldisilane, followed by condensation of the products with nitrogen at 10 K, were applied as synthetic procedures. In a similar manner, complex 1 ⋅CO can be generated. The results are supported by isotopic‐labeling studies. The structural elucidation of the new species is based on the comparison of experimental IR and UV/Vis spectra with data from density functional theory calculations.