Hybrid siloxane-silica coatings have been prepared by hydrolysis and c
ondensation of N-[3-triethoxysilylpropyl]-2,4-dinitrophenylamine (TSDP
) and tetramethoxysilane (TMOS) precursors. Hetero- and home-condensat
ions between both precursors have been demonstrated to occur in the ea
rly stages of the process via O-17 and Si-29 nuclear magnetic resonanc
e (NMR) in solution. These hybrids can be described as nanocomposites
made of polysiloxane-based domains cross-linked by silica-based nanopa
rticles, as evidenced bd solid-state NMR, differential scanning calori
metry (DSC) and Fourier-transform infrared (FTIR) studies. Moreover, t
he high degree of interpenetration occurring in these materials is evi
denced by the presence of some Q and T subunits sequestered within the
se polysiloxane and silica-based domains, respectively. The high-resol
ution solid-state C-13 NMR technique has shown that the mobility of th
e propyl 2,4-dinitrophenylamine chromophores is correlated with the gl
ass-transition phenomenon of the matrix.