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We present in this study a spectroscopic investigation of spontaneous delamination of amorphous carbon nitride (a-CNx) films deposited on silicon substrates (Si) by rf magnetron sputtering of a graphite target in pure Ar/N2 gas mixture. The microstructural properties of the films were determined in their as-deposited state using infrared absorption and Raman spectroscopy experiments. Various shapes of debonding patterns have been observed. Based on the present experimental evidence, a description of nitrogen incorporation and the resulting hybridization states of the CN bonds in the a-CNx films prior and after delamination are proposed to elucidate the microstructural origin of this delamination occurring along the a-CNx/Si interface and the physicochemical mechanism that governed its dynamic.

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