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Highly reactive intermediates, Azidoketene O=C=CH–NNN and Isocyanatoketene O=C=CH–N=C=O have attracted much attention in computational chemistry. Full geometry optimizations are carried out on singlet and triplet states of ketene substituted Azidoketene O=C=CH–NNN and Isocyanatoketene O=C=CH– N=C=O by HF, HF+ MP2, LDA, BLYP, B3LYP, MP2, MP3 and MP4 methods using 6–311++G (d, p) basis set of the Gaussian 09.