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The pure rotational transitions in the 220–460 GHz spectral range of TiO (X3Δr) and TiN(X2Σ+) have been observed using a source-modulated submillimeter-wave spectrometer. In addition, the two lowest rotational transitions of TiO at 63 and 94 GHz have been observed using molecular beam pump/probe microwave optical double resonance (PPMODR) technique. An improved set of spectroscopic parameters for...