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Experimental-computational techniques for investigation of the mechanisms of physicochemical processes in nitrogenated plasma discharges are presented. These techniques are based on combining level-to-level semiempirical collisional-radiative models (CRMs) of low-temperature plasma and optical diagnostics methods. Nonstationary level-to-level semiempirical CRMs include computer codes for (i) processing and simulation of the optical emission and coherent anti-Stokes Raman scattering spectra and (ii) solution of the kinetic Boltzmann equation for electrons, thermal conductivity equation, and balance equations for most of plasma neutral, excited, and charged particles. Banks of data were created for the processing and simulation of spectra and the solution of kinetic equations. The models were validated by comparison of the obtained results with numerous known data of experiments and calculations for different parameters. The optical diagnostics of discharges includes coherent anti-Stokes Raman spectroscopy, optical interferometry, and emission spectroscopy.