Abstract: A new scheme was proposed for investigating homogeneous gas phase chemical reaction kinetics.Direct mathematical deconvolution through inverse problem scheme was achieved by taking the advantage of the spatial resolved nature of Raman spectroscopy.Three-dimentional, spatially resolved gas phase species concentration profiles along the centerline of a cylindrical inverted vertical impinging flow reactor were obtained by in situ measuring the ratio of the vibrational Raman intensity of reactant to that of N₂.Gas phase temperature profile along the centerline was obtained simultaneously through N₂ Raman rotational spectra.Binary diffusion coefficient and homogeneous gas phase chemical reaction rate constant were then estimated through the output least square method.The stability of the inverse problem was achieved by using the Tikhonov regularization method.TMGa-N₂ binary diffusion coefficient and homogeneous decomposition reaction rate constant of TMGa in N₂ were identified.The identified TMGa-N₂ binary mass diffusion coefficient and TMGa thermal decomposition rate constant are 0.08 cm²•s^-1 and 3.4×10¹⁵ exp(60.1/RT) respectively, which match literature values very well.