A method is introduced for quantitatively analyzing photon echo decay measurements to characterize excitation-induced decoherence resulting from the phenomenon of instantaneous spectral diffusion. Detailed analysis is presented that allows fundamental material properties to be extracted that predict and describe excitation-induced decoherence for a broad range of measurements, applications and experimental conditions. Motivated by the need for a method that enables systematic studies of ultra-low decoherence systems and direct comparison of properties between optical materials, this approach employs simple techniques and analytical expressions that avoid the need for difficult to measure and often unknown material parameters or numerical simulations. This measurement and analysis approach is demonstrated for the 3H6to 3H4optical transition of three thulium-doped crystals, Tm3+:YAG, Tm3+:LiNbO3and Tm3+:YGG, that are currently employed in quantum information and classical signal processing demonstrations where minimizing decoherence is essential to achieve high efficiencies and large signal bandwidths. These new results reveal more than two orders of magnitude variation in sensitivity to excitation-induced decoherence among the materials studied and establish that the Tm3+:YGG system offers the longest optical coherence lifetimes and the lowest levels of excitation-induced decoherence yet observed for any known thulium-doped material.