Due to unnoticeable changes in complex refractive index of tissue under varied pathological and physiological states, the traditional optical coherence tomography (OCT) is deficient in molecular characterization. In this paper, the stimulated-emission based optical coherence tomography is proposed, which provides both molecular contrast and scattering contrast OCT imaging simultaneously. Based on the established ultra-high resolution spectral domain OCT system, a pump-probe spectral domain OCT system with a single wide-bandwidth light source is developed through an added modulated pump beam via spectrum splitting. In addition, the theory about the stimulated-emission signal and the image formulation under the modulated pump beam is presented. The coherent detection of the transient stimulated emission is realized by the developed pump-probe spectral domain OCT system. With the stimulated-emission OCT signal and the traditional OCT signal obtained at the same time, molecular contrast OCT images of the samples consisting of nitride powder are reconstructed successfully.