Cascaded difference frequency generation in organic crystal 4'-dimethylamino-N-methyl-4-stilbazolium tosylate

In this Letter, we verified, for the first time to the best of our knowledge, an efficient cascaded difference frequency generation (DFG) with multi-order red shift. The experiment was performed with homemade organic crystals pumped by an optical parametric oscillator. The characteristics of energy conversion during DFG were investigated comprehensively at different frequencies and crystal thicknesses. Theoretical explanations were provided, based on the coupled-wave equations. The calculations predicted that the cascading effect contributed to a sustained growth of the DFG output (free from the saturation and shrinkage), especially in thick crystals. By measuring the optical spectrum, remarkable cascading processes of at least seven orders were observed. This effect shows the potential to overcome the quantum defect of the terahertz-wave DFG and fundamentally improve the conversion efficiency.