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In parametric conversion, phase-matching techniques such as birefringence and quasi phase-matching (PM) with the designed crystal angle or periodically poled polarities are employed to fulfill the requirement of momentum conservation. However, directly using phase-mismatched interactions in nonlinear media with large quadratic nonlinear coefficient remains unheeded. Here, for the first time to the best of our knowledge, we study the phase-mismatched difference-frequency generation (DFG) in an isotropic cadmium telluride (CdTe) crystal, with the comparison of other DFG processes based on birefringence-PM, quasi-PM, and random-quasi-PM. Long-wavelength mid-infrared (LWMIR) phase-mismatched DFG with an ultra-broadband spectral tuning range of 6–17 µm based on CdTe is demonstrated. Thanks to the giant quadratic nonlinear coefficient (∼109 pm/V) and good figure of merit in the parametric process, the output power up to 100 µW is obtained, which is comparable to or even better than the DFG output from a polycrystalline ZnSe with the same thickness facilitated by random-quasi-PM. A proof-of-concept demonstration in gas sensing of CH4 and SF6 is conducted based on the phase-mismatched DFG as a typical application. Our results demonstrate the feasibility of phase-mismatched parametric conversion in producing useful LWMIR power and ultra-broadband tunability in a simple and convenient way without the necessity of controlling the polarization, phase-matching angle, or pole periods, which could find applications in the fields of spectroscopy and metrology.

We demonstrate the first (to the best of our knowledge) tunable femtosecond (fs) mid-infrared (MIR) optical parametric amplifier (OPA) based on BaGa4Se7 (BGSe) crystal with an ultra-broadband spectral range. Benefiting from the broad transparency range, high nonlinearity, and relatively large bandgap of BGSe, the MIR OPA pumped at 1030 nm with a repetition of 50 kHz has an output spectrum that is tunable across an extremely wide spectral range spanning from 3.7 to 17 µm. The maximum output power of the MIR laser source is measured as 10 mW at a center wavelength of 16 µm, corresponding to a quantum conversion efficiency of 5%. Power scaling is straightforwardly achieved by using a stronger pump in BGSe with an available large aperture size. A pulse width of 290 fs centered at 16 µm is supported by the BGSe OPA. Our experimental result indicates that BGSe crystal could serve as a promising nonlinear crystal for fs MIR generation with an ultra-broadband tuning spectral range via parametric downconversion for applications such as MIR ultrafast spectroscopy.