We investigated the high-purity entangled photon-pair generation in five kinds of “non-poled” potassium titanyl phosphate (KTP) isomorphs (i.e., KTiOPO4, RbTiOPO4, KTiOAsO4, RbTiOAsO4, and CsTiOAsO4). The technique is based on the spontaneous parametric down-conversion (SPDC) under Type II extended phase matching (EPM), where the phase matching and the group velocity matching are simultaneously achieved between the interacting photons in non-poled crystals rather than periodically poled (PP) KTPs that are widely used for quantum experiments. We discussed both theoretically and numerically all aspects required to generate photon pairs in non-poled KTP isomorphs, in terms of the range of the beam propagation direction (or the spectral range of photons) and the corresponding effective nonlinearities and beam walk-offs. We showed that the SPDC efficiency can be increased in non-poled KTP isomorphs by 29% to 77% compared to PPKTP cases. The joint spectral analyses showed that photon pairs can be generated with high purities of 0.995–0.997 with proper pump filtering. In contrast to the PPKTP case, where the EPM is achieved only at one specific wavelength, the spectral position of photon pairs in the non-poled KTP isomorphs can be chosen over the wide range of 1883.8–2068.1 nm.
The mid-infrared (mid-IR) continuum generation based on broadband second harmonic generation (SHG) (or difference frequency generation) is of great interest in a wide range of applications such as free space communications, environmental monitoring, thermal imaging, high-sensitivity metrology, gas sensing, and molecular fingerprint spectroscopy. The second-order nonlinear optic (NLO) crystals have been spotlighted as a material platform for converting the wavelengths of existing lasers into the mid-IR spectral region or for realizing tunable lasers. In particular, the spectral coverage could be extended to ~19 µm with non-oxide NLO crystals. In this paper, we theoretically and numerically investigated the broadband SHG properties of non-oxide mid-IR crystals in three categories: chalcopyrite semiconductors, defect chalcopyrite, and orthorhombic ternary chalcogenides. The technique is based on group velocity matching between interacting waves in addition to birefringent phase matching. We will describe broadband SHG characteristics in terms of beam propagation directions, spectral positions of resonance, effective nonlinearities, spatial walk-offs between interacting beams, and spectral bandwidths. The results will show that the spectral bandwidths of the fundamental wave allowed for broadband SHG to reach several hundreds of nm. The corresponding SH spectral range spans from 1758.58 to 4737.18 nm in the non-oxide crystals considered in this study. Such broadband SHG using short pulse trains can potentially be applied to frequency up-conversion imaging in the mid-IR region, in information transmission, and in nonlinear optical signal processing.
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