Constraint-free wavelength conversion supported by giant optical refraction in a 3D perovskite supercrystal

Nonlinear response in a material increases with its index of refraction as n(4). Commonly, n - 1 so that diffraction, dispersion, and chromatic walk-off limit nonlinear scattering. Ferroelectric crystals with a periodic 3D polarization structure overcome some of these constraints through versatile Cherenkov and quasi-phase-matching mechanisms. Three-dimensional self-structuring can also lead to a giant optical refraction. Here, we perform second-harmonic-generation experiments in KTN:Li in conditions of giant broadband refraction. Enhanced response causes wavelength conversion to occur in the form of bulk Cherenkov radiation without diffraction and chromatic walk-off, even in the presence of strong wave-vector mismatch and highly focused beams. The process occurs with a wide spectral acceptance of more than 100 nm in the near infrared spectrum, an ultra-wide angular acceptance of up to 40 degrees, with no polarization selectivity, and can be tuned to allow bulk supercontinuum generation. Results pave the way to highly efficient and adaptable nonlinear optical devices with the promise of single-photon-to-single-photon nonlinear optics.