Yan Sheng

Nonlinear photonic crystals (NPCs) with spatially modulated second‐order nonlinear coefficients are indispensable in nonlinear optics and modern photonics. To access full degrees of freedom in the generation and control of coherent light at new frequencies, three dimensional (3D) NPCs have been recently fabricated employing the femtosecond laser writing technique in ferroelectric crystals. However, the nonlinear interaction efficiencies in 3D NPCs so far are rather low, which has been a major barrier to further development. Here, fabrication challenges of large‐scale 3D NPCs have been overcome to realize more than four orders of magnitude efficiency improvement over previously reported crystals. With the generation of second harmonic vortex beam as an example, the measured conversion efficiencies as high as 2.9 × 10 −6 W −1 (femtosecond pulse‐pumped) and 1.2 × 10 −5 W −1 (continuous‐wave‐pumped) are comparable with those in 1D or 2D NPCs. A general approach of structural simplification to relax fabrication challenge of truly complex 3D structures without sacrificing the predesigned functions is also presented. This realization of efficient nonlinear interactions in 3D NPCs paves the way for their novel applications in nonlinear photonics and quantum optics including nonlinear orbital angular momentum multiplexing and high‐dimensional entangled source.