Pushing periodic-disorder-induced phase matching into the deep-ultraviolet spectral region: theory and demonstration

Nonlinear frequency conversion is a ubiquitous technique that is used to obtain broad-range lasers and supercontinuum coherent sources. The phase-matching condition (momentum conservation relation) is the key criterion but a challenging bottleneck in highly efficient conversion. Birefringent phase matching (BPM) and quasi-phase matching (QPM) are two feasible routes but are strongly limited in natural anisotropic crystals or ferroelectric crystals. Therefore, it is in urgent demand for a general technique that can compensate for the phase mismatching in universal nonlinear materials and in broad wavelength ranges. Here, an additional periodic phase (APP) from order/disorder alignment is proposed to meet the phase-matching condition in arbitrary nonlinear crystals and demonstrated from the visible region to the deep-ultraviolet region (e.g., LiNbO₃ and quartz). Remarkably, pioneering 177.3-nm coherent output is first obtained in commercial quartz crystal with an unprecedented conversion efficiency above 1‰. This study not only opens a new roadmap to resuscitate those long-neglected nonlinear optical crystals for wavelength extension, but also may revolutionize next-generation nonlinear photonics and their further applications.