Three-dimensional direct femtosecond laser writing of second-order nonlinearities in glass

We demonstrate that direct femtosecond laser writing in silver-containing zinc and gallium phosphate glass enables generation of three-dimensional (3D) optical second-order nonlinear microstructures having an χ(2) value about 2.5 times that of quartz. The proposed physical model involves photo-reduction, photo-dissociation, and migration of silver species within the glass matrix. 3D laser-written second-order nonlinear structures could become a new class of nonlinear optical components.