Three-dimensional femtosecond laser nanolithography of crystals

So far, nanostructuring of hard optical crystals has been exclusively limited to their surface, as stress-induced crack formation and propagation render high-precision volume processes ineffective(1,2). Here, we show that the rate of nanopore chemical etching in the popular laser crystals yttrium aluminium garnet and sapphire can be enhanced by more than five orders of magnitude (from <0.6 nm h(-1) to similar to 100 mu m h(-1)) by the use of direct laser writing, before etching. The process makes it possible to produce arbitrary three-dimensional nanostructures with 100 nm feature sizes inside centimetre-scale laser crystals without brittle fracture. To showcase the potential of the technique we fabricate subwavelength diffraction gratings and nanostructured optical waveguides in yttrium aluminium garnet and millimetre-long nanopores in sapphire. The approach offers a pathway for transferring concepts from nanophotonics to the fields of solid-state lasers and crystal optics.