Nanostructured arrays with feature sizes < 100 nm are desirable for a wide variety of applications in the fields of optics and electronics. One limitation of traditional lithographic methods is that such small feature sizes are difficult to cost-effectively pattern at high throughputs. Consequently, it is very important to develop novel strategies for rapidly fabricating three-dimensional nanostructured arrays. True engineering of nanoscale architectures also requires the ability to control the material composition and the structural arrangement which, until now, has been limited.

This thesis demonstrates two new high-throughput methods of three-dimensional nanostructured synthesis. These techniques yield large-area, array-type nanostructures with 2D and 3D periodicities, with feature sizes < 100 nm. Specifically, 2D periodic air-hole arrays and 3D periodic ferroelectric inverse opal films are fabricated.

In the first part of the thesis, 2D periodic, nanoporous arrays were fabricated for the first time using conventional, broad-beam ion implantation of heavy ions through self-organized, nanochannel alumina (NCA) templates. The significant features of this technique are that minimum feature sizes of ~ 40 nm are achievable in a parallel process over a large area (~ cm²) using a non-material specific process, with successful nanoscale patterning achieved in both single crystal InP and SrTiO₃. In addition, this work represents the first study of the selective etch character of amorphous SrTi03. The nanoengineering of complex profiles, including membrane structures, is also demonstrated using this novel technique.

In the second part of the thesis, the first fabrication of 3D periodic, ferroelectric, BaTiO₃ inverse opals, and a simple, adjustable process for the fabrication of large, high-quality, inverse opal ferroelectric films are reported. Highly ordered, ferroelectric, Pb-doped Ba_0.7Sr_0.3TiO₃ (BST) inverse opal films were fabricated by spin-coating a sol-gel precursor into a polystyrene colloidal template followed by heat treatment. The excellent quality of the thin film inverse opal is evident from SEM analysis and the good correspondence between the optical reflectance data and theoretical simulations. Also, for the first time, crack-free, sol-gel derived, inverse opal ferroelectric thin films were fabricated over areas comparable to that of the initial crack-free polystyrene template (~ 100 × 100 μm²).