Two-photon luminescence microscopy of large-area gold nanostructures on templates of anodized aluminum

Using linear reflection spectroscopy and far-field two-photon luminescence (TPL) scanning optical microscopy, we characterize highly enhancing, large-area gold nanostructures formed on porous templates made by anodization of aluminum with either oxalic acid or phosphoric acid. These templates are formed by a newly developed, stepwise technique making use of protective top oxide layers facilitating continuously tunable interpore distances. The upper, porous alumina layers are subsequently removed and the remaining embossed barrier layer is used as template for the sputtered gold, where the density of gold particles covering the sample is adjusted by regulating the sputtering conditions. We observe spatially averaged field intensity enhancement (FE) factors of up to ~5.2⋅102 and bright spots in the TPL-images exhibiting maximum FE factors of up to ~14⋅102 which is the largest estimated FE from any hitherto examined structures with our setup. We relate this large-area massive FE to constructive interference of surface plasmon (SP) polaritons scattered from the densely packed, randomly distributed gold particles and directly correlate this particle density with the strong and broad SP resonances as well as the magnitude of the FE factors. The average FE and the position of high enhancements in the TPL-images are dictated by the excitation wavelength, and the structures could evidently serve as versatile structures facilitating practical molecular sensing.