Shrinking-hole colloidal lithography: self-aligned nanofabrication of complex plasmonic nanoantennas

Plasmonic nanoantennas create locally strongly enhanced electric fields in so-called hot spots. To place a relevant nanoobject with high accuracy in such a hot spot is crucial to fully capitalize on the potential of nanoantennas to control, detect, and enhance processes at the nanoscale. With state-of-the-art nanofabrication, in particular when several materials are to be used, small gaps between antenna elements are sought, and large surface areas are to be patterned, this is a grand challenge. Here we introduce self-aligned, bottom-up and self-assembly based Shrinking-Hole Colloidal Lithography, which provides (i) unique control of the size and position of subsequently deposited particles forming the nanoantenna itself, and (ii) allows delivery of nanoobjects consisting of a material of choice to the antenna hot spot, all in a single lithography step and, if desired, uniformly covering several square centimeters of surface. We illustrate the functionality of SHCL nanoantenna arrangements by (i) an optical hydrogen sensor exploiting the polarization dependent sensitivity of an Au-Pd nanoantenna ensemble; and (ii) single particle hydrogen sensing with an Au dimer nanoantenna with a small Pd nanoparticle in the hot spot.