Raman-enhancing structures include a layer of dielectric material, a superlens configured to focus electromagnetic radiation having a wavelength greater than about 100 nanometers to a two-dimensional focal area having linear dimensions less than about 100 nanometers on a surface of the layer of dielectric material, and at least two nanoparticles comprising a Raman-enhancing material disposed proximate the focal area. Additional Raman-enhancing structures include a layer of dielectric material, a layer of conductive material, and at least two nanoparticles comprising a Raman-enhancing material disposed on a second, opposite surface of the layer of dielectric material. The layer of conductive material has a plurality of apertures therethrough that are arranged in a two-dimensional array. Methods for conducting Raman spectroscopy are performed using such structures and systems.