A NERS-active structure includes a deformable, active nanoparticle support structure for supporting a first nanoparticle and a second nanoparticle that is disposed proximate the first nanoparticle. The nanoparticles each comprise a NERS-active material. The deformable, active nanoparticle support structure is configured to vary the distance between the first nanoparticle and the second nanoparticle while performing NERS. Various active nanoparticle support structures are disclosed. A NERS system includes such a NERS-active structure, a radiation source for generating radiation scatterable by an analyte located proximate the NERS-active structure, and a radiation detector for detecting Raman scattered radiation scattered by the analyte. A method for performing NERS includes providing such a NERS-active structure, providing an analyte at a location proximate the NERS-active structure, irradiating the NERS-active structure and the analyte with radiation, varying the distance between the nanoparticles, and detecting Raman scattered radiation scattered by the analyte.