3D-configurated stereoisomers cis-cup-tris[C60>(DPAF-C9)] were found to exhibit photoswitchable dielectric amplification phenomena at GHz frequency. Observation was correlated to photoactivation with plasmonic energy to enhance intramolecular e‒-transfer. Accumulated plasmonic resonance energy was effective to distribute negative charges along the outer C60> fullerosome shell layer of trilayered NPs.