The Role of Electron Transfer in the Nonlinear Response of Ge₂Sb₂Te₅-Mediated Plasmonic Dimers

Here, we study the possibility of exquisitely selective harmonic generation based on the concept of charge transfer plasmons (CTPs) in bridged nanoparticle assemblies. By choosing plasmonic dimer nanoantenna, as a fundamental member of the nanocluster family, and bridging the capacitive gap space between the proximal nanoparticles with an optothermally controllable substance, we judiciously showed that variations in the generation of third harmonic light in the visible regime can be possible by considering distinct states of the functional bridge. To this end, the conductive connection between the nanoparticles is mediated with Ge₂Sb₂Te₅ (GST) with inherently opposite optical and electrical properties below (dielectric, amorphous state) and above 477 °C (conductive, crystalline state). This helped to actively control the transition of charges across the bridge and thereby control the excitation of CTP resonances and provide a switching feature between dipolar and CTP modes. This versatile approach also allowed for production of the intended harmonic signal at different wavelengths depending on the conductivity of the interparticle nanojunction.