Charge-Transfer Plasmon Polaritons at Graphene/α-RuCl(3) Interfaces

[Image: see text] Nanoscale charge control is a key enabling technology in plasmonics, electronic band structure engineering, and the topology of two-dimensional materials. By exploiting the large electron affinity of α-RuCl(3), we are able to visualize and quantify massive charge transfer at graphene/α-RuCl(3) interfaces through generation of charge-transfer plasmon polaritons (CPPs). We performed nanoimaging experiments on graphene/α-RuCl(3) at both ambient and cryogenic temperatures and discovered robust plasmonic features in otherwise ungated and undoped structures. The CPP wavelength evaluated through several distinct imaging modalities offers a high-fidelity measure of the Fermi energy of the graphene layer: E(F) = 0.6 eV (n = 2.7 × 10(13) cm(–2)). Our first-principles calculations link the plasmonic response to the work function difference between graphene and α-RuCl(3) giving rise to CPPs. Our results provide a novel general strategy for generating nanometer-scale plasmonic interfaces without resorting to external contacts or chemical doping.