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Abstract

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-RuCl₃, we are able to visualize and quantify massive charge transfer at graphene/α-RuCl₃ interfaces through generation of charge-transfer plasmon polaritons (CPPs). We performed nanoimaging experiments on graphene/α-RuCl₃ 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 × 10¹³ cm^-2). Our first-principles calculations link the plasmonic response to the work function difference between graphene and α-RuCl₃ 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.