Charge-Transfer Plasmon Polaritons at Graphene/α-RuCl3Interfaces

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: EF = 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.
Research at Columbia was supported as part of the Energy Frontier Research Center on Programmable Quantum Materials funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award No. DE-SC0019443. J.Z., L.X., and A.R. were supported by the European Research Council (ERC-2015-AdG694097), the Cluster of Excellence “Advanced Imaging of Matter” (AIM) EXC 2056 - 390715994, funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under RTG 2247, Grupos Consolidados (IT1249-19) and SFB925 “Light induced dynamics and control of correlated quantum systems”. J.Z. acknowledges funding received from the European Union Horizon 2020 research and innovation program under Marie Sklodowska-Curie Grant Agreement 886291 (PeSD-NeSL). J.Z., L.X., and A.R. would like to acknowledge Nicolas Tancogne-Dejean for fruitful discussions and also acknowledge support by the Max Planck Institute-New York City Center for Non-Equilibrium Quantum Phenomena. The Flatiron Institute is a division of the Simons Foundation. D.G.M. acknowledges support from the Gordon and Betty Moore Foundation’s EPiQS Initiative, Grant GBMF9069. Work at ORNL was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan, Grant JPMXP0112101001, JSPS KAKENHI Grant JP20H00354, and the CREST (JPMJCR15F3), JST. S.E.N. was supported by the Division of Scientific User Facilities of the U.S. DOE Basic Energy Sciences. M.M.F. acknowledges support from the Office of Naval Research Grant N00014-18-1-2722. D.N.B. is the Vannevar Bush Faculty ONR-VB: N00014-19-1-2630 and Moore investigator in Quantum Materials EPIQS program #9455. A.S.M acknowledges support from award 80NSSC19K1210 under the NASA Laboratory Analysis of Returned Samples program.