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Ambipolar charge-transfer graphene plasmonic cavities


Plasmon polaritons in van der Waals materials hold promise for various photonics applications1,2,3,4. The deterministic imprinting of spatial patterns of high carrier density in plasmonic cavities and nanoscale circuitry can enable the realization of advanced nonlinear nanophotonic5 and strong light–matter interaction platforms6. Here we demonstrate an oxidation-activated charge transfer strategy to program ambipolar low-loss graphene plasmonic structures. By covering graphene with transition-metal dichalcogenides and subsequently oxidizing the transition-metal dichalcogenides into transition-metal oxides, we activate charge transfer rooted in the dissimilar work functions between transition-metal oxides and graphene. Nano-infrared imaging reveals ambipolar low-loss plasmon polaritons at the transition-metal-oxide/graphene interfaces. Further, by inserting dielectric van der Waals spacers, we can precisely control the electron and hole densities induced by oxidation-activated charge transfer and achieve plasmons with a near-intrinsic quality factor. Using this strategy, we imprint plasmonic cavities with laterally abrupt doping profiles with nanoscale precision and demonstrate plasmonic whispering-gallery resonators based on suspended graphene encapsulated in transition-metal oxides.

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Fig. 1: OCT for on-demand graphene plasmonics.
Fig. 2: Achieving reconfigurable ambipolar carrier density and high plasmonic quality factor in van der Waals OCT structures.
Fig. 3: Nano-imprinting graphene plasmonic cavities via programmable OCT.
Fig. 4: Whispering-gallery modes in suspended graphene plasmonic cavities encapsulated in WOx.

Data availability

The data that support the findings within this paper are available from the corresponding authors upon reasonable request.


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Research on nanophotonic devices is solely supported as part of Programmable Quantum Materials, an Energy Frontier Research Center funded by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under award DE-SC0019443. Research on charge-transfer interfaces is supported by DOE-BES under award DE-SC0018426. D.N.B. is Moore Investigator in Quantum Materials (EPIQS, GBMF9455) and Vannevar Bush Faculty Fellow (ONR-VB, N00014-19-1-2630).

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Authors and Affiliations



B.S.Y.K., J.C.H. and D.N.B. conceived the project and designed the experiments. B.S.Y.K. and M.S.C. fabricated the devices with assistance from T.S.C., A.R., A.N. and S.H.C.; B.S.Y.K. and A.J.S. performed measurements with assistance from A.S.M., L.X. and Y.D.; and S.L. grew the WSe2 crystals. Z.S. performed the graphene plasmon scattering rate and Fano resonance simulations. B.S.Y.K. performed the full-wave eigenmode simulations with assistance from F.L.R. and A.S.M.; B.S.Y.K. and Y.S. performed the Kelvin probe force microscopy measurements. A.Z. performed the cross-sectional transmission electron microscopy measurements. X.X., A.J.M., P.J.S., C.R.D., J.C.H. and D.N.B. supervised the project. B.S.Y.K. analysed the data. B.S.Y.K. and D.N.B. cowrote the paper with input from all authors.

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Correspondence to Brian S. Y. Kim or D. N. Basov.

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Nature Materials thanks Alexey Nikitin and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–23 and Discussion Sections 1–4.

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Kim, B.S.Y., Sternbach, A.J., Choi, M.S. et al. Ambipolar charge-transfer graphene plasmonic cavities. Nat. Mater. 22, 838–843 (2023).

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