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We report adjusting the charge-transfer-plasmon (CTP) resonances of aluminum (Al) bowties on suspended monolayer graphene via controlled nanofabrication and focused electron-beam irradiation. CTP resonances of bowties with a conductive junction blue-shift with an increase in junction width, whereas their 3λ/2 and λ resonances barely red-shift. These plasmon modes are derived and confirmed by an LC circuit model and electromagnetic simulations performed with boundary-element and frequency-domain methods. A monotonic decay of the CTP lifetime is observed, while the junction width is extended. Instead, the lifetimes of 3λ/2 and λ resonances are nearly independent of junction width. When the junction is shrunk by electron-beam irradiation, all antenna resonances red-shift. Having created an electron-beam-induced sub 5 nm gap in bowties, we monitor the unambiguous transition of a CTP into a bonding-type gap mode, which is highly sensitive to the separation distance. Meanwhile, the 3λ/2 and λ resonances evolve into dipolar bright and dipolar dark modes.

Uncovering the Evolution of Low-Energy Plasmons in Nanopatterned Aluminum Plasmonics on Graphene