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The extension of plasmonics to materials beyond the conventional noble metals opens up a novel and exciting regime after the inspiring discovery of characteristic localized surface plasmon resonances (LSPRs) in doped semiconductor nanocrystals originating from the collective oscillations of free holes in the valence band. We herein prepare colloidal monodisperse eccentric dual plasmonic noble metal-nonstoichiometric copper chalcogenide (Au@Cu2−xSe) hybrid hetero-nanostructures with precisely controlled semiconductor shell size and two tunable LSPRs in both visible (VIS) and near-infrared (NIR) regions associated with Au and Cu2−xSe, respectively. Through systematic evaluations of the photocatalytic performance of Au@Cu2−xSe upon sole NIR and dual VIS + NIR simultaneous excitations, we are capable of unambiguously elucidating the role of plasmonic coupling between two dissimilar building blocks on the accelerated photocatalytic reactions with greater rate constants from both experimental and computational perspectives. The significantly enhanced strength of the electromagnetic field arising from efficient plasmonic coupling under the excitation of two LSPRs results in the superior activities of dual plasmonic Au@Cu2−xSe in photocatalysis. The new physical and chemical insights gained from this work provide the keystone for the rational design and construction of high-quality dual- or even multi-plasmonic nano-systems with optimized properties for widespread applications ranging from photocatalysis to molecular spectroscopies.

Catalytic transformations under light irradiation have been extensively demonstrated by the excitation of the localized surface plasmon resonances (LSPRs) in noble metal-based nanoparticles. To fully harness the potential of noble metal-based nanocatalysts, it is fundamentally imperative to explore hybrid nano-systems with the most desirable enhanced LSPRs and intrinsic catalytic activities. Pd-containing hollow multimetallic nanostructures transformed from the sacrificial template of Ag