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Helical dichroism (HD), based on the interaction between chiral plasmonicnanostructures and light with orbital angular momentum (OAM), has attractedresearchers in a wide range of fields from the viewpoint of fundamental physicsand applications. However, the relation between the HD and the excited plasmonmodes has been poorly understood in experiments. Because of the weak chiralinteraction between the chiral structures and OAM light, the structure size hadto be much larger than the incident light wavelength to obtain a sufficient HDsignal in an experiment, resulting in a complex superposition of higher-orderplasmon modes. Recently, we experimentally demonstrated that a twisted goldnanorod dimer, one of the simplest 3D chiral plasmonic structures, exhibitsgiant circular dichroism due to strong plasmon coupling between the nanorods,followed by the hybridization of dipole mode. In this study, we reveal that theHD of this nanorod dimer appears due to the hybridization of quadrupole plasmonmode rather than dipole mode. Furthermore, the measurement of the HD signal canbe achieved by using the array of the twisted dimers. The dependence of the HDon the incident light wavelength exhibits that the HD sign changes around thequadrupole plasmon resonance, which is in good agreement with the simulation.These results open new avenues for the profound understanding of thelight-matter interaction with respect to angular momentum.

Helical dichroism for hybridized quadrupole plasmon modes in twisted metal nanorods