“…To induce unnatural magnetic dipole (MD) or quadrupole (MQ) resonances, more than three Au NSs need to be closely clustered with a nanometer gap. ,− ,− Herein, as a representative example, we self-assembled a close-packed heptamer, as this cluster can induce strong MD and its interference with ED. ,,− Especially, the bright ED mode can be partially used to induce MQ mode (i.e., Fano resonance); thus, this Fano resonance can be evidenced by scattering spectral dip (i.e., Fano minima). ,,− Meanwhile, Se NSs themselves can excite MD as well as ED without clustering. ,, More importantly, higher-order electric quadrupole (EQ) and MQ can be excited within individual Se NSs. Coupling between fundamental and higher-order modes enables a directional far-field scattering, ,, which can further elucidate the importance of low optical loss in both transmissive and reflective dark-field microscopic studies.…”