Orientation-Dependent Handedness of Chiral Plasmons on Nanosphere Dimers: How to Turn a Right Hand into a Left Hand

Optical activity, which is used as a discriminator of chiral enantiomers, is demonstrated to be orientation dependent on individual, and nominally achiral, plasmonic nanosphere dimers. Through measurements of their giant Raman optical activity, we demonstrate that L/R-handed enantiomers can be continuously turned into their R/L-handed mirror images without passing through an achiral state. The primitive uniaxial multipolar response, with demonstrable broken parity and time reversal symmetry, reproduces the observations as resonant Raman scattering on plasmons that carry angular momentum. The analysis underscores that chirality does not have a quantitative continuous measure and recognizes the manipulation of superpositions of multipolar plasmons as a paradigm for novel optical materials with artificial magnetism.