Optical Synthesis of Transient Chirality in Achiral Plasmonic Metasurfaces

Abstract: As much as chiral metasurfaces are significant in stereochemistry and polarization control, tunable chiroptical response is important for their dynamic counterparts. A single metasurface device with invertible chiral states can selectively harness or manipulate both handedness of circularly polarized light upon demand, where in fact chiral inversion in molecules is an active research field. Tactics for chirality switching can be classified into geometry modification and refractive index tuning. However, these generally confront slow modulation speed or restrained refractive index tuning effects in the visible regime with forbidden 'true' inversion. Here, we reconfigure the 'optical' geometry through inhomogeneous spatiotemporal distribution of hot carriers as a breakthrough, transforming a plasmonic achiral metasurface into an ultrafast transient chiral medium with near-perfectly-invertible handedness in the visible. The photoinduced chirality relaxes through the fast spatial diffusion process of electron temperature compared to electron-phonon relaxation, empowering hot-carrier-based devices to be particularly suitable for ultrafast chiroptics.