Plasmonic nanosystems and metamaterials have recently attracted considerable attention because of their ability to enhance the light–matter interactions. One of such optical phenomena is the chiral‐ or handedness‐dependent response which typically requires 3D samples. Planar structures that can exhibit chiral response are highly desirable because of their facile fabrication, however fundamental challenges arising from the 2D nature of these systems prevent the generation of strong chiro‐optical effects. In this work, giant enhancement of the handedness‐dependent optical response in planar metallic nanostructures is shown by exploring the hybridization of plasmonic–photonic modes in a chiral metasurface. The resulting planar hybrid metasurface exhibits over an order of magnitude difference in nonlinear optical response when illuminated with excitation light of opposite circular polarizations. The unique properties of the hybridized plasmonic–photonic modes are shown to be responsible for the giant chiral nonlinear response. This platform allows to study the fundamental framework of chiral optical effects that arise from the combination of planar chirality and collective interaction of discrete nanosystems.
Designing broadband enhanced chirality is of strong interest to the emerging fields of chiral chemistry and sensing, or to control the spin orbital momentum of photons in recently introduced nanophotonic chiral quantum and classical optical applications. However, chiral light‐matter interactions have an extremely weak nature, are difficult to control and enhance, and cannot be made tunable or broadband. In addition, planar ultrathin nanophotonic structures to achieve strong, broadband, and tunable chirality at the technologically important visible to ultraviolet spectrum still remain elusive. Here, these important problems are tackled by experimentally demonstrating and theoretically verifying spectrally tunable, extremely large, and broadband chiroptical response by nanohelical metamaterials. The reported new designs of all‐dielectric and dielectric‐metallic (hybrid) plasmonic metamaterials permit the largest and broadest ever measured chiral Kuhn's dissymmetry factor achieved by a large‐scale nanophotonic structure. In addition, the strong circular dichroism of the presented bottom‐up fabricated optical metamaterials can be tuned by varying their dimensions and proportions between their dielectric and plasmonic helical subsections. The currently demonstrated ultrathin optical metamaterials are expected to provide a substantial boost to the developing field of chiroptics leading to significantly enhanced and broadband chiral light‐matter interactions at the nanoscale.
more » « less- Award ID(s):
- 1808715
- NSF-PAR ID:
- 10452315
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Functional Materials
- Volume:
- 31
- Issue:
- 20
- ISSN:
- 1616-301X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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