Chiroptical Response of Aluminum Nanocrescents at Ultraviolet Wavelengths.

Manipulation of plasmon modes at ultraviolet wavelengths using engineered nanophotonic devices allows for the development of high-sensitivity chiroptical spectroscopy systems. We present here an experimental framework based on aluminum-based crescent-shaped nanostructures that exhibit a strong chiroptical response at ultraviolet wavelengths. Through utilization of higher-order plasmon modes in wavelength-scale nanostructures, we address the inherent fabrication challenges in scaling the response to higher frequencies. Additionally, the distinct far-field spectral response types are analyzed within a coupled-oscillator model framework. We find two competing chiroptical response types that contribute toward potential ambiguity in the interpretation of the circular dichroism spectra. The first, optical activity, originates from the interaction between hybridized eigenmodes, whereas the second manifests as a response superficially similar to optical activity but originating instead from differential near-field absorption modes. The study of the chiroptical response from nanoplasmonic devices presented here is expected to aid the development of next-generation chiroptical spectroscopy systems.

Microscopic origin of the chiroptical response of optical media.

The potential for enhancing the optical activity of natural chiral media using engineered nanophotonic components has been central in the quest toward developing next-generation circular-dichroism spectroscopic techniques. Through confinement and manipulation of optical fields at the nanoscale, ultrathin optical elements have enabled a path toward achieving order-of-magnitude enhancements in the chiroptical response. Here, we develop a model framework to describe the underlying physics governing the origin of the chiroptical response in optical media. The model identifies optical activity to originate from electromagnetic coupling to the hybridized eigenstates of a coupled electron-oscillator system, whereas differential absorption of opposite handedness light, though resulting in a far-field chiroptical response, is shown to have incorrectly been identified as optical activity. We validate the model predictions using experimental measurements and show them to also be consistent with observations in the literature. The work provides a generalized framework for the design and study of chiroptical systems.

Aperiodic nanoplasmonic devices for directional colour filtering and sensing.

Exploiting the wave-nature of light in its simplest form, periodic architectures have enabled a panoply of tunable optical devices with the ability to perform useful functions such as filtering, spectroscopy, and multiplexing. Here, we remove the constraint of structural periodicity to enhance, simultaneously, the performance and functionality of passive plasmonic devices operating at optical frequencies. By using a physically intuitive, first-order interference model of plasmon-light interactions, we demonstrate a simple and efficient route towards designing devices with flexible, multi-spectral optical response, fundamentally not achievable using periodic architectures. Leveraging this approach, we experimentally implement ultra-compact directional light-filters and colour-sorters exhibiting angle- or spectrally-tunable optical responses with high contrast, and low spectral or spatial crosstalk. Expanding the potential of aperiodic systems to implement tailored spectral and angular responses, these results hint at promising applications in solar-energy harvesting, optical signal multiplexing, and integrated sensing.