Using a series of highly regular nanostructures consisting of periodic Ag nanowires fabricated in porous aluminum oxide, we validate the overwhelmingly plasmonic origin of the most intense SERS signals such as those responsible for single-molecule SERS, demonstrating its sensitive dependence on the system's nanogeometry. By varying the interwire gap distance from 35 to 10 nm, the SERS intensity excited with 785 nm laser light, increased over 200-fold. These observations were shown to agree quantitatively with electromagnetic field calculations carried out using the free space green's tensor method.

Achieving larger electromagnetic enhancement using a nanogap between neighboring metallic nanostructures has been long pursued for boosting light–matter interactions. However, the quantitative probing of this enhancement is hindered by the lack of a reliable experimental method for measuring the local fields within a subnanometer gap. Here, we use layered MoS2 as a two-dimensional atomic crystal probe in nanoparticle-on-mirror nanoantennas to measure the plasmonic enhancement in the gap by quantitative surface-enhanced Raman scattering. Our designs ensure that the probe filled in the gap has a well-defined lattice orientation and thickness, enabling independent extraction of the anisotropic field enhancements. We find that the field enhancement can be safely described by pure classical electromagnetic theory when the gap distance is no <1.24 nm. For a 0.62 nm gap, the probable emergence of quantum mechanical effects renders an average electric field enhancement of 114-fold, 38.4% lower than classical predictions.

Polarization optics plays a pivotal role in diffractive, refractive, and emerging flat optics, and has been widely employed in contemporary optical industries and daily life. Advanced polarization manipulation leads to robust control of the polarization direction of light. Nevertheless, polarization control has been studied largely independent of the phase or intensity of light. Here, we propose and experimentally validate a Malus-metasurface-assisted paradigm to enable simultaneous and independent control of the intensity and phase properties of light simply by polarization modulation. The orientation degeneracy of the classical Malus's law implies a new degree of freedom and enables us to establish a one-to-many mapping strategy for designing anisotropic plasmonic nanostructures to engineer the Pancharatnam-Berry phase profile, while keeping the continuous intensity modulation unchanged. The proposed Malus metadevice can thus generate a near-field greyscale pattern, and project an independent far-field holographic image using an ultrathin and single-sized metasurface. This concept opens up distinct dimensions for conventional polarization optics, which allows one to merge the functionality of phase manipulation into an amplitudemanipulation-assisted optical component to form a multifunctional nano-optical device without increasing the complexity of the nanostructures. It can empower advanced applications in information multiplexing and encryption, anti-counterfeiting, dual-channel display for virtual/augmented reality, and many other related fields.