RESUMEN
Chiral plasmonic nanostructures possess a chiroptical response orders of magnitude stronger than that of natural biomolecular systems, making them highly promising for a wide range of biochemical, medical, and physical applications. Despite extensive efforts to artificially create and tune the chiroptical properties of chiral nanostructures through compositional and geometrical modifications, a fundamental understanding of their underlying mechanisms remains limited. In this study, we present a comprehensive investigation of individual gold nanohelices by using advanced analytical electron microscopy techniques. Our results, as determined by angle-resolved cathodoluminescence polarimetry measurements, reveal a strong correlation between the circular polarization state of the emitted far-field radiation and the handedness of the chiral nanostructure in terms of both its dominant circularity and directional intensity distribution. Further analyses, including electron energy-loss measurements and numerical simulations, demonstrate that this correlation is driven by longitudinal plasmonic modes that oscillate along the helical windings, much like straight nanorods of equal strength and length. However, due to the three-dimensional shape of the structures, these longitudinal modes induce dipolar transverse modes with charge oscillations along the short axis of the helices for certain resonance energies. Their radiative decay leads to observed emission in the visible range. Our findings provide insight into the radiative properties and underlying mechanisms of chiral plasmonic nanostructures and enable their future development and application in a wide range of fields, such as nano-optics, metamaterials, molecular physics, biochemistry, and, most promising, chiral sensing via plasmonically enhanced chiral optical spectroscopy techniques.
RESUMEN
The study of spin-orbit coupling (SOC) of light is crucial to explore the light-matter interactions in sub-wavelength structures. By designing a plasmonic lattice with chiral configuration that provides parallel angular momentum and spin components, one can trigger the strength of the SOC phenomena in photonic or plasmonic crystals. Herein, we explore the SOC in a plasmonic crystal, both theoretically and experimentally. Cathodoluminescence (CL) spectroscopy combined with the numerically calculated photonic band structure reveals an energy band splitting that is ascribed to the peculiar spin-orbit interaction of light in the proposed plasmonic crystal. Moreover, we exploit angle-resolved CL and dark-field polarimetry to demonstrate circular-polarization-dependent scattering of surface plasmon waves interacting with the plasmonic crystal. This further confirms that the scattering direction of a given polarization is determined by the transverse spin angular momentum inherently carried by the SP wave, which is in turn locked to the direction of SP propagation. We further propose an interaction Hamiltonian based on axion electrodynamics that underpins the degeneracy breaking of the surface plasmons due to the spin-orbit interaction of light. Our study gives insight into the design of novel plasmonic devices with polarization-dependent directionality of the Bloch plasmons. We expect spin-orbit interactions in plasmonics will find much more scientific interests and potential applications with the continuous development of nanofabrication methodologies and uncovering new aspects of spin-orbit interactions.
RESUMEN
Strong electron-light interactions supported by the surface plasmon polaritons excited in metallic thin films can lead to faster optoelectronic devices. Merging surface polaritons with photonic crystals leads to the formation of Bloch plasmons, allowing for the molding of the flow of polaritons and the controlling of the optical density of states for even stronger electron-light interactions. Here, we use a two-dimensional square lattice of holes incorporated inside a plasmonic gold layer to investigate the interaction of surface plasmon polaritons with the square lattice and the formation of plasmonic Bloch modes. Cathodoluminescence spectroscopy and hyperspectral imaging are used for imaging the spatio-spectral near-field distribution of the optical Bloch modes in the visible to near infrared spectral ranges. In addition, the higher-order Brillouin zones of the plasmonic lattice are demonstrated by using angle-resolved cathodoluminescence mapping. We further complement our experimental results with numerical simulations of the optical modes supported by the plasmonic lattice that helps to better resolve the superposition of the various modes excited by the electron beam. Next to previous works in this context, our results thus place cathodoluminescence scanning spectroscopy and angle-resolved mapping as complementary techniques to uncover the spatio-spectral distribution of optical Bloch modes in real and reciprocal spaces.
