Chiral Light Emission from a Sphere Revealed by Nanoscale Relative Phase Mapping

Circularly polarized light (CPL) is currently receiving much attention as a key ingredient for next-generation information technologies, such as quantum communication and encryption. CPL photon generation for such applications is commonly realized by coupling achiral optical quantum emitters to chiral nanoantennas. Here, we explore a different strategy consisting in exciting a nanosphere -- the ultimate symmetric structure -- to produce all-directional CPL emission. Specifically, we demonstrate chiral emission from a silicon nanosphere induced by an electron beam based on two different strategies: dissolving the degeneracy of orthogonal dipole modes, and interference of electric and magnetic modes. We prove these concepts by visualizing the phase and polarization using a newly developed polarimetric four-dimensional cathodoluminescence method. Besides their fundamental interest, our results support the use of free-electron-induced light emission from spherically symmetric systems as a versatile platform for the generation of chiral light with on-demand control over the phase and degree of polarization

Simultaneous nanoscale excitation and emission mapping by cathodoluminescence

Free-electron-based spectroscopies can reveal the nanoscale optical properties of semiconductor materials and nanophotonic devices with a spatial resolution far beyond the diffraction limit of light. However, the retrieved spatial information is constrained to the excitation space defined by the electron beam position, while information on the delocalization associated with the spatial extension of the probed optical modes in the specimen has so far been missing, despite its relevance in ruling the optical properties of nanostructures. In this study, we demonstrate a cathodoluminescence method that can access both excitation and emission spaces at the nanoscale, illustrating the power of such simultaneous excitation and emission mapping technique by revealing a sub-wavelength emission position modulation as well as by visualizing electromagnetic energy transport in nanoplasmonic systems. Besides the fundamental interest of these results, our technique grants us access into previously inaccessible nanoscale optical properties

Surface plasmon resonance sensing with thin films of palladium and platinum - quantitative and real-time analysis

Surface plasmon resonance (SPR) is a highly useful technique in biology and is gradually becoming useful also for materials science. However, measurements to date have been performed almost exclusively on gold, which limits the possibility to probe chemical modifications of other metals. In this work we show that 20 nm Pd and Pt films work "fairly well" for quantitative SPR sensing of organic films despite the high light absorption. In the interval between total reflection and the SPR angle, high intensity changes occur when a film is formed on the surface. Fresnel models accurately describe the full angular spectra and our data analysis provides good resolution of surface coverage in air (a few ng cm(-2)). Overall, the Pd sensors behave quite similarly to 50 nm gold in terms of sensitivity and field extension, although the noise level in real-time measurements is similar to 5 times higher. The Pt sensors exhibit a longer extension of the evanescent field and similar to 10 times higher noise compared to gold. Yet, formation of organic layers a few nm in thickness can still be monitored in real-time. As a model system, we use thiolated poly(ethylene glycol) to make Pd and Pt protein repelling. Our findings show how SPR can be used for studying chemical modifications of two metals that are important in several contexts, for instance within heterogeneous catalysis. We emphasize the advantages of simple sample preparation and accurate quantitative analysis in the planar geometry by Fresnel models

Optical sensing and determination of complex reflection coefficients of plasmonic structures using transmission interferometric plasmonic sensor

The combination of interferometry and plasmonic structure, which consists of gold nanoparticle layer, sputter coated silicon oxide spacer layer, and aluminum mirror layer, was studied in transmission mode for biosensing and refractive index sensing applications. Because of the interferometric nature of the system, the information of the reflection amplitude and phase of the plasmonic layer can be deduced from one spectrum. The modulation amplitude in the transmission spectrum, caused by the interference between the plasmonic particle layer and the mirror layer, increases upon the refractive index increase around the plasmonic particles due to their coherent backscattering property. Our proposed evaluation method requires only two light sources with different wavelengths for a stable self-referenced signal, which can be easily and precisely tuned by a transparent spacer layer thickness. Unlike the standard localized surface plasmon sensors, where a sharp resonance peak is essential, a broad band plasmon resonance is accepted in this method. This leads to large fabrication tolerance of the plasmonic structures. We investigated bulk and adsorption layer sensitivities both experimentally and by simulation. The highest sensitivity wavelength corresponded to the resonance of the plasmonic particles, but useful signals are produced in a much broader spectral range. Analysis of a single transmission spectrum allowed us to access the wavelength-dependent complex reflection coefficient of the plasmonic particle layer, which confirmed the reflection amplitude increase in the plasmonic particle layer upon molecular adsorption