Non-imaging metasurface design for collimated beam shaping.

Non-imaging optical lenses can shape the light intensity from incoherent sources to a desired target intensity profile, which is important for applications in lighting, solar light concentration, and optical beam shaping. Their surface curvatures are designed to ensure optimal transfer of energy from the light source to the target. The performance of such lenses is directly linked to their asymmetric freeform surface curvature, which is challenging to manufacture. Metasurfaces can mimic any surface curvature without additional fabrication difficulty by imparting a spatially-dependent phase delay using optical antennas. As a result, metasurfaces are uniquely suited to realize non-imaging optics, but non-imaging design principles have not yet been established for metasurfaces. Here, we take an important step in connecting non-imaging optics and metasurface optics, by presenting a phase-design method for beam shaping based on the concept of optimal transport. We establish a theoretical framework that enables a collimated beam to be redistributed by a metasurface to a desired output intensity profile. The optimal transport formulation leads to metasurface phase profiles that transmit all energy from the incident beam to the output beam, resulting in an efficient beam shaping process. Through a variety of examples, we show that our approach accommodates a diverse range of different input and output intensity profiles. Last but not least, a full field simulation of a metasurface has been done to verify our phase-design framework.

On-Demand Intracellular Delivery of Single Particles in Single Cells by 3D Hollow Nanoelectrodes.

Delivery of molecules into intracellular compartments is one of the fundamental requirements in molecular biology. However, the possibility of delivering a precise number of nano-objects with single-particle resolution is still an open challenge. Here we present an electrophoretic platform based on 3D hollow nanoelectrodes to enable delivery of single nanoparticles into single selected cells and monitoring of the single-particle delivery by surface-enhanced Raman scattering (SERS). The gold-coated hollow nanoelectrode capable of confinement and enhancement of electromagnetic fields upon laser illumination can distinguish the SERS signals of a single nanoparticle flowing through the nanoelectrode. Tight wrapping of cell membranes around the nanoelectrodes allows effective membrane electroporation such that single gold nanorods are delivered on demand into a living cell by electrophoresis. The capability of the 3D hollow nanoelectrodes to porate cells and reveal single emitters from the background in continuous flow is promising for the analysis of both intracellular delivery and sampling.

Isotropically polarized speckle patterns.

The polarization of the light scattered by an optically dense and random solution of dielectric nanoparticles shows peculiar properties when the scatterers exhibit strong electric and magnetic polarizabilities. While the distribution of the scattering intensity in these systems shows the typical irregular speckle patterns, the helicity of the incident light can be fully conserved when the electric and magnetic polarizabilities of the scatterers are equal. We show that the multiple scattering of helical beams by a random dispersion of "dual" dipolar nanospheres leads to a speckle pattern exhibiting a perfect isotropic constant polarization, a situation that could be useful in coherent control of light as well as in lasing in random media.

Correcting vortex splitting in higher order vortex beams.

We demonstrate a general method for the first order compensation of singularity splitting in a vortex beam at a single plane. By superimposing multiple forked holograms on the SLM used to generate the vortex beam, we are able to compensate vortex splitting and generate beams with desired phase singularities of order ℓ = 0, 1, 2, and 3 in one plane. We then extend this method by application of a radial phase, in order to simultaneously compensate the observed vortex splitting at two planes (near and far field) for an ℓ = 2 beam.

Dual and anti-dual modes in dielectric spheres.

We present how the angular momentum of light can play an important role to induce a dual or anti-dual behaviour on a dielectric particle. Although the material the particle is made of is not dual, i.e. a dielectric does not interact with an electrical field in the same way as it does with a magnetic one, a spherical particle can behave as a dual system when the correct excitation beam is chosen. We study the conditions under which this dual or anti-dual behaviour can be induced.

Electromagnetic duality symmetry and helicity conservation for the macroscopic Maxwell's equations.

In this Letter, we show that the electromagnetic duality symmetry, broken in the microscopic Maxwell's equations by the presence of charges, can be restored for the macroscopic Maxwell's equations. The restoration of this symmetry is shown to be independent of the geometry of the problem. These results provide a tool for the study of light-matter interactions within the framework of symmetries and conservation laws. We illustrate its use by determining the helicity content of the natural modes of structures possessing spatial inversion symmetries and by elucidating the root causes for some surprising effects in the scattering off magnetic spheres.

Excitation of single multipolar modes with engineered cylindrically symmetric fields.

We present a new method to address multipolar resonances and to control the scattered field of a spherical scatterer. This method is based on the engineering of the multipolar content of the incident beam. We propose experimentally feasible techniques to generate light beams which contain only a few multipolar modes. The technique uses incident beams with a well defined component of the angular momentum and appropriate focusing with aplanatic lenses. The control of the multipolar content of light beams allow for the excitation of single Mie resonances and unprecedented control of the scattered field from spherical particles.

Vortex Circular Dichroism: An experimental technique to assess the scalar/vectorial regime of diffraction.

Background: In classical electrodynamics, light-matter interactions are modelled using Maxwell equations. The solution of Maxwell equations, which is typically given by means of the electric and magnetic field, is vectorial in nature. Yet it is well known that light-matter interactions can be approximately described in a scalar (polarization independent) way for many optical applications. While the accuracy of the scalar approximation can be theoretically computed, to the best of our knowledge, it has never been determined experimentally. Here, we introduce Vortex Circular Dichroism ( VCD), an optical measurement that has the required features to assess the vectoriality of diffraction. Methods: VCD is measured as the differential transmission (or absorption) of left and right circularly polarized vortex beams. We test the VCD measurement with two different systems: i) an experimental set of single circular nano-apertures drilled in a gold film with diameters ranging from 150 to 1950 nm; and ii) a theoretical set of golden spheres with the same diameters as the nano-apertures. Results: We observe that in both systems, VCD > 0 for smaller diameters, VCD ≲ 0 for intermediate values and VCD ≈ 0 for larger values of the diameter. Furthermore, the simulations show that a diffraction process characterized by a VCD ≈ 0 ( VCD ≠ 0) is polarization-independent (polarization-dependent). As a result, we relate VCD ≠ 0 to a vectorial diffraction, and VCD ≈ 0 to a scalar one. Conclusions: Overall, our results show compelling evidence that it is possible to experimentally assess the scalar/vectorial regime of a diffraction process, and that the VCD technique possesses the required features to measure the vectoriality of diffraction processes involving plasmonic cylindrically symmetric structures.

Two-state switchable plasmonic tweezers for dynamic manipulation of nano-objects.

In this work, we present a plasmonic platform capable of trapping nano-objects in two different spatial configurations. The switch between the two trapping states, localized on the tip and on the outer wall of a vertical gold nanochannel, can be activated by varying the focusing position of the excitation laser along the main axis of the nanotube. We show that the switching of the trapping site is induced by changes in the distribution of the electromagnetic field and of the trapping force. The "inner" and "outer" trapping states are characterized by a static and a dynamic behavior respectively, and their stiffness is measured by analyzing the positions of the trapped specimens as a function of time. In addition, we demonstrate that the stiffness of the static state is high enough to trap particles with diameter as small as 40 nm. These results show a simple, controllable way to generate a switchable two-state trapping regime, which could be used as a model for the study of dynamic trapping or as a mechanism for the development of nanofluidic devices.

Site-selective functionalization of plasmonic nanopores for enhanced fluorescence emission rate and Förster resonance energy transfer.

In this work, we use a site-selective functionalization strategy to decorate plasmonic nanopores with fluorescent dyes. Using an easy and robust fabrication method, we manage to build plasmonic rings on top of dielectric nanotubes with different inner diameters. The modulation of the dimension of the nanopores allows us to tailor their field confinement and their Purcell factor in the visible spectral range. In order to investigate how the changes in geometry influence the fluorescence emission rate efficiency, thiol-conjugated dyes are anchored on the plasmonic ring, thus forming a functional nanopore. We study the lifetime of ATTO 520 and ATTO 590 attached in two different configurations: single dye and FRET pair. For the single dye configuration, we observe that the lifetime of both single dyes decreases as the size of the nanopore is reduced. The smallest nanopores yield an experimental Purcell factor of 6. For the FRET pair configuration, we measure two regimes. For large nanopore sizes, the FRET efficiency remains constant. Whereas for smaller sizes, the FRET efficiency increases from 30 up to 45% with a decrease of the nanopore size. These findings, which have been supported by numerical simulations, may open new perspectives towards energy transfer engineering in plasmonic nanopores with potential applications in photonics and biosensing, in particular in single-molecule detection and sequencing.

A hybrid metal-dielectric zero mode waveguide for enhanced single molecule detection.

We fabricated hybrid metal-dielectric nanoslots and measured their optical response at three different wavelengths. The nanostructure is fabricated on a bilayer film formed by the sequential deposition of silicon and gold on a transparent substrate. The optical characterization is done via fluorescence spectroscopy measurements. We characterized the fluorescence enhancement, as well as the lifetime and the detection volume reduction for each wavelength. We observe that the hybrid metal-dielectric nanoslots behave as enhanced zero mode waveguides in the near-infrared spectral region. Their detection volume is such that they can perform enhanced single-molecule detection at tens of µM. We compared their behavior with that of a golden ZMW, and we demonstrated that the dielectric silicon layer improves both the optical performance and the stability of the device.

Plasmonic zero mode waveguide for highly confined and enhanced fluorescence emission.

We fabricate a plasmonic nanoslot that is capable of performing enhanced single molecule detection at 10 µM concentrations. The nanoslot combines the tiny detection volume of a zero-mode waveguide and the field enhancement of a plasmonic nanohole. The nanoslot is fabricated on a bi-metallic film formed by the sequential deposition of gold and aluminum on a transparent substrate. Simulations of the structure yield an average near-field intensity enhancement of two orders of magnitude at its resonant frequency. Experimentally, we measure the fluorescence stemming from the nanoslot and compare it with that of a standard aluminum zero-mode waveguide. We also compare the detection volume for both structures. We observe that while both structures have a similar detection volume, the nanoslot yields a 25-fold fluorescence enhancement.

Tailoring the chirality of light emission with spherical Si-based antennas.

Chirality of light is of fundamental importance in several enabling technologies with growing applications in life sciences, chemistry and photodetection. Recently, some attention has been focused on chiral quantum emitters. Consequently, optical antennas which are able to tailor the chirality of light emission are needed. Spherical nanoresonators such as colloids are of particular interest to design optical antennas since they can be synthesized at a large scale and they exhibit good optical properties. Here, we show that these colloids can be used to tailor the chirality of a chiral emitter. To this purpose, we derive an analytic formalism to model the interaction between a chiral emitter and a spherical resonator. We then compare the performances of metallic and dielectric spherical antennas to tailor the chirality of light emission. It is seen that, due to their strong electric dipolar response, metallic spherical nanoparticles spoil the chirality of light emission by yielding achiral fields. In contrast, thanks to the combined excitation of electric and magnetic modes, dielectric Si-based particles feature the ability to inhibit or to boost the chirality of light emission. Finally, it is shown that dual modes in dielectric antennas preserve the chirality of light emission.

Far-field measurements of vortex beams interacting with nanoholes.

We measure the far-field intensity of vortex beams going through nanoholes. The process is analyzed in terms of helicity and total angular momentum. It is seen that the total angular momentum is preserved in the process, and helicity is not. We compute the ratio between the two transmitted helicity components, γm,p. We observe that this ratio is highly dependent on the helicity (p) and the angular momentum (m) of the incident vortex beam in consideration. Due to the mirror symmetry of the nanoholes, we are able to relate the transmission properties of vortex beams with a certain helicity and angular momentum, with the ones with opposite helicity and angular momentum. Interestingly, vortex beams enhance the γm,p ratio as compared to those obtained by Gaussian beams.

Fano-like resonance emerging from magnetic and electric plasmon mode coupling in small arrays of gold particles.

In this work we theoretically and experimentally analyze the resonant behavior of individual 3 × 3 gold particle oligomers illuminated under normal and oblique incidence. While this structure hosts both dipolar and quadrupolar electric and magnetic delocalized modes, only dipolar electric and quadrupolar magnetic modes remain at normal incidence. These modes couple into a strongly asymmetric spectral response typical of a Fano-like resonance. In the basis of the coupled mode theory, an analytical representation of the optical extinction in terms of singular functions is used to identify the hybrid modes emerging from the electric and magnetic mode coupling and to interpret the asymmetric line profiles. Especially, we demonstrate that the characteristic Fano line shape results from the spectral interference of a broad hybrid mode with a sharp one. This structure presents a special feature in which the electric field intensity is confined on different lines of the oligomer depending on the illumination wavelength relative to the Fano dip. This Fano-type resonance is experimentally observed performing extinction cross section measurements on arrays of gold nano-disks. The vanishing of the Fano dip when increasing the incidence angle is also experimentally observed in accordance with numerical simulations.

Angular momentum-induced circular dichroism in non-chiral nanostructures.

Circular dichroism, that is, the differential absorption of a system to left and right circularly polarized light, is one of the only techniques capable of providing morphological information of certain samples. In biology, for instance, circular dichroism spectroscopy is widely used to study the structure of proteins. More recently, it has also been used to characterize metamaterials and plasmonic structures. Typically, circular dichorism can only be observed in chiral objects. Here we present experimental results showing that a non-chiral sample such as a subwavelength circular nanoaperture can produce giant circular dichroism when a vortex beam is used to excite it. These measurements can be understood by studying the symmetries of the sample and the total angular momentum that vortex beams carry. Our results show that circular dichroism can provide a wealth of information about the sample when combined with the control of the total angular momentum of the input field.