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We optimize silicon nano-antennas to enhance and steer the emission of local quantum sources. We combine global evolutionary optimization (EO) with frequency domain electrodynamical simulations, and compare design strategies based on resonant and non-resonant building blocks. Specifically, we investigate the performance of models with different degrees of freedom but comparable amount of available material. We find that simpler geometric models allow significantly faster convergence of the optimizer, which, expectedly, comes at the cost of a reduced optical performance. We finally analyze the physical mechanisms underlying the directional emission that also comes with an emission rate enhancement, and find a surprising robustness against perturbations of the source emitter location. This makes the structures highly interesting for actual nano-fabrication. We believe that optimized, all-dielectric silicon nano-antennas have high potential for genuine breakthroughs in a multitude of applications in nanophotonics and quantum technologies., Comment: 8 pages, 6 figures more...

We investigate - both experimentally and theoretically - the inelastic interaction between fast electrons and the electromagnetic field scattered by metallic apertures and nanostructures on dielectric membranes using photon induced near-field electron microscopy. The experiments - performed in a high brightness ultrafast transmission electron microscope - on gold apertures on silicon nitride membranes reveal strong modulations of the electron-light coupling strength. We demonstrates that this effect results from the combined action of the electric field scattered by the aperture edges and the reflection and transmission of the incident wave by the dielectric membrane. Moreover, when a nanostructure is added inside the metallic aperture, the new scattered field interferes with the previous contributions, thus imprinting the optical response of the nanostructure in additional modulations of the electron-light coupling strength. Using systematic electrodynamics simulations based on the Green dyadic method, we quantitatively analyze these different contributions to the electron-light coupling and propose further applications. more...

The multipole expansion of a nano-photonic structure's electromagnetic response is a versatile tool to interpret optical effects in nano-optics, but it only gives access to the modes that are excited by a specific illumination. In particular the study of various illuminations requires multiple, costly numerical simulations. Here we present a formalism we call "generalized polarizabilities", in which we combine the recently developed exact multipole decomposition [Alaee et al., Opt. Comms. 407, 17-21 (2018)] with the concept of a generalized field propagator. After an initial computation step, our approach allows to instantaneously obtain the exact multipole decomposition for any illumination. Most importantly, since all possible illuminations are included in the generalized polarizabilities, our formalism allows to calculate the total density of multipole modes, regardless of a specific illumination, which is not possible with the conventional multipole expansion. Finally, our approach directly provides the optimum illumination field distributions that maximally couple to specific multipole modes. The formalism will be very useful for various applications in nano-optics like illumination-field engineering, or meta-atom design e.g. for Huygens metasurfaces. We provide a numerical open source implementation compatible with the pyGDM python package., Comment: 13 pages, 6 figures. Includes a supporting information pdf and python examples more...

Using Localized Surface Plasmon Resonance (LSPR) as an optical probe we demonstrate the presence of free carriers in phosphorus doped silicon nanocrystals (SiNCs) embedded in a silica matrix. In small SiNCs, with radius ranging from 2.6 to 5.5 nm, the infrared spectroscopy study coupled to numerical simulations allows us to determine the number of electrically active phosphorus atoms with a precision of a few atoms. We demonstrate that LSP resonances can be supported with only about 10 free electrons per nanocrystal, confirming theoretical predictions and probing the limit of the collective nature of plasmons. We reveal a phenomenon, unique to embedded nanocrystals, with the appearance of an avoided crossing behavior linked to the hybridization between the localized surface plasmon in the doped nanocrystals and the silica matrix phonon modes. Finally, a careful analysis of the scattering time dependence versus carrier density in the small size regime allows us to detect the appearance of a new scattering process at high dopant concentration. more...

Optical interactions have an important impact on the optical response of nanostructures in complex environments. Accounting for interactions in large ensembles of structures requires computationally demanding numerical calculations. In particular if no periodicity can be exploited, full field simulations can become prohibitively expensive. Here we propose a method for the numerical description of aperiodic assemblies of plasmonic nanostructures. Our approach is based on dressed polarizabilities, which are conventionally very expensive to calculate, a problem which we alleviate using a deep convolutional neural network as surrogate model. We demonstrate that the method offers high accuracy with errors in the order of a percent. In cases where the interactions are predominantly short-range, e.g. for out-of-plane illumination of planar metasurfaces, it can be used to describe aperiodic metasurfaces of basically unlimited size, containing many thousands of unordered plasmonic nanostructures. We furthermore show that the model is capable to spectrally resolve coupling effects. The approach is therefore of highest interest for the field of metasurfaces. It provides significant advantages in applications like homogenization of large aperiodic planar metastructures or the design of sophisticated wavefronts at the micrometer scale, where optical interactions play a crucial role., Comment: 13 pages, 8 figures + supporting informations pdf more...

Near- and far-field optical properties of silicon nanostructures under linear polarization (Gaussian beam), and azimuthally or radially focused cylindrical vector beams are investigated by finite-difference time-domain method (FDTD) in Meep open-source software. A python toolkit allowing FDTD simulations in Meep for using those excitation sources is provided. In addition to the preferential excitation of specific electric or magnetic resonance modes as function of the excitation beam polarization, it is shown in the case of spheroids that shape anisotropy affects the resonance wavelength and the dipole orientation of the magnetic or electric dipole mode. For radial or linear polarization, the electric dipole resonance is split by an anapole mode depending on the spheroid symmetry axis with respect to the electric field orientation. Finally, the optical properties in both far-field (scattering pattern) and near-field (electric and magnetic field hot spots) can be tuned by changing the excitation polarization at a fixed wavelength and selecting properly the spheroid shape and dimensions. These numerical simulations can be extended to more complex shapes, or fabrication-friendly nanostructures such as nanocylinders with circular or elliptic sections. more...

pyGDM is a python toolkit for electro-dynamical simulations of individual nano-structures, based on the Green Dyadic Method (GDM). pyGDM uses the concept of a generalized propagator, which allows to solve cost-efficiently monochromatic problems with a large number of varying illumination conditions such as incident angle scans or focused beam raster-scan simulations. We provide an overview of new features added since the initial publication [Wiecha, Computer Physics Communications 233, pp.167-192 (2018)]. The updated version of pyGDM is implemented in pure python, removing the former dependency on fortran-based binaries. In the course of this re-write, the toolkit's internal architecture has been completely redesigned to offer a much wider range of possibilities to the user such as the choice of the dyadic Green's functions describing the environment. A new class of dyads allows to perform 2D simulations of infinitely long nanostructures. While the Green's dyads in pyGDM are based on a quasistatic description for interfaces, we also provide as new external python package pyGDM2_retard a module with retarded Green's tensors for an environment with two interfaces. We have furthermore added functionalities for simulations using fast-electron excitation, namely electron energy loss spectroscopy and cathodoluminescence. Along with several further new tools and improvements, the update includes also the possibility to calculate the magnetic field and the magnetic LDOS inside nanostructures, field-gradients in- and outside a nanoparticle, optical forces or the chirality of nearfields. All new functionalities remain compatible with the evolutionary optimization module of pyGDM for nano-photonics inverse design., Comment: 29 pages, 20 figures more...

Deep learning in the context of nano-photonics is mostly discussed in terms of its potential for inverse design of photonic devices or nanostructures. Many of the recent works on machine-learning inverse design are highly specific, and the drawbacks of the respective approaches are often not immediately clear. In this review we want therefore to provide a critical review on the capabilities of deep learning for inverse design and the progress which has been made so far. We classify the different deep learning-based inverse design approaches at a higher level as well as by the context of their respective applications and critically discuss their strengths and weaknesses. While a significant part of the community's attention lies on nano-photonic inverse design, deep learning has evolved as a tool for a large variety of applications. The second part of the review will focus therefore on machine learning research in nano-photonics "beyond inverse design". This spans from physics informed neural networks for tremendous acceleration of photonics simulations, over sparse data reconstruction, imaging and "knowledge discovery" to experimental applications., Comment: Review article of 18 pages, 7 figures, 4 info-boxes more...

Scanning near-field optical imaging (SNOM) using local active probes provides in general images of the electric part of the photonic local density of states. However, certain atomic clusters can supply more information by simultaneously revealing both the magnetic (m-LDOS) and the electric (e-LDOS) local density of states in the optical range. For example, nanoparticles doped with rare-earth elements like europium or terbium provide both electric dipolar (ED) and magnetic dipolar (MD) transitions. In this theoretical article, we develop a quantum description of active systems (rare earth ions) coupled to a photonic nanostructure, by solving the optical Bloch equations together with Maxwell's equations. This allows us to access the population of the emitting energy levels for all atoms excited by the incident light, degenerated at the extremity of the tip of a near-field optical microscope. We show that it is possible to describe the collected light intensity due to ED and MD transitions in a scanning configuration. By carrying out simulations on different experimentally interesting systems, we demonstrate that our formalism can be of great value for the interpretation of experimental configurations including various external parameters (laser intensity, polarization and wavelength, the SNOM probe size, the nature of the sample ...)., Comment: 10 pages, 8 figures more...

When the sizes of photonic nanoparticles are much smaller than the excitation wavelength, their optical response can be efficiently described with a series of polarizability tensors. Here, we propose a universal method to extract the different components of the response tensors associated with small plasmonic or dielectric particles. We demonstrate that the optical response can be faithfully approximated, as long as the effective dipole is not induced by retardation effects, hence do not depend on the phase of the illumination. We show that the conventional approximation breaks down for a phase-driven dipolar response, such as optical magnetic resonances in dielectric nanostructures. To describe such retardation induced dipole resonances in intermediate-size dielectric nanostructures, we introduce "pseudo-polarizabilities" including first-order phase effects, which we demonstrate at the example of magnetic dipole resonances in dielectric spheres and ellipsoids. Our method paves the way for fast simulations of large and inhomogeneous meta-surfaces., Comment: 13 pages, 11 figures more...

We demonstrate inverse design of plasmonic nanoantennas for directional light scattering. Our method is based on a combination of full-field electrodynamical simulations via the Green dyadic method and evolutionary optimization (EO). Without any initial bias, we find that the geometries reproducibly found by EO, work on the same principles as radio-frequency antennas. We demonstrate the versatility of our approach by designing various directional optical antennas for different scattering problems. EO based nanoantenna design has tremendous potential for a multitude of applications like nano-scale information routing and processing or single-molecule spectroscopy. Furthermore, EO can help to derive general design rules and to identify inherent physical limitations for photonic nanoparticles and metasurfaces., Comment: 13 pages, 9 figures more...

We propose a simple experimental technique to separately map the emission from electric and magnetic dipole transitions close to single dielectric nanostructures, using a few nanometer thin film of rare-earth ion doped clusters. Rare-earth ions provide electric and magnetic dipole transitions of similar magnitude. By recording the photoluminescence from the deposited layer excited by a focused laser beam, we are able to simultaneously map the electric and magnetic emission enhancement on individual nanostructures. In spite of being a diffraction-limited far-field method with a spatial resolution of a few hundred nanometers, our approach appeals by its simplicity and high signal-to-noise ratio. We demonstrate our technique at the example of single silicon nanorods and dimers, in which we find a significant separation of electric and magnetic near-field contributions. Our method paves the way towards the efficient and rapid characterization of the electric and magnetic optical response of complex photonic nanostructures., Comment: 10 pages and 7 figures more...

High refractive index dielectric nanostructures provide original optical properties thanks to the occurrence of size- and shape-dependent optical resonance modes. These modes commonly present a spectral overlap of broad, low-order modes (\textit{e.g}. dipolar modes) and much narrower, higher-order modes. The latter are usually characterized by a rapidly varying frequency-dependent phase, which - in superposition with the lower order mode of approximately constant phase - leads to typical spectral features known as Fano resonances. Interestingly, such Fano resonances occur in dielectric nanostructures of the simplest shapes. In spheroidal nanoparticles, interference between broad magnetic dipole and narrower electric dipole modes can be observed. In high aspect-ratio structures like nanowires, either the electric or the magnetic dipolar mode (depending on the illumination conditions) interferes with higher order multipole contributions of the same nature (electric or magnetic). Using the analytical Mie theory, we analyze the occurrence of Fano resonances in high-index dielectric nanowires and discuss their consequences like unidirectional scattering. By means of numerical simulations, we furthermore study the impact on those Fano resonances of the shape of the nanowire cross-sections as well as the coupling of two parallel nanowires. The presented results show that all-dielectric nanostructures, even of simple shapes, provide a reliable low-loss alternative to plasmonic nanoantennas., Comment: 30 pages, 8 figures. To appear as a chapter in the book "Fano resonances in optics and microwaves: Physics and application", Springer (2018). Ed. by E. O. Kamenetskii, A. Sadreev, and A. Miroshnichenko more...

We report on the development of an ultrafast Transmission Electron Microscope based on a cold field emission source which can operate in either DC or ultrafast mode. Electron emission from a tungsten nanotip is triggered by femtosecond laser pulses which are tightly focused by optical components integrated inside a cold field emission source close to the cathode. The properties of the electron probe (brightness, angular current density, stability) are quantitatively determined. The measured brightness is the largest reported so far for UTEMs. Examples of imaging, diffraction and spectroscopy using ultrashort electron pulses are given. Finally, the potential of this instrument is illustrated by performing electron holography in the off-axis configuration using ultrashort electron pulses., Comment: 23 pages, 9 figures more...

In this article, we propose a concise theoretical framework based on mixed field-susceptibilities to describe the decay of magnetic dipoles induced by non--magnetic nanostructures. This approach is first illustrated in simple cases in which analytical expressions of the decay rate can be obtained. We then show that a more refined numerical implementation of this formalism involving a volume discretization and the computation of a generalized propagator can predict the dynamics of magnetic dipoles in the vicinity of nanostructures of arbitrary geometries. We finally demonstrate the versatility of this numerical method by coupling it to an evolutionary optimization algorithm. In this way we predict a structure geometry which maximally promotes the decay of magnetic transitions with respect to electric emitters., Comment: 8 pages, 5 figures. Separate supporting informations of 12 pages and 13 figures more...

Aluminum nanostructures have recently been at the focus of numerous studies due to their properties including oxidation stability and surface plasmon resonances covering the ultraviolet and visible spectral windows. In this article, we reveal a new facet of this metal relevant for both plasmonics purpose and photo-thermal conversion. The field distribution of high order plasmonic resonances existing in two-dimensional Al structures is studied by nonlinear photoluminescence (nPL) microscopy in a spectral region where electronic interband transitions occur. The polarization sensitivity of the field intensity maps shows that the electric field concentration can be addressed and controlled on-demand. We use a numerical tool based on the Green dyadic method to analyze our results and to simulate the absorbed energy that is locally converted into heat. The polarization-dependent temperature increase of the Al structures is experimentally quantitatively measured, and is in an excellent agreement with theoretical predictions. Our work highlights Al as a promising candidate for designing thermal nanosources integrated in coplanar geometries for thermally assisted nanomanipulation or biophysical applications., Comment: 8 pages 6 figures main article; 7 pages 9 figures supporting informations more...

It has been experimentally demonstrated only recently that a simultaneous excitation of interfering electric and magnetic resonances can lead to uni-directional scattering of visible light in zero-dimensional dielectric nanoparticles. We show both theoretically and experimentally, that strongly anisotropic scattering also occurs in individual dielectric nanowires. The effect occurs even under either pure transverse electric or pure transverse magnetic polarized normal illumination. This allows for instance to toggle the scattering direction by a simple rotation of the incident polarization. Finally, we demonstrate that directional scattering is not limited to cylindrical cross-sections, but can be further tailored by varying the shape of the nanowires., Comment: 12 pages, 6 figures + supporting informations of 12 pages, 19 figures more...

We report about the experimental observation and characterization of nonlinear optical properties of individual silicon nanowires of different dimensions. Our results show that the nonlinear light has different components, one of them corresponding to the second harmonic generation (SHG). The SHG strongly depends on the polarization of the optical excitation and nanowire diameter, and gives access to the local electromagnetic field intensity distribution. Furthermore, we show that the second harmonic, when observed, is enhanced compared to bulk silicon and is sensitive to optical resonances supported by the nanowires. This offers different perspectives on the definition of silicon-based nonlinear photonic devices., Comment: 5 pages, 5 figures + 3 pages supplemental material including 3 additional figures more...

The rational design of photonic nanostructures consists in anticipating their optical response from simple models or as variations of reference systems. This strategy is limited when different objectives are simultaneously targeted. Inspired from biology, evolutionary approaches drive the morphology of a nano-object towards an optimum through several cycles of selection, mutation and cross-over, mimicking the process of natural selection. However, their extension to scenarii with multiple objectives demands efficient computational schemes. We present a numerical technique to design photonic nanostructures with optical properties optimized along several arbitrary objectives. This combination of evolutionary multi-objective algorithms with frequency-domain electro-dynamical simulations is used to design silicon nanostructures resonant at user-defined, polarization-dependent wavelengths. The spectra of pixels fabricated by electron beam lithography following the optimized design show excellent agreement with the targeted objectives. The method is self-adaptive to arbitrary constraints, and therefore particularly interesting for the design of complex structures within technological limits., Comment: 10 pages, 6 figures + 10 pages of supporting informations including 17 additional figures more...

We investigate Second Harmonic Generation from individual silicon nanowires and study the influence of resonant optical modes on the far-field nonlinear emission. We find that the polarization of the Second Harmonic has a size-dependent behavior and explain this phenomenon by a combination of different surface and bulk nonlinear susceptibility contributions. We show that the Second Harmonic Generation has an entirely different origin, depending on whether the incident illumination is polarized parallel or perpendicularly to the nanowire axis. The results open perspectives for further geometry-based studies on the origin of Second Harmonic Generation in nanostructures of high-index centrosymmetric semiconductors., Comment: 7 Pages, 4 Figures + 3 Pages, 6 Figures in Appendix more...

Self-assembled Plasmonic Nanoparticle Networks (PNN) composed of chains of 12-nm diameter crystalline gold nanoparticles exhibit a longitudinally coupled plasmon mode cen- tered at 700 nm. We have exploited this longitudinal absorption band to efficiently confine light fields and concentrate heat sources in the close vicinity of these plasmonic chain net- works. The mapping of the two phenomena on the same superstructures was performed by combining two-photon luminescence (TPL) and fluorescence polarization anisotropy (FPA) imaging techniques. Besides the light and heat concentration, we show experimentally that the planar spatial distribution of optical field intensity can be simply modulated by controlling the linear polarization of the incident optical excitation. On the contrary, the heat production, which is obtained here by exciting the structures within the optically transparent window of biological tissues, is evenly spread over the entire PNN. This contrasts with the usual case of localized heating in continuous nanowires, thus opening opportunities for these networks in light-induced hyperthermia applications. Furthermore, we propose a unified theoretical framework to account for both the non-linear optical and thermal near-fields around PNN. The associated numerical simulations, based on a Green s function formalism, are in excellent agreement with the experimental images. This formalism therefore provides a versatile tool for the accurate engineering of optical and thermodynamical properties of complex plasmonic colloidal architectures. more...