arXiv subjects

Joseph Zyss

Publications and source records attributed to Joseph Zyss.

14 recordsLinked to original sources

arXiv2025

Plasmonic Metasurfaces with Structural Chirality and Pseudo-Chirality for Enhanced Circular Dichroism and Enantiomeric Recognition

We present the design and optical characterization of a plasmonic metasurface engineered to exhibit strong polarization anisotropy under both linearly and circularly polarized light. The metasurface consists of geometrically asymmetric gold nanostructures arranged periodically on a glass substrate. Each nanostructure is formed by the fusion of three equilateral triangles. The nanostructures simultaneously break mirror and inversion symmetries, resulting in chiral and pseudo-chiral optical responses that manifest as linear and circular polarization-dependent spectral features. Our numerical and experimental results reveal clear chiroptical effects in both near- and far-field. Near-field scanning optical microscopy confirms the excitation of polarization-selective localized plasmonic modes, with spatially distinct hot-spots lighting up under different incident polarizations. Furthermore, we demonstrate that the metasurface exhibits a measurable enantiospecific optical response when coated with thin left- or right-handed chiral overlayers. The differential circular dichroism signals observed in the presence of opposite enantiomers highlight the potential of the metasurface for label-free chiral sensing. These findings provide new insights into the interplay between structural anisotropy, pseudo-chirality, and enantioselective interactions in planar plasmonic systems. Our findings highlight the ability of planar metasurfaces to emulate chiral optical behavior without requiring volumetric 3D structures.

physics.optics↗

arXiv2023

Interplay of gain and loss in arrays of nonlinear plasmonic nanoparticles: toward parametric downconversion and amplification

With the help of a theoretical model and finite-difference-time-domain simulations based on the hydrodynamic-Maxwell model, we examine the effect of difference frequency generation in an array of L-shaped metal nano-particles characterized by intrinsic plasmonic nonlinearity. The outcomes of the calculations reveal the spectral interplay of the gain and loss in the vicinity of the fundamental frequency of the localized surface-plasmon resonances. Subsequently, we identify different array depths and pumping regimes facilitating parametric amplification and parametric down-conversion. Our results suggest that the parametric amplification regime becomes feasible on a scale of hundreds of nanometers and parametric downconversion on the scale of tens of nanometers, opening up new exciting opportunities for developing building blocks of photonic metasurfaces.

physics.optics↗

arXiv2021

Möbius Strip Microlasers: a Testbed for Non-Euclidean Photonics

We report on experiments with Möbius strip microlasers which were fabricated with high optical quality by direct laser writing. A Möbius strip, i.e., a band with a half twist, exhibits the fascinating property that it has a single nonorientable surface and a single boundary. We provide evidence that, in contrast to conventional ring or disk resonators, a Möbius strip cavity cannot sustain whispering gallery modes (WGM). Comparison between experiments and 3D finite difference time domain (FDTD) simulations reveals that the resonances are localized on periodic geodesics.

physics.optics↗

arXiv2021

Second harmonic generation by strongly coupled exciton-plasmons: the role of polaritonic states in nonlinear dynamics

We investigate second harmonic generation (SHG) from hexagonal periodic arrays of triangular nano-holes of aluminum using a self-consistent methodology based on the hydrodynamics-Maxwell-Bloch approach. It is shown that angular polarization patterns of the far-field second harmonic response abide to three-fold symmetry constraints on tensors. When a molecular layer is added to the system and its parameters are adjusted to achieve the strong coupling regime between a localized plasmon mode and molecular excitons, Rabi splitting is observed from occurrence of both single- and two-photon transition peaks within the SHG power spectrum. It is argued that the splitting observed for both transitions results from direct transitions between lower and upper polaritonic states of the strongly coupled system. This interpretation can be accounted by a tailored three-level quantum model, with results in agreement with the unbiased numerical approach. Our results suggest the hybrid states formed in strongly coupled systems directly contribute to the nonlinear dynamics. This opens new directions in designing THz sources and nonlinear frequency converters.

physics.optics↗

arXiv2020

Nanoscale ordering of planar octupolar molecules for nonlinear optics at higher temperatures

We develop scenarios for orientational ordering of an in-plane system of small flat octupolar molecules at the low-concentration limit, aiming towards nonlinear-optical (NLO) applications at room temperatures. The octupoles interact with external electric poling fields and intermolecular interactions are neglected. Simple statistical-mechanics models are used to analyze the orientational order in the very weak poling limit, sufficient for retrieving the NLO signals owing to the high sensitivity of NLO detectors and measurement chains. Two scenarios are discussed. Firstly, the octupolar poling field is imparted by a system of point charges; the setup is subject to cell-related constraints imposed by mechanical strength and dielectric breakdown limit. The very weak octupolar order of benchmarking TATB molecules is shown to emerge at Helium temperatures. The second scenario addresses the dipoling of octupolar molecules with a small admixture of electric dipolar component. It requires a strong field regime to become effective at Nitrogen temperature range. An estimation of the nonlinear susceptibility coefficient matrix for both scenarios is done in the high-temperature (weak interaction) limit formalism. We argue that moderate modifications of the system like, e.g., an increase of the size of the octupole, accompanied by dipole-assisted octupoling, can increase the poling temperature above Nitrogen temperatures.

physics.optics↗

arXiv2014

Vertically coupled polymer microracetrack resonators for Label-Free Biochemical sensors

We report on the efficient design and fabrication of polymeric microracetrack optical resonators for label-free biosensing purposes. Vertically-coupled microresonators immersed in deionised water display high Q-factors (>35000) and finesses up to 25. A surface sensing experiment performed with these microresonators using 5-TAMRA cadaverine as a test molecule demonstrated both the high sensitivity and low detection limit of our device.

physics.optics↗

arXiv2014

Three-Dimensional Organic Microlasers with Low Lasing Thresholds Fabricated by Multiphoton Lithography

Cuboid-shaped organic microcavities containing a pyrromethene laser dye and supported upon a photonic crystal have been investigated as an approach to reducing the lasing threshold of the cavities. Multiphoton lithography facilitated fabrication of the cuboid cavities directly on the substrate or on the decoupling structure, while similar structures were fabricated on the substrate by UV lithography for comparison. Significant reduction of the lasing threshold by a factor of ~30 has been observed for cavities supported by the photonic crystal relative to those fabricated on the substrate. The lasing mode spectra of the cuboid microresonators provide strong evidence showing that the lasing modes are localized in the horizontal plane, with the shape of an inscribed diamond.

physics.optics↗

arXiv2014

Long Range Coupling between Metallic Nanocavities

When two or more metallic nanoparticles are in close proximity, their plasmonic modes may interact through the near field, leading to additional resonances of the coupled system or to shifts of their resonant frequencies. This process is analogous to atom-hybridization, as had been proposed by Gersten and Nitzan and modeled by Nordlander et al. The coupling between plasmonic modes can be in-phase (symmetric) or out-of-phase (anti-symmetric), reflecting correspondingly, the "bonding" and "anti-bonding" nature of such configurations. Since the incoming light redistributes the charge distribution around the metallic nanoparticles, its polarization features play a major role in the nonlinear optical probing of the energy-level landscape upon hybridization. Thus, controlling the nature of coupling between metallic nanostructures is of a great importance as it enables tuning their spectral responses leading to novel devices which may surpass the diffraction limit.

physics.optics↗

arXiv2013

Three-dimensional emission from organic Fabry-Perot microlasers

We measured the far-field emission patterns in three dimensions of flat organic dye microlasers using a solid angle scanner. Polymer-based microcavities of ribbon shape (i.e., Fabry-Perot type) were investigated. Out of plane emission from the cavities was observed, with significant differences for the two cases of resonators either fully supported by the substrate or sustained by a pedestal. In both cases, the emission diagrams are accounted for by a model combining diffraction at the cavity edges and reflections from the substrate.

physics.optics↗

arXiv2013

From individual to strongly coupled metallic nanocavities

Localized plasmonic modes of metallic nanoparticles may hybridize like those of atoms forming a molecule. However, the rapid decay of the plasmonic fields outside the metal severely limits the range of these interactions to tens of nanometers. Herein, we demonstrate very strong coupling of nanocavities in metal films, sparked by propagating surface plasmons and evident even at much larger distances of hundreds of nanometers for the properly selected metal/wavelength combination. Such strong coupling drastically changes the symmetry of the charge distribution around the nanocavities making it amenable to probing by the nonlinear optical response of the medium. We show that when strongly coupled, equilateral triangular nanocavities lose their individual three-fold symmetry to adopt the lower symmetry of the coupled system and then respond like a single dipolar entity. A quantitative model is suggested for the transition from individual to strongly coupled nanocavities.

physics.optics↗

arXiv2012

Shape and Size Resonances in Second Harmonic Generation from Plasmonic Nano-Cavities

The nonlinear response of sub wavelength nano-cavities in thin metal films is investigated. We report the resonant dependence of the Second Harmonic Generation by individual triangular and square holes on shape, size and wavelength. For cavities with internal nano-corrugations, giant field enhancements are observed, making them excellent candidates for high sensitivity spectroscopy.

cond-mat.mes-hall↗

arXiv2003

In-situ diagnostics of the crystalline nature of single organic nanocrystals by nonlinear microscopy

We elucidate the crystalline nature and the three-dimensional orientation of isolated organic nanocrystals embedded in a sol-gel matrix, using a polarized nonlinear microscopy technique that combines two-photon fluorescence and second harmonic generation. This technique allows the distinction between mono-crystalline structures and nano-scale poly-crystalline aggregates responsible for incoherent second harmonic signals.

cond-mat.mtrl-sci↗

arXiv2003

Dramatic Shape Sensitivity of Directional Emission Patterns from Similarly Deformed Cylindrical Polymer Lasers

Recent experiments on similarly shaped polymer micro-cavity lasers show a dramatic difference in the far-field emission patterns. We show for different deformations of the ellipse, quadrupole and hexadecapole that the large differences in the far-field emission patterns is explained by the differing ray dynamics corresponding to each shape. Analyzing the differences in the appropriate phase space for ray motion, it is shown that the differing geometries of the unstable manifolds of periodic orbits are the decisive factors in determining the far-field pattern. Surprisingly, we find that strongly chaotic ray dynamics is compatible with highly directional emission in the far-field.

physics.optics↗

arXiv2003

Monitoring of Orientation in Molecular Ensembles by Polarization Sensitive Nonlinear Microscopy

We present high resolution two-photon excitation microscopy studies combining two-photon fluorescence (TPF) and second harmonic generation (SHG) in order to probe orientational distributions of molecular ensembles at room temperature. A detailed polarization analysis of TPF and SHG signals is used in order to unravel the parameters of the molecular orientational statistical distribution, using a technique which can be extended and generalized to a broad variety of molecular arrangements. A polymer film containing molecules active for TPF and/or SHG emission is studied as a model system. Polarized TPF is shown to provide information on specific properties pertaining to incoherent emission in molecular media, such as excitation transfer. SHG, being highly sensitive to a slight departure from centrosymmetry such as induced by an external electric field in the medium, complements TPF. The response of each signal to a variable excitation polarization allows investigation of molecular behavior in complex environments which affect their orientations and interactions.

cond-mat.soft↗