arXiv subjects

A. Femius Koenderink

Publications and source records attributed to A. Femius Koenderink.

At least 19 recordsLinked to original sources

arXiv2026

Broadband Single-Particle Absorption Circular Dichroism Reveals Chiroptical Heterogeneity in Gold Helicoids

Quantitative measurements of absorption circular dichroism (CD) at the single-particle level are essential for understanding how individual chiral nanostructures dissipate optical energy, yet broadband absorptance measurements remain experimentally challenging. Here, we introduce a wavelength-tunable integrating-sphere microscope that determines the absorptance of individual nanoparticles under right- and left-circularly polarized illumination through direct optical energy balance, enabling broadband measurement of the absorption dissymmetry factor, gabs. Measurements of achiral gold nanospheres and strongly anisotropic gold nanorods establish the apparent absorption CD baseline and demonstrate minimal detectable linear-dichroism-to-circular-dichroism (LD-to-CD) leakage under the experimental conditions. Applying this approach to 87 chiral gold helicoids synthesized using L-glutathione (L-helicoids) and 96 synthesized using D-glutathione (D-helicoids) reveals mean particle-level gabs values of opposite sign, with a statistically significant difference between the two populations. Individual particles nevertheless exhibit pronounced heterogeneity in response sign, magnitude, spectral position, and line shape. More than one-third of the particles in each population display opposite-sign absorption CD responses relative to their population-average tendency. Correlative SEM analysis of the L-helicoid population further shows that opposite-sign responses persist among isolated particles exhibiting the characteristic projected helicoid morphology, indicating that aggregation and gross differences in projected morphology are insufficient to explain the observed heterogeneity. These results establish broadband single-particle absorption CD spectroscopy as a direct probe of absorptive chiroptical heterogeneity and reveal particle-specific responses obscured by ensemble averaging.

physics.optics↗

arXiv2026

Revealing time characteristics of optical excitations in dielectric and plasmonic structures through cathodoluminescence interferometry

Cathodoluminescence (CL) spectroscopy provides access to optical excitations with nanometer spatial resolution, but direct time-resolved measurements of optical resonances remain challenging. Here, we demonstrate that CL interferometry provides access to the temporal response, phase behavior, and modal spectral structure of resonant nanoscale scatterers without requiring ultrafast pump-probe schemes. We develop an analytical framework in which Fourier transformation angle- and frequency-resolved CL interferograms yields the decay time of optical resonances governed by the linear optical response. Multimode resonators exhibit characteristic temporal CL beating signatures associated with spectral mode splitting. By exploiting transition radiation emitted from a nearby metallic surface as a broadband reference, we further demonstrate phase retrieval and cross-correlation measurements between instantaneous and resonant emission processes. Experimental measurements on Au nanoparticles, broadband plasmonic emitters, Au nanostars, and Si nanospheres supporting multipolar Mie resonances confirm the theoretical predictions, and decay times in the range 1-10 fs are derived for each system. Our results establish CL interferometry as a powerful approach for accessing spectral, spatial, and phase information within a single nanoscale measurement with fs resolution.

cond-mat.mes-hall↗

arXiv2025

Metasurface lasers programmed by optical pump patterns

Metasurface lasers offer unprecedented control over light emission, yet their spatial and modal characteristics are typically fixed post-fabrication. Here, we introduce a reconfigurable plasmonic metasurface laser platform in which the lasing area geometry, and thus the emission properties, are dynamically programmed via spatially structured optical pumping. Using hexagonal arrays of silver nanoparticles embedded in dye-doped waveguides, we demonstrate lasing at high-symmetry points of the Brillouin zone, including the K and M points. K-point lasing exhibits spontaneous symmetry breaking (SSB) in relative intensity between degenerate K and K' modes, with no bias induced by pump geometry, even for geometries that explicitly break symmetry. In contrast, M-point lasing allows deterministic control over emission channels via asymmetric pumping. We further show that spatially separated K-point lasers synchronize in phase and amplitude, undergoing SSB in lockstep. A theoretical density matrix approach cast into stochastic differential equations reproduces the observed real- and Fourier-space intensity distributions and SSB behavior. Our findings establish spatially programmable metasurface lasers as a versatile platform for exploring dynamic phenomena in photonic lattices, with potential applications in vortex beam shaping, optical logic, and true random number generation.

physics.optics↗

arXiv2025

Uncovering hidden resonances in non-Hermitian systems with scattering thresholds

The points where diffraction orders emerge or vanish in the propagating spectrum of periodic non-Hermitian systems are referred to as scattering thresholds. Close to these branch points, resonances from different Riemann sheets can tremendously impact the optical response. However, these resonances are so far elusive for two reasons. First, their contribution to the signal is partially obscured, and second, they are inaccessible for standard computational methods. Here, the interplay of scattering thresholds with resonances is explored and a multi-valued rational approximation is introduced to access the hidden resonances. The theoretical and numerical approach is used to analyze the resonances of a plasmonic line grating. This work elegantly explains the occurrence of pronounced spectral features at scattering thresholds applicable to many nanophotonic systems of contemporary and future interest.

physics.optics↗

arXiv2023

Spontaneous symmetry breaking in plasmon lattice lasers

Spontaneous symmetry breaking (SSB) is key for our understanding of phase transitions and the spontaneous emergence of order. Photonics provide versatile systems to study SSB. In this work, we report that for a two-dimensional (2D) periodic nonlocal metasurface with gain, SSB occurs in the lasing transition, breaking parity symmetry. We study diffractive hexagonal plasmon nanoparticle lattices, where the K-points in momentum space provide two modes that are exactly degenerate in frequency and identically distributed in space. Using femtosecond pulses to energize the gain medium, we simultaneously capture single shot realspace and wavevector resolved Fourier images of laser emission. By combining Fourier- and real-space, we resolve the two order parameters for which symmetry breaking simultaneously occurs: spatial parity and U(1) (rotational) symmetry breaking, evident respectively as random relative mode amplitude and phase. Thereby, we quantify for the first time SSB in 2D periodic metasurfaces. These currently receive much interest as experimentally accessible implementations of seminal solid-state physics Hamiltonians and provide a large design space for exploring SSB in scenarios with different symmetries, mode degeneracies and topological properties. The methodology reported in this work is generally applicable to 2D plasmonic and dielectric metasurfaces and opens numerous opportunities for the study of SSB and emergence of spatial coherence in metaphotonics.

physics.optics↗

arXiv2023

Hybrid cavity-antenna architecture for strong and tunable sideband-selective molecular Raman scattering enhancement

Plasmon resonances at the surface of plasmonic antennas allow for extremely strong enhancement of Raman scattering. Intrinsic to plasmonics, however, is that extreme field confinement lacks precise spectral control, which would hold great promise in shaping the optomechanical interaction between light and molecular vibrations at will. We demonstrate an experimental platform composed of a plasmonic nanocube-on-mirror antenna coupled to an open, tunable Fabry-Perot microcavity for selective addressing of individual vibrational lines of molecules with strong Raman scattering enhancement. Multiple narrow and intense optical resonances arising from the hybridization of the cavity modes and the plasmonic broad resonance are used to simultaneously enhance the laser pump and the local density of optical states (LDOS) and are characterized using rigorous modal analysis. The versatile bottom-up fabrication approach permits quantitative comparison with the bare nanocube-on-mirror system, both theoretically and experimentally. This shows that the hybrid system allows for similar SERS enhancement ratios with narrow optical modes, paving the way for dynamical back action effects in molecular optomechanics.

physics.optics↗

arXiv2023

Direct Linearly-Polarised Electroluminescence from Perovskite Nanoplatelet Superlattices

Polarised light is critical for a wide range of applications, but is usually generated by filtering unpolarised light, which leads to significant energy losses and requires additional optics. Herein, the direct emission of linearly-polarised light is achieved from light-emitting diodes (LEDs) made of CsPbI3 perovskite nanoplatelet superlattices. Through use of solvents with different vapour pressures, the self-assembly of perovskite nanoplatelets is achieved to enable fine control over the orientation (either face-up or edge-up) and therefore the transition dipole moment. As a result of the highly-uniform alignment of the nanoplatelets, as well as their strong quantum and dielectric confinement, large exciton fine-structure splitting is achieved at the film level, leading to pure-red LEDs exhibiting a high degree of linear polarisation of 74.4% without any photonic structures. This work unveils the possibilities of perovskite nanoplatelets as a highly promising source of linearly-polarised electroluminescence, opening up the development of next-generation 3D displays and optical communications from this highly versatile, solution-processable system.

physics.optics↗

arXiv2022

Integrated Sideband-Resolved SERS with a Dimer on a Nanobeam Hybrid

In analogy to cavity optomechanics, enhancing specific sidebands of a Raman process with narrowband optical resonators would allow for parametric amplification, entanglement of light and molecular vibrations, and reduced transduction noise. We report on the demonstration of waveguide-addressable sideband-resolved surface-enhanced Raman scattering (SERS). We realized a hybrid plasmonic-photonic resonator consisting of a 1D photonic crystal cavity decorated with a sub-20 nm gap dimer nanoantenna. Hybrid resonances in the near-IR provide designer Q-factors of 1000, and $Q/V=(λ^3/10^6)^{-1}$, with SERS signal strength on par with levels found in state-of-the-art purely plasmonic systems. We evidence Fano-lineshapes in the SERS enhancement of organic molecules, and quantitatively separate out the pump enhancement and optical reservoir contributions.

physics.optics↗

arXiv2021

Hybrid Photonic-Plasmonic Cavities based on the Nanoparticle-on-a-Mirror Configuration

Hybrid photonic-plasmonic cavities have emerged as a new platform to increase light-matter interaction capable to enhance the Purcell factor in a singular way not attainable with either photonic or plasmonic cavities separately. In the hybrid cavities proposed so far, mainly consisting of metallic bow-tie antennas, the plasmonic gap sizes defined by lithography in a repeatable way are limited to minimum values \approx 10 nm. Nanoparticle-on-a-mirror (NPoM) cavities are far superior to achieve the smallest possible mode volumes, as gaps smaller than 1 nm can be created. Here, we design a hybrid cavity that combines a NPoM plasmonic cavity and a dielectric-nanobeam photonic crystal cavity operating at transverse-magnetic (TM) polarization. The metallic nanoparticle can be placed very close (< 1 nm) to the upper surface of the dielectric cavity, which acts as a low-reflectivity mirror. We demonstrate through numerical calculations that this kind of hybrid plasmonic-photonic cavity architecture exhibits quality factors, Q, above 10^{3} and normalized mode volumes, V , down to 10^{\num{-3}}, thus resulting in high Purcell factors (FP \approx 10^5), whilst being experimentally feasible with current technology. Our results suggest that hybrid cavities with sub-nm gaps should open new avenues for boosting light-matter interaction in nanophotonic systems.

physics.optics↗

arXiv2021

Integrated molecular optomechanics with hybrid dielectric-metallic resonators

Molecular optomechanics stems from the description of Raman scattering in the presence of an optical resonator using a cavity optomechanics formalism. We extend the molecular optomechanics formalism to the case of hybrid dielectric-plasmonic resonators, with multiple optical resonances and with both free-space and waveguide addressing. We demonstrate how the Raman enhancement is the product of a pump enhancement and a modified LDOS, that simply depend on the complex response functions of the hybrid system. The Fano lineshapes that result from hybridization of a broadband and narrowband modes allows reaching strong Raman enhancement with high-Q resonances, paving the way towards sideband resolved molecular optomechanics. The model allows prediction of the Raman emission ratio into different output ports and enables demonstrating a fully integrated high-Q Raman resonator exploiting multiple cavity modes coupled to the same waveguide.

physics.optics↗

arXiv2021

Calibration-based overlay sensing with minimal-footprint targets

Overlay measurements are a critical part of modern semiconductor fabrication, but overlay targets have not scaled down in the way devices have. In this work, we produce overlay targets with very small footprint, consisting of just a few scattering nanoparticles in two separate device layers. Using moiré patterns to deterministically generate many overlay errors on a single chip, we demonstrate successful readout of the relative displacement between the two layers and show that calibration on one realization of the targets can be used for overlay measurements on subsequent instances. Our results suggest using greater quantities of smaller overlay targets may benefit performance both directly and through finer sampling of deformation.

physics.app-ph↗

arXiv2021

Intermittency of CsPbBr$_3$ perovskite quantum dots analyzed by an unbiased statistical analysis

We analyze intermittency in intensity and fluorescence lifetime of CsPbBr$_3$ perovskite quantum dots by applying unbiased Bayesian inference analysis methods. We apply changepoint analysis (CPA) and a Bayesian state clustering algorithm to determine the timing of switching events and the number of states between which switching occurs in a statistically unbiased manner, which we have benchmarked particularly to apply to highly multistate emitters. We conclude that perovskite quantum dots display a plethora of gray states in which brightness broadly speaking correlates inversely with decay rate, confirming the multiple recombination centers model. We leverage the CPA partitioning analysis to examine aging and memory effects. We find that dots tend to return to the bright state before jumping to a dim state, and that when choosing a dim state they tend to explore the entire set of states available.

cond-mat.mes-hall↗

arXiv2021

A Python toolbox for unbiased statistical analysis of fluorescence intermittency of multi-level emitters

We report on a Python-toolbox for unbiased statistical analysis of fluorescence intermittency properties of single emitters. Intermittency, i.e., step-wise temporal variations in the instantaneous emission intensity and fluorescence decay rate properties are common to organic fluorophores, II-VI quantum dots and perovskite quantum dots alike. Unbiased statistical analysis of intermittency switching time distributions, involved levels and lifetimes is important to avoid interpretation artefacts. This work provides an implementation of Bayesian changepoint analysis and level clustering applicable to time-tagged single-photon detection data of single emitters that can be applied to real experimental data and as tool to verify the ramifications of hypothesized mechanistic intermittency models. We provide a detailed Monte Carlo analysis to illustrate these statistics tools, and to benchmark the extent to which conclusions can be drawn on the photophysics of highly complex systems, such as perovskite quantum dots that switch between a plethora of states instead of just two.

physics.comp-ph↗

arXiv2019

High-index dielectric metasurfaces performing mathematical operations

Image processing and edge detection are at the core of several newly emerging technologies, such as augmented reality, autonomous driving and more generally object recognition. Image processing is typically performed digitally using integrated electronic circuits and algorithms, implying fundamental size and speed limitations, as well as significant power needs. On the other hand, it can also be performed in a low-power analog fashion using Fourier optics, requiring however bulky optical components. Here, we introduce dielectric metasurfaces that perform optical image edge detection in the analog domain using a subwavelength geometry that can be readily integrated with detectors. The metasurface is composed of a suitably engineered array of nanobeams designed to perform either 1st- or 2nd-order spatial differentiation. We experimentally demonstrate the 2nd-derivative operation on an input image, showing the potential of all-optical edge detection using a silicon metasurface geometry working at a numerical aperture as large as 0.35.

physics.optics↗

arXiv2017

Controlling nanoantenna polarizability through backaction via a single cavity mode

The polarizability $α$ determines the absorption, extinction and scattering by small particles. Beyond being purely set by scatterer size and material, in fact polarizability can be affected by backaction: the influence of the photonic environment on the scatterer. As such, controlling the strength of backaction provides a tool to tailor the (radiative) properties of nanoparticles. Here, we control the backaction between broadband scatterers and a single mode of a high-quality cavity. We demonstrate that backaction from a microtoroid ring resonator significantly alters the polarizability of an array of nanorods: the polarizability is renormalized as fields scattered from -- and returning to -- the nanorods via the ring resonator depolarize the rods. Moreover, we show that it is possible to control the strength of the backaction by exploiting the diffractive properties of the array. This perturbation of a strong scatterer by a nearby cavity has important implications for hybrid plasmonic-photonic resonators and the understanding of coupled optical resonators in general.

physics.optics↗

arXiv2016

Antenna-cavity hybrids: matching polar opposites for Purcell enhancements at any linewidth

Strong interaction between light and a single quantum emitter is essential to a great number of applications, including single photon sources. Microcavities and plasmonic antennas have been used frequently to enhance these interactions through the Purcell effect. Both can provide large emission enhancements: the cavity typically through long photon lifetimes (high $Q$), and the antenna mostly through strong field enhancement (low mode volume $V$). In this work, we demonstrate that a hybrid system, which combines a cavity and a dipolar antenna, can achieve stronger emission enhancements than the cavity or antenna alone. We show that such systems can be used as a versatile platform to tune the bandwidth of enhancement to any desired value, while simultaneously boosting emission enhancement. Our fully consistent analytical model allows to identify the underlying mechanisms of boosted emission enhancement in hybrid systems, which include radiation damping and constructive interference between multiple-scattering paths. Additionally, we find excellent agreement between strongly boosted enhancement spectra from our analytical model and from finite-element simulations on a realistic cavity-antenna system. Finally, we demonstrate that hybrid systems can simultaneously boost emission enhancement and maintain a near-unity outcoupling efficiency into a single cavity decay channel, such as a waveguide.

physics.optics↗

arXiv2016

Backaction in metasurface etalons

We consider the response of etalons created by a combination of a conventional mirror and a metasurface, composed of a periodic lattice of metal scatterers with a resonant response. This geometry has been used previously for perfect absorption, in so-called Salisbury screens, and for hybridization of localized plasmons with Fabry-Perot resonances. The particular aspect we address is if one can assume an environment-independent reflectivity for the metasurface when calculating the reflectivity of the composite system, as in a standard Fabry-Perot analysis, or whether the fact that the metasurface interacts with its own mirror image renormalizes its response. Using lattice sum theory, we take into account all possible retarded dipole-dipole interactions of scatterers in the metasurface amongst each other, and through the mirror. We show that while a layer-by-layer Fabry-Perot formalism captures the main qualitative features of metasurface etalons, in fact the mirror modifies both the polarizability and reflectivity of the metasurface in a fashion that is akin to Drexhage's modification of the radiative properties of a single dipole.

physics.optics↗

arXiv2015

General point dipole theory for periodic metasurfaces: magnetoelectric scattering lattices coupled to planar photonic structures

We study semi-analytically the light emission and absorption properties of arbitrary stratified photonic structures with embedded two-dimensional magnetoelectric point scattering lattices, as used in recent plasmon-enhanced LEDs and solar cells. By employing dyadic Green's function for the layered structure in combination with Ewald lattice summation to deal with the particle lattice, we develop an efficient method to study the coupling between planar 2D scattering lattices of plasmonic, or metamaterial point particles, coupled to layered structures. Using the `array scanning method' we deal with localized sources. Firstly, we apply our method to light emission enhancement of dipole emitters in slab waveguides, mediated by plasmonic lattices. We benchmark the array scanning method against a reciprocity-based approach to find that the calculated radiative rate enhancement in k-space below the light cone shows excellent agreement. Secondly, we apply our method to study absorption-enhancement in thin-film solar cells mediated by periodic Ag nanoparticle arrays. Lastly, we study the emission distribution in k-space of a coupled waveguide-lattice system. In particular, we explore the dark mode excitation on the plasmonic lattice using the so-called Array Scanning Method. Our method could be useful for simulating a broad range of complex nanophotonic structures, i.e., metasurfaces, plasmon-enhanced light emitting systems and photovoltaics.

physics.optics↗