arXiv subjects

Baptiste Auguié

Publications and source records attributed to Baptiste Auguié.

11 recordsLinked to original sources

arXiv2026

T-matrix representation of optical scattering response: Suggestion for a data format

The transition matrix, frequently abbreviated as T-matrix, contains the complete information in a linear approximation of how a spatially localized object scatters an incident field. The T-matrix is used to study the scattering response of an isolated object and describes the optical response of complex photonic materials made from ensembles of individual objects. T-matrices of certain common structures, potentially, have been repeatedly calculated all over the world again and again. This is not necessary and constitutes a major challenge for various reasons. First, the resources spent on their computation represent an unsustainable financial and ecological burden. Second, with the onset of machine learning, data is the gold of our era, and it should be freely available to everybody to address novel scientific challenges. Finally, the possibility of reproducing simulations could tremendously improve if the considered T-matrices could be shared. To address these challenges, we found it important to agree on a common data format for T-matrices and to enable their collection from different sources and distribution. This document aims to develop the specifications for storing T-matrices and associated metadata. The specifications should allow maximum freedom to accommodate as many use cases as possible without introducing any ambiguity in the stored data. The common format will assist in setting up a public database of T-matrices.

physics.optics↗

arXiv2023

Generalised coupled-dipole model for core-satellite nanostructures

Plasmonic core-satellite nanostructures have recently attracted interest in photocatalytic applications. The core plasmonic nanoparticle acts like an antenna, funnelling incident light into the near-field region, where it excites the smaller satellite nanoparticles with resonantly enhanced absorption. Computer simulations of the optical absorption by such structures can prove challenging, even with state-of-the-art numerical methods, due to the large difference in size between core and satellite particles. We present a generalised coupled-dipole model that enables efficient computations of light absorption in such nanostructures, including those with many satellites. The method accurately predicts the local absorption in each satellite despite being two orders of magnitude weaker than the absorption in the core particle. We assess the range of applicability of this model by comparing the results against the superposition $T$-matrix method, a rigorous solution of Maxwell's equations that is much more resource-intensive and becomes impractical as the number of satellite particles increases.

physics.optics↗

arXiv2022

Orientation-averaged light scattering by nanoparticle clusters: far-field and near-field benchmarks of numerical cubature methods

The optical properties of nanoparticles can be substantially affected by their assembly in compact aggregates. This is a common situation notably for nanoparticles synthesised and self-assembled into rigid clusters in colloidal form, where they may be further characterised or used in spectroscopic applications. The theoretical description of such experiments generally requires averaging the optical response over all possible cluster orientations, as they randomly orient themselves over the course of a measurement. This averaging is often done numerically by simulating the optical response for several directions of incidence, using a spherical cubature method. The simulation time increases with the number of directions and can become prohibitive, yet few studies have examined the trade-off between averaging accuracy and computational cost. We benchmark seven commonly-used spherical cubature methods for both far-field and near-field optical responses for a few paradigmatic cluster geometries: dimers of nanospheres and of nanorods, and a helix. The relative error is rigorously evaluated in comparison to analytical results obtained with the superposition T-matrix method. Accurate orientation averaging is especially important for quantities relating to optical activity, the differential response to left and right circularly polarised light, and our example calculations include in particular far-field circular dichroism and near-field local degree of optical chirality.

physics.optics↗

arXiv2021

Multiple scattering of light in nanoparticle assemblies: user guide for the TERMS program

We introduce TERMS, an open-source Fortran program to simulate near-field and far-field optical properties of clusters of particles. The program solves rigorously the Maxwell equations via the superposition T-matrix method, where incident and scattered fields are decomposed into series of vector spherical waves. TERMS implements several algorithms to solve the coupled system of multiple scattering equations that describes the electromagnetic interaction between neighbouring scatterers. From this formal solution, the program can compute a number of physically-relevant optical properties, such as far-field cross-sections for extinction, absorption, scattering and their corresponding circular dichroism, as well as local field intensities and degree of optical chirality. By describing the incident and scattered fields in a basis of spherical waves the T-matrix framework lends itself to analytical formulas for orientation-averaged quantities, corresponding to systems of particles in random orientation; TERMS offers such computations for both far-field and near-field quantities of interest. This user guide introduces the program, summarises the relevant theory, and is supplemented by a comprehensive suite of stand-alone examples in the website accompanying the code.

physics.comp-ph↗

arXiv2021

Orientation dependence of optical activity in light scattering by nanoparticle clusters

The optical properties of nanoparticle clusters vary with the spatial arrangement of the constituent particles, but also the overall orientation of the cluster with respect to the incident light. This is particularly important in the context of nanoscale chirality and associated chiroptical responses, such as circular dichroism or differential scattering of circularly polarised light in the far-field, or local degree of optical chirality in the near-field. We explore the angular dependence of such quantities for a few archetypal geometries: a dimer of gold nanorods, a helix of gold nanospheres, and a linear chain of silicon particles. The examples serve to illustrate the possible variation of chiroptical responses with the direction of light's incidence, but also, consequently, the importance of a robust orientation-averaging procedure when modelling general clusters of particles in random orientation. Our results are obtained with the rigorous superposition T-matrix method, which provides analytical formulas for exact orientation-averaged properties.

physics.optics↗

arXiv2021

Core-Shell Bimetallic Nanoparticle Trimers for Efficient Light-to-Chemical Energy Conversion

Incorporation of catalytically active materials into plasmonic metal nanostructures can efficiently merge the reactivity and energy harvesting abilities of both types of materials for visible light photocatalysis. Here we explore the influence of electromagnetic hotspots in the ability of plasmonic core-shell colloidal structures to induce chemical transformations. For this study, we developed a synthetic strategy for the fabrication of Au nanoparticle (NP) trimers in aqueous solution through fine controlled galvanic replacement between Ag nanoprisms and Au precursors. Core-shell Au@M NP trimers with catalytically active metals (M = Pd, Pt) were subsequently synthesized using Au NP trimers as templates. Our experimental and computational results highlight the synergy of geometry and composition in plasmonic catalysts for plasmon-driven chemical reactions.

physics.chem-ph↗

arXiv2020

Orientation Averaging of Optical Chirality Near Nanoparticles and Aggregates

Artificial nanostructures enable fine control of electromagnetic fields at the nanoscale, a possibility that has recently been extended to the interaction between polarised light and chiral matter. The theoretical description of such interactions, and its application to the design of optimised structures for chiroptical spectroscopies, brings new challenges to the common set of tools used in nano-optics. In particular, chiroptical effects often depend crucially on the relative orientation of the scatterer and the incident light, but many experiments are performed with randomly-oriented scatterers, dispersed in a solution. We derive new expressions for the orientation-averaged local degree of optical chirality of the electromagnetic field in the presence of a nanoparticle aggregate. This is achieved using the superposition T -matrix framework, ideally suited for the derivation of efficient orientation-averaging formulas in light scattering problems. Our results are applied to a few model examples, and illustrate several non-intuitive aspects in the distribution of orientation-averaged degree of chirality around nanostructures. The results will be of significant interest for the study of nanoparticle assemblies designed to enhance chiroptical spectroscopies, and where the numerically-efficient computation of the averaged degree of optical chirality enables a more comprehensive exploration of the many possible nanostructures.

physics.optics↗

arXiv2019

Laplace's equation for a point source near a sphere: improved internal solution using spheroidal harmonics

As shown recently [Phys. Rev. E 95, 033307 (2017)], spheroidal harmonics expansions are well suited for the external solution of Laplace's equation for a point source outside a spherical object. Their intrinsic singularity matches the line singularity of the analytic continuation of the solution and the series solution converges much faster than the standard spherical harmonic solution. Here we extend this approach to internal potentials using the Kelvin transformation, i.e. radial inversion, of the spheroidal coordinate system. This transform converts the standard series solution involving regular solid spherical harmonics into a series of irregular spherical harmonics. We then substitute the expansion of irregular spherical harmonics in terms of transformed irregular spheroidal harmonics into the potential. The spheroidal harmonic solution fits the image line singularity of the solution exactly and converges much faster. We also discuss why a solution in terms of regular solid spheroidal harmonics cannot work, even though these functions are finite everywhere in the sphere. We also present the analogous solution for an internal point source, and two new relationships between the solid spherical and spheroidal harmonics.

math-ph↗

arXiv2015

Modified optical absorption of molecules on metallic nanoparticles at sub-monolayer coverage

Enhanced optical absorption of molecules in the vicinity of metallic nanostructures is key to a number of surface-enhanced spectroscopies and of great general interest to the fields of plasmonics and nano-optics. Yet, experimental access to this absorbance has long proven elusive. We here present direct measurements of the intrinsic absorbance of dye-molecules adsorbed onto silver nanospheres, and crucially, at sub-monolayer concentrations where dye--dye interactions become negligible. With a large detuning from the plasmon resonance, distinct shifts and broadening of the molecular resonances reveal the intrinsic properties of the dye in contact with the metal colloid, in contrast to the often studied strong-coupling regime where the optical properties of the dye-molecules cannot be isolated. The observation of these shifts together with the ability to routinely measure them has broad implications in the interpretation of experiments involving resonant molecules on metallic surfaces, such as surface-enhanced spectroscopies and many aspects of molecular plasmonics.

physics.optics↗

arXiv2012

Radiative correction in approximate treatments of electromagnetic scattering by point and body scatterers

The transition-matrix ($T$-matrix) approach provides a general formalism to study scattering problems in various areas of physics, including acoustics (scalar fields) and electromagnetics (vector fields), and is related to the theory of the scattering matrix ($S$-matrix) used in quantum mechanics and quantum field theory. Focusing on electromagnetic scattering, we highlight an alternative formulation of the $T$-matrix approach, based on the use of the reactance matrix or $K$-matrix, which is more suited to formal studies of energy conservation constraints (such as the optical theorem). We show in particular that electrostatics or quasi-static approximations can be corrected within this framework to satisfy the energy conservation constraints associated with radiation. A general formula for such a radiative correction is explicitly obtained, and empirical expressions proposed in earlier studies are shown to be special cases of this general formula. This work therefore provides a justification of the empirical radiative correction to the dipolar polarizability and a generalization of this correction to any types of point or body scatterers of arbitrary shapes, including higher multipolar orders.

physics.optics↗

arXiv2012

Diffractive arrays of gold nanoparticles near an interface: critical role of the substrate

The optical properties of periodic arrays of plasmonic nanoantennas are strongly affected by coherent multiple scattering in the plane of the array, which leads to sharp spectral resonances in both transmission and reflection when the wavelength is commensurate with the period. We demonstrate that the presence of a substrate (i.e., an asymmetric refractive-index environment) can inhibit long-range coupling between the particles and suppress lattice resonances, in agreement with recent experimental results. We find the substrate-to-superstrate index contrast and the distance between the array and the interface to be critical parameters determining the strength of diffractive coupling. Our rigorous electromagnetic simulations are well reproduced by a simple analytical model. These findings are important in the design of periodic structures and in the assessment of their optical resonances for potential use in sensing and other photonic technologies.

physics.optics↗