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Shaping the structure of light with flat optical devices has driven significant advancements in our fundamental understanding of light and light-matter interactions, and enabled a broad range of applications, from image processing and microscopy to optical communication, quantum information processing, and the manipulation of microparticles. Yet, pushing the boundaries of structured light beyond the linear optical regime remains an open challenge. Nonlinear optical interactions, such as wave mixing in nonlinear flat optics, offer a powerful platform to unlock new degrees of freedom and functionalities for generating and detecting structured light. In this study, we experimentally demonstrate the non-trivial structuring of third-harmonic light enabled by the addition of total angular momentum projection in a nonlinear, isotropic flat optics element -- a single thin film of amorphous silicon. We identify the total angular momentum projection and helicity as the most critical properties for analyzing the experimental results. The theoretical model we propose, supported by numerical simulations, offers quantitative predictions for light structuring through nonlinear wave mixing under various pumping conditions, including vectorial and non-paraxial pump light. Notably, we reveal that the shape of third-harmonic light is highly sensitive to the polarization state of the pump. Our findings demonstrate that harnessing the addition of total angular momentum projection in nonlinear wave mixing can be a powerful strategy for generating and detecting precisely controlled structured light.

The study of the modes of optical resonators is beneficial for theoretical and practical endeavors. Here, we introduce a scalar product, originally devised for radiation fields, to such studies. This scalar product allows one to normalize and compare resonant modes using their corresponding radiation fields. Such fields are polychromatic fields free of divergences, which are determined for any given mode by its complex frequency and the modal field on the surface of the resonator. The scalar product is expressed as a surface integral involving the modal fields, multiplied by a closed-form factor incorporating the complex frequencies. In a practical application, we study the modes of disk-shaped whispering gallery resonators, and we show that the proposed scalar product accurately predicts the geometry-dependent coupling between modes.

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., Comment: This is a revised version of the article as submitted to the Journal of Quantitative Spectroscopy and Radiative Transfer that was finally published there

Pairs of entangled photons are important for applications in quantum nanophotonics, where their theoretical description must accommodate their bipartite character. Such character is shared at the other end of the intensity range by, for example, the two degenerate instances of the pump field involved in second-harmonic generation. The description and numerical simulation of the interaction of nanophotonic structures with bipartite states of light is challenging regardless of their intensity, and has important technological applications. To address such a challenge, we develop here a theoretical and computational framework for studying the interaction of material structures with bipartite states of light. The theory of the framework rests on the symmetrized tensor product space of two copies of an electromagnetic Hilbert space. For the computational side, the convenient T-matrix method is extended to the tensor product space. When the response of the object to one part of the state is independent of the other part, the T-matrix for bipartite states is a simple function of the typical T-matrix of the single Hilbert space. Such separable material response is relevant, for example, in the interaction of entangled biphoton states with nanostructures. Non-separable operators are identified as the adequate objects to fully integrate non-linear effects such as sum frequency generation or parametric down-conversion. As an example of application, we derive selection rules for second-order non-linear processes in objects with rotational and/or mirror symmetries, and verify them numerically in two different MoS$_2$ clusters., Comment: 17 pages, 3 figures

Many physically interesting quantities of the electromagnetic field can be computed using the electromagnetic scalar product. However, none of the existing expressions for such scalar product are directly applicable when the fields are only known in a spatially-bounded domain, as is the case for many numerical Maxwell solvers. In here, we derive an expression for the electromagnetic scalar product between radiation fields that only involves integrals over closed spatial surfaces. The expression readily leads to formulas for the number of photons, energy, and helicity of generic polychromatic light pulses of incoming or outgoing character. The capabilities of popular Maxwell solvers in spatially-bounded computational domains are thereby augmented, for example, by a straightforward method for normalizing emitted fields so that they contain a single photon.

The interaction of light with short light pulses is relevant in optical traps, optical tweezers, and many other applications. The theoretical description of such polychromatic light-matter interaction is challenging, and more so when the object is moving with respect to the light source, albeit with constant speed. Light sails are futuristic examples where such speed should reach the relativistic regime. In here, we provide a methodology for the theoretical and numerical analysis of the interaction of light pulses with objects moving with constant speed. The methodology allows one, in particular, to readily compute the transfer of fundamental quantities such as energy and momentum from the light pulse to the object. As an example, we compute the transfer of energy and momentum between a given pulse and a silicon sphere moving at relativistic speeds. The methodology, however, is valid for generic pulses and objects. Particularizing the equations to the case of zero speed allows one to treat static or quasi-static objects. The method is based on the polychromatic T-matrix formalism, which leverages the many publicly available resources for computing T-matrices.

The control of thermal radiation by means of micro-structured materials is an active area of research with applications such as thermophotovoltaics and radiative cooling. The original theories of thermal radiation were derived for electromagnetically large objects, and predict unpolarized, omnidirectional, and uncorrelated radiation. Microstructures, however, exhibit thermal emissions that can be polarized, highly directional, and spatially and temporally correlated. The original theories are also restricted to thermal equilibrium situations and do not apply to steady-state emissions of electromagnetically small objects under a stationary illumination. In here, we establish a polychromatic framework to predict thermal radiation in the stationary regime, which includes thermal equilibrium. After identifying an object--adapted set of independent polychromatic absorption modes, we assume that the emission also occurs independently through the outgoing versions of each polychromatic mode. Energy conservation leads then to a Kirchhoff-like law for each polychromatic mode. The salient properties of the polychromatic theory are: Emission in frequencies that are absent in the illumination, change in the number of photons, and applicability to both thermal radiation and luminescence upon illumination with a continuous wave laser, as long as the emitted power depends linearly on the input intensity. These properties are independent of the chosen set of polychromatic modes. In this work, we chose the absorption modes derived from the scattering operator of a given object, and use the T-matrix formalism for computations, which applies to general objects, including microscopic ones. Some counter-intuitive results motivate the future search for a different set of modes.

The chirality of an object can be studied by measuring the circular dichroism, that is, the difference in absorption of light with different helicity. The chiral optical response of an object, however, can have two different origins. On the one hand, it can be linked to the chiral geometry of the object. On the other hand, it can be linked to the chiral material from which the object is made. Whereas previously, no distinction between the two contributions could be made, we report here a computational approach that allows us to separate these two contributions to the circular dichroism of an object. We consider separately the cases where geometry-related resonances affect the optical response and where they are absent. In both cases, we find the circular dichroism to be easily decomposable if a geometrically achiral object has a similar absorption spectrum to the chiral object under investigation. Furthermore, in the non-resonant case, the contribution attributed to the material can be obtained without taking any geometry into account. Besides being of fundamental importance, the possibility of disentangling both contributions will be important for guiding the future design of chiral objects and devices.

Second harmonic generation (SHG) is forbidden in centrosymmetric molecular materials. However, a signal is frequently observed from interfaces where the symmetry is broken. Whereas the effect can be phenomenologically accommodated, an ab initio qualitative and quantitative description has remained elusive, preventing the exploration of fascinating questions such as how deep below the surface the second harmonic can still be generated. To answer such questions, we present an ab initio multiscale approach to compute the total and layer-dependent intensity of surface SHG from molecular crystals. The microscopic origin of surface SHG is identified in layer-dependent models with embedding partial charges combined with density functional theory. The models show increasing symmetry-breaking distortions of the electron cloud around the molecules as the surface layer is approached. The SHG at the molecular level is determined using time-dependent density functional theory and then brought to the scale of macroscopic films through a rigorous self-consistent multiple scattering formalism capable of predicting the measurable optical intensities of the generated second harmonic signal. We study crystalline molecular films with centrosymmetric unit cells of 7,9-Dibromobenzo[h]quinolin-10-ol. The intensity of the SHG at the surface layer is two orders of magnitude larger than at the next layer below and three orders of magnitude larger than two layers below. Besides providing fundamental understanding, our approach can be used for designing and optimizing optical devices containing nonlinear molecular materials, such as molecular laminates. We show that a relatively basic Kretschmann-like setup can enhance the surface SHG of a crystalline film of centrosymmetric molecular unit cells a thousand times., Comment: 12 pages, 6 figures

Nanophotonic concepts can improve many measurement techniques by enhancing and tailoring the light-matter interaction. However, the optical response of devices that implement such techniques can be intricate, depending on the sample under investigation. That combination of a promise and a challenge makes nanophotonics a ripe field for applying the concept of a digital twin: a digital representation of an entire real-world device. In this work, we detail the concept of a digital twin with the example of a nanophotonically-enhanced chiral sensing platform. In that platform, helicity-preserving cavities with diffractive mirrors enhance the light-matter interaction between chiral molecules and circularly polarized light, allowing a faster measurement of the circular dichroism of the molecules. However, the sheer presence of the molecules affects the cavity's functionality, demanding a holistic treatment to understand the device's performance. In our digital twin, optical and quantum chemistry simulations are fused to provide a comprehensive description of the device with the molecules across all length scales and predict the circular dichroism spectrum of the device containing molecules to be sensed. Performing simulations in lockstep with the experiment will allow a clear interpretation of the results of complex measurements. We also demonstrate how to design a cavity-enhanced circular dichroism spectrometer by utilizing our digital twin. The digital twin can be used to guide experiments and analyze results, and its underlying concept can be translated to many other optical experiments., Comment: 17 pages, 6 figures

We report the publication of treams, a new software for electromagnetic scattering computations based on the T-matrix method. Besides conventional T-matrix calculations for individual scatterers and finite clusters of particles, a unique feature of the code is its full support for periodic boundaries in one, two, and all three spatial dimensions. We use highly efficient and quickly converging lattice summation techniques based on the Ewald method to evaluate the arising lattice sums in these cases. In addition to the common use of vector spherical waves as a basis set for the T-matrix, vector cylindrical waves are also implemented. To describe stratified media, vector plane waves are used with an S-matrix description of the electromagnetic scattering. All basis sets and the associated methods can be used together with chiral constitutive relations. This contribution outlines the basic methods implemented and the program structure. Two interfaces to the implemented functionality are available: a flexible and fast low-level interface and a high-level interface for added convenience and plausibility checks. We conclude with two examples: a demonstration of the field calculation in various lattices and the explorations of quasi-bound states in the continuum. The presented code was already used in calculations for various physical systems: from the mode properties of molecular arrays in cavities to analytical models for metasurfaces and from moir\'{e} lattices to the homogenization of artificial photonic materials. With the publication of treams and the associated documentation, we hope to empower more scientists to make an efficient, fast, and precise exploration of nanophotonic systems that can be described in the broader framework of scattering theory. The full code is published at https://github.com/tfp-photonics/treams with the documentation at https://tfp-photonics.github.io/treams .

Nonlinear optics is essential for many recent photonic technologies. Here, we introduce a novel multi-scale approach to simulate the nonlinear optical response of molecular nanomaterials combining ab initio quantum-chemical and classical Maxwell-scattering computations. In this approach, the first hyperpolarizability tensor is computed with time-dependent density-functional theory and translated into a multi-scattering formalism that considers the optical interaction between neighboring molecules. A novel object is introduce to perform this transition from quantum-chemistry to classical scattering theory: the Hyper-Transition(T)-matrix. With this object at hand, the nonlinear optical response from single molecules and also from entire photonic devices can be computed, incorporating the full tensorial and dispersive nature of the optical response of the molecules. To demonstrate the applicability of our novel approach, the generation of a second-harmonic signal from a thin film of a Urea molecular crystal is computed and compared to more traditional simulations. Furthermore, an optical cavity is designed, which enhances the second-harmonic response of the molecular film by more than two orders of magnitude. Our approach is highly versatile and accurate and can be the working horse for the future exploration of nonlinear photonic molecular materials in structured photonic environments.

The T-matrix is a powerful tool that provides the complete description of the linear interaction between the electromagnetic field and a given object. In here, we generalize the usual monochromatic formalism to the case of polychromatic field-matter interaction. The group of transformations of special relativity provides the guidance for building the new formalism, which is inherently polychromatic. The polychromatic T-matrix affords the direct treatment of the interaction of electromagnetic pulses with objects, even when the objects move at constant relativistic speeds.

Electronic circular dichroism is an important optical phenomenon offering insights into chiral molecular materials. On the other hand, metal-organic frameworks (MOFs) are a novel group of crystalline porous thin-film materials that provide tailor-made chemical and physical properties by carefully selecting their building units. Combining these two aspects of contemporary material research and integrating chiral molecules into MOFs promises devices with unprecedented functionality. However, considering the nearly unlimited degrees of freedom concerning the choice of materials and the geometrical details of the possibly structured films, we urgently need to complement advanced experimental methods with equally strong modeling techniques. Most notably, these modeling techniques must cope with the challenge that the material and devices thereof cover size scales from {\AA}ngstr\"oms to mm. In response to that need, we outline a computational workflow that seamlessly combines quantum chemical methods to capture the properties of individual molecules with optical simulations to capture the properties of functional devices made from these molecular materials. We concentrate on chiral properties and apply our work to UiO-67-BINOL MOFs, for which experimental results are available to benchmark the results of our simulations and explore the optical properties of cavities and metasurfaces made from that chiral material.

Electromagnetic waves impinging on three-dimensional helical metallic metamaterials have been shown to exhibit chiral effects of large magnitude both theoretically and in experimental realizations. Chirality here describes different responses of scatterers, materials, or metamaterials to left and right circularly polarized electromagnetic waves. These differences can be quantified in terms of electromagnetic chirality measures. In this work we consider the optimal design of thin metallic free-form nanowires that possess measures of electromagnetic chirality as large as fundamentally possible. We focus on optical frequencies and use a gradient based optimization scheme to determine the optimal shape of highly chiral thin silver and gold nanowires. The electromagnetic chirality measures of our optimized nanowires exceed that of traditional metallic helices. Therefore, these should be well suited as building blocks of novel metamaterials with an increased chiral response. We discuss a series of numerical examples, and we evaluate the performance of different optimized designs.

The accurate and efficient computation of the electromagnetic response of objects made from artificial materials is crucial for designing photonic functionalities and interpreting experiments. Advanced fabrication techniques can nowadays produce new materials as three-dimensional lattices of scattering unit cells. Computing the response of objects of arbitrary shape made from such materials is typically computationally prohibitive unless an effective homogeneous medium approximates the discrete material. In here, we introduce a homogenization method based on the effective T-matrix. Such a matrix captures the exact response of the discrete material, is determined by the T-matrix of the isolated unit cell and the material lattice vectors, and is free of spatial dispersion. The truncation of the effective T-matrix to dipolar order determines the common bi-anisotropic constitutive relations. When combined with quantum-chemical and Maxwell solvers, the method allows one to compute the response of arbitrarily-shaped volumetric patchworks of structured molecular materials and metamaterials.

We introduce a systematic way to obtain expressions for computing the amount of fundamental quantities such as helicity and angular momentum contained in static matter, given its charge and magnetization densities. The method is based on a scalar product that we put forward, which is invariant under the ten-parameter conformal group in three-dimensional Euclidean space. Such group is obtained as the static restriction (frequency $\omega=0$) of the symmetry group of Maxwell equations: The fifteen-parameter conformal group in 3+1 Minkowski spacetime. In an exemplary application, we compute the helicity and angular momentum squared stored in a magnetic Hopfion.

The evaluation of the interaction between objects arranged on a lattice requires the computation of lattice sums. A scenario frequently encountered are systems governed by the Helmholtz equation in the context of electromagnetic scattering in an array of particles forming a metamaterial, a metasurface, or a photonic crystal. While the convergence of direct lattice sums for such translation coefficients is notoriously slow, the application of Ewald's method converts the direct sums into exponentially convergent series. We present a derivation of such series for the 2D and 3D solutions of the Helmholtz equation, namely spherical and cylindrical solutions. When compared to prior research, our novel expressions are especially aimed at computing the lattice sums for several interacting sublattices in 1D lattices (chains), 2D lattices (gratings), and 3D lattices. We verify our results by comparison with the direct computation of the lattice sums.

Designing objects with predefined optical properties is a task of fundamental importance for nanophotonics, and chirality is a prototypical example of such a property, with applications ranging from photochemistry to nonlinear photonics. A measure of electromagnetic chirality with a well-defined upper bound has recently been proposed. Here, we optimize the shape of silver helices at discrete frequencies ranging from the far infrared to the optical band. Gaussian process optimization, taking into account also shape derivative information of the helices scattering response, is used to maximize the electromagnetic chirality. We show that the theoretical designs achieve more than 90 percent of the upper bound of em-chirality for wavelenghts \SI{3}{\micro\meter} or larger, while their performance decreases towards the optical band. We fabricate and characterize helices for operation at \SI{800}{\nano\meter}, and identify some of the imperfections that affect the performance. Our work motivates further research both on the theoretical and fabrication sides to unlock potential applications of objects with large electromagnetic chirality at optical frequencies, such as helicity filtering glasses. We show that, at \SI{3}{\micro\meter}, a thin slab of randomly oriented helices can absorb 99 percent of the light of one helicity while absorbing only 9 percent of the opposite helicity.

The differential response of chiral molecules to incident left- and right- handed circularly polarized light is used for sensing the handedness of molecules. Currently, significant effort is directed towards enhancing weak differential signals from the molecules, with the goal of extending the capabilities of chiral spectrometers to lower molecular concentrations or small analyte volumes. Previously, optical cavities for enhancing vibrational circular dichroism have been introduced. Their enhancements are mediated by helicity-preserving cavity modes which maintain the handedness of light due to their degenerate TE and TM components. In this article, we simplify the design of the cavity, and numerically compare it with the previous one using an improved model for the response of chiral molecules. We use parameters of molecular resonances to show that the cavities are capable of bringing the vibrational circular dichroism signal over the detection threshold of typical spectrometers for concentrations that are one to three orders of magnitude smaller than those needed without the cavities, for a fixed analyte volume. Frequency resolutions of current spectrometers result in enhancements of more than one order (two orders) of magnitude for the new (previous) design. With improved frequency resolution, the new design achieves enhancements of three orders of magnitude. We show that the TE/TM degeneracy in perfectly helicity preserving modes is lifted by factors that are inherent to the cavities. More surprisingly, this degeneracy is also lifted by the molecules themselves due to their lack of electromagnetic duality symmetry, that is, due to the partial change of helicity during the light-molecule interactions., Comment: This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in Applied Physics Reviews 7, 041413 (2020) and may be found at https://aip.scitation.org/doi/abs/10.1063/5.0025006

The electromagnetic helicity of the free electromagnetic field and the static magnetic helicity are shown to be two different embodiments of the same physical quantity, the total helicity. The total helicity is the sum of two terms: a term that measures the difference between the number of left-handed and right-handed photons of the free field, and another term that measures the screwiness of the static magnetization density in matter. Each term is the manifestation of the total helicity in different frequency regimes: $\omega$ > 0 and $\omega$ = 0, respectively. This unification establishes the theoretical basis for studying the conversion between the two embodiments of total helicity upon light-matter interaction.

The measurement of circular dichroism (CD) has widely been exploited to distinguish the different enantiomers of chiral structures. It has been applied to natural materials (e.g. molecules) as well as to artificial materials (e.g. nanophotonic structures). However, especially for chiral molecules the signal level is very low and increasing the signal-to-noise ratio is of paramount importance to either shorten the necessary measurement time or to lower the minimum detectable molecule concentration. As one solution to this problem, we propose here to use quantum states of light in CD sensing to reduce the noise below the shot noise limit that is encountered when using coherent states of light. Through a multi-parameter estimation approach, we identify the ultimate quantum limit to precision of CD sensing, allowing for general schemes including additional ancillary modes. We show that the ultimate quantum limit can be achieved by various optimal schemes. It includes not only Fock state input in direct sensing configuration but also twin-beam input in ancilla-assisted sensing configuration, for both of which photon number resolving detection needs to be performed as the optimal measurement setting. These optimal schemes offer a significant quantum enhancement even in the presence of additional system loss. The optimality of a practical scheme using a twin-beam state in direct sensing configuration is also investigated in details as a nearly optimal scheme for CD sensing when the actual CD signal is very small. Alternative schemes involving single-photon sources and detectors are also proposed. This work paves the way for further investigations of quantum metrological techniques in chirality sensing., Comment: 9 pages, 5 figures

Predicting the optical response of macroscopic arrangements of individual scatterers is a computational challenge, as the problem involves length scales across multiple orders of magnitude. We present a full-wave optical method to highly efficiently compute the scattering of light at objects that are arranged in bi-periodic arrays. Multiple arrays or homogeneous thin-films can be stacked to build up an entire multicomposite material in the third dimension. The scattering properties of the individual objects in each array are described by the T-matrix formalism. Therefore, arbitrarily shaped objects and even molecules can be the basic constituent of the arrays. Taking the T-matrix of the individual scatterer as the point of departure allows to explain the optical properties of the bulk material from the scattering properties of its constituents. We use solutions of Maxwell's equations with well defined helicity. Therefore, chiral media are particularly easy to consider as materials for both scatterers or embedding media. We exemplify the efficiency of the algorithm with an exhaustive parametric study of anti-reflective coatings for solar cells made from cylinders with a high degree of helicity preservation. The example shows a speed-up of about 500 with respect to finite-element computations. A second example specifically exploits the use helicity modes to investigate the enhancement of the circular dichroism signal in a chiral material.

We present an electromagnetic chirality measure for 2D arrays of subwavelength periodicities under normal illumination. The calculation of the measure uses only the complex reflection and transmission coefficients from the array. The measure allows the ordering of arrays according to their electromagnetic chirality, which further allows a quantitative comparison of different design strategies. The measure is upper bounded, and the extreme properties of objects with high values of electromagnetic chirality make them useful in both near- and far-field applications. We analyze the consequences that different possible symmetries of the array have on its electromagnetic chirality. We use the measure to study four different arrays. The results indicate the suitability of helices for building arrays of high electromagnetic chirality, and the low effectiveness of a substrate for breaking the transverse mirror symmetry.

The photonic environment can significantly influence emission properties and interactions among atomic systems. In such scenarios, frequently the electric dipole approximation is assumed that is justified as long as the spatial extent of the atomic system is negligible compared to the spatial variations of the field. While this holds true for many canonical systems, it ceases to be applicable for more contemporary nanophotonic structures. To go beyond the electric dipole approximation, we propose and develop in this article an analytical framework to describe the impact of the photonic environment on emission and interaction properties of atomic systems beyond the electric dipole approximation. Particularly, we retain explicitly magnetic dipolar and electric quadrupolar contributions to the light-matter interactions. We exploit a field quantization scheme based on electromagnetic Green's tensors, suited for dispersive materials. We obtain expressions for spontaneous emission rate, Lamb shift, multipole-multipole shift and superradiance rate, all being modified with dispersive environment. The considered influence could be substantial for suitably tailored nanostructured photonic environments, as demonstrated exemplarily., Comment: 2 figures + supplementary material, 21 pages altogether

The average helicity of a given electromagnetic field measures the difference between the number of left- and right-handed photons contained in the field. In here, the average helicity is derived using the conformally-invariant inner-product for Maxwell fields. Several equivalent integral expressions in momentum space, in $(\mathbf{r},t)$ space, and in the time-harmonic $(\mathbf{r},\omega)$ space are obtained, featuring Riemann-Silberstein-like fields and potentials. The time-harmonic expressions can be directly evaluated using the outputs of common numerical solvers of Maxwell equations. The results are shown to be equivalent to the well-known volume integral for the average helicity, featuring the electric and magnetic fields and potentials.

Recent experiments demonstrated strongly directional coupling of light into waveguide modes. We identify here the mechanisms behind this effect. We consider emitters near a waveguide, either centered on the median plane of the waveguide, or displaced from such plane. We show that, independently of the displacement, the directionality is mostly due to a mirror symmetry breaking caused by the axial character of the angular momentum of the emitted light. The sign of the angular momentum along an axis transverse to the waveguide determines the preferential coupling direction. The degree of directionality grows exponentially as the magnitude of such transverse angular momentum increases linearly. We trace this exponential dependence back to a property of the evanescent angular spectrum of the emissions. A binary and less pronounced directional coupling effect due to the chiral character of the handedness of the emission is possible when the displacement of the emitter breaks another of the mirror symmetries of the waveguide. We find a selection rule that allows or prevents the coupling of centered electric(magnetic) multipolar emissions onto the waveguide modes. We also show that the selection of a different angular momentum axis made in some experiments causes significant differences in the way in which directionality depends on angular momentum. We then use these differences to propose an experiment featuring a transverse magnetic bias that allows to aggregate the directional emissions from quantum dots on top of waveguides. Our symmetry-based results apply to any emitted multipolar order, clarify the spin-momentum locking concept, and generalize it to an exponentially-strong locking between the transverse angular momentumand the preferential coupling direction.

Researchers routinely sense molecules by their infrared vibrational "fingerprint" absorption resonances. In addition, the dominant handedness of chiral molecules can be detected by circular dichroism (CD), the normalized difference between their optical response to incident left- and right- handed circularly polarized light. Here, we introduce a cavity composed of two parallel arrays of helicity-preserving silicon disks that allows to enhance the CD signal by more than two orders of magnitude for a given molecule concentration and given thickness of the cell containing the molecules. The underlying principle is first-order diffraction into helicity-preserving modes with large transverse momentum and long lifetimes. In sharp contrast, in a conventional Fabry-Perot cavity, each reflection flips the handedness of light, leading to large intensity enhancements inside the cavity, yet to smaller CD signals than without the cavity.

Suppressing the reflection from material interfaces or entire layer stacks across an extended spectral range is important for various applications. While many approaches have been described for this purpose, we look at the problem here from the perspective of helicity preservation. Specifically, the anti-reflection performance of nano-particle arrays on top of solar cell stacks is related to two conditions: a high enough degree of discrete rotational symmetry and the ability of the system to suppress cross-talk between the two handednesses (helicities) of the electromagnetic field upon light-matter interaction. For particle-lattice systems with high enough degree of discrete rotational symmetry ($2\pi/n$ for $n>2$), our numerical studies link the suppression of backscattering to the ability of the system to avoid the mixing between the two helicity components of the incident field. In an exemplary design, we use an array of TiO$_2$ disks placed on top of a flat heterojunction solar cell stack, and analyze the helicity preservation properties of the system. We show numerically that a hexagonal array lattice, featuring a higher degree of discrete rotational symmetry, can improve over the anti-reflection performance of a square lattice. Importantly, the disks are introduced in an electrically decoupled manner such that the passivation and electric properties of the device are not disturbed., Comment: 23 pages, 4 figures

Manipulating the excitation of resonant electric and magnetic multipole moments in structured dielectric media has unlocked many sophisticated electromagnetic functionalities. This article demonstrates the experimental realization of a broadband Huygens' source. This Huygens' source consists of a spherical particle that exhibits a well-defined forward-scattering pattern across more than an octave-spanning spectral band at GHz frequencies, where the scattering in the entire backward hemisphere is suppressed. Two different low-index nonmagnetic spheres are studied that differ in their permittivity. This causes them to offer a different shape for the forward-scattering pattern. The theoretical understanding of this broadband feature is based on the approximate equality of the resonant electric and magnetic multipole moments in both amplitude and phase in low permittivity spheres. This is a key condition to approximate the electromagnetic duality symmetry which, together with the spherical symmetry, suppresses the backscattering. With such a configuration, broadband Huygens' sources can be designed even if magnetic materials are unavailable. This article provides guidelines for designing broadband Huygens' sources using low-index spheres that could be valuable to a plethora of applications., Comment: 14 pages, 6 figures

We derive a set of design requirements that lead to structures suitable for molecular circular dichroism (CD) enhancement. Achirality of the structure and two suitably selected sequentially incident beams of opposite helicity ensures that the CD signal only depends on the chiral absorption properties of the molecules, and not on the achiral ones. Under this condition, a helicity preserving structure, which prevents the coupling of the two polarization handednesses, maximizes the enhancement of the CD signal for a given ability of the structure to enhance the field. When the achirality and helicity preservation requirements are met, the enhancement of the CD signal is directly related to the enhancement of the field. Next, we design an exemplary structure following the requirements. The considered system is a planar array of silicon cylinders under normally incident plane-wave illumination. Full-wave numerical calculations show that the enhancement of the transmission CD signal is between 6.5 and 3.75 for interaction lengths between 1.25 and 3 times the height of the cylinders., Comment: This document is the unedited Authors version of a Submitted Work that was subsequently accepted for publication in ACS Photonics, copyright American Chemical Society after peer review. To access the final edited and published work see 10.1021/acsphotonics.8b01454. The corrections published in 10.1021/acsphotonics.0c00113 are included in this arxiv document

Decomposing the field scattered by an object into vector spherical harmonics (VSH) is the prime task when discussing its optical properties on more analytical grounds. Thus far, it was frequently required in the decomposition that the scattered field is available on a spherical surface enclosing the scatterer; being with that adapted to the spatial dependency of the VSHs but being rather incompatible with many numerical solvers. To mitigate this problem, we propose an orthogonal expression for the decomposition that holds for any surface that encloses the scatterer, independently of its shape. We also show that the orthogonal relations remain unchanged when the radiative VSH used for the expansion of the scattered field are substituted by the VSH used for the expansion of the illumination as test functions. This is a key factor for the numerical stability of our decomposition. As example, we use a finite-element based solver to compute the multipole response of a nanorod illuminated by a plane wave and study its convergence properties.

We establish a link between quantum mechanical molecular simulations and the transfer matrix of a molecule. The transfer matrix (T-matrix) of an object provides a complete description of its electromagnetic response. Once the T-matrices of the individual components of an ensemble are known, the electromagnetic response of the ensemble can be efficiently computed. This holds for arbitrary arrangements of large number of molecules, as well as for periodic arrays. We provide T-matrix based formulas for computing traditional chiro-optical properties like Circular Dichroism and Oriented Circular Dichroism, and also for quantifying electromagnetic duality and electromagnetic chirality, two properties that are fundamentally related to chiral interactions, and also technologically relevant. The formulas are valid for light-matter interactions of arbitrary high multipolar orders. We exemplify our approach by first computing the T-matrix of a cross-like arrangement of four copies of a chiral molecule from the time-dependent Hartree-Fock theory simulation data of the individual molecule, and then computing the aforementioned electromagnetic properties of both the cross and the individual molecule. The link that we establish is a necessary step towards obtaining T-matrix based constitutive relations of general bulk molecular materials from quantum mechanical simulations of their molecular constituents.

Symmetry is one of the most general and useful concepts in physics. A theory or a system that has a symmetry is fundamentally constrained by it. The same constraints do not apply when the symmetry is broken. The quantitative determination of "how much a system breaks a symmetry" allows to reach beyond this binary situation and is a necessary step towards the quantitative connection between symmetry breaking and its effects. We introduce measures of symmetry breaking for a system interacting with external fields (particles). They can be computed from measurements of the system-mediated coupling strengths between subspaces of incoming and outgoing fields (particles) that transform in a definite way under the symmetry. The generality of these symmetry breaking measures and their tight connection to experimental measurements make them applicable to a very wide range of physics, like quantification of phase transitions, constraints in dynamical evolution, and the search for hidden symmetries., Comment: Link to published article: http://iopscience.iop.org/article/10.1088/2399-6528/aada25

Material electromagnetic duality symmetry requires a system to have equal electric and magnetic responses. Electromagnetic duality enables technologically important effects like artificial optical activity and zero back-scattering, is a requirement for metamaterials in transformation optics, Huygens wave-front control, and maximal electromagnetic chirality, and appears in topological photonic systems. Intrinsically dual materials that meet the duality conditions at the level of the constitutive relations do not exist in many frequency bands. Nevertheless, discrete objects like metallic helices and homogeneous dielectric spheres can be engineered to approximate the dual behavior. The discrete objects can then be used as building blocks with the objective of obtaining composite systems with high duality symmetry. Here, we exploit the extra degrees of freedom of a core-shell dielectric sphere to obtain a particle whose duality symmetry is more than one order of magnitude better than previously reported non-magnetic objects. We show that the improvement is transferred onto the duality symmetry of composite objects when the core-shell particle is used as a building block instead of homogeneous spheres., Comment: 5 pages, 3 figures, 1 table

The exact suppression of backscattering from rotationally symmetric objects requires dual symmetric materials where ${\epsilon_r} = {\mu_r}$. This prevents their design at many frequency bands, including the optical one, because magnetic materials are not available. Electromagnetically small non-magnetic spheres of large permittivity offer an alternative. They can be tailored to exhibit balanced electric and magnetic dipole polarizabilities, which result in approximate zero backscattering. In this case, the effect is inherently narrowband. Here, we put forward a different alternative that allows broadband functionality: Electromagnetically large spheres made from low permittivity materials. The effect occurs in a parameter regime that approaches the trivial ${\epsilon_r} \to {\mu_r} =1$ case, where approximate duality is met in a weakly wavelength dependence fashion. Despite the low permittivity, the overall scattering response of the spheres is still significant. Radiation patterns from these spheres are shown to be highly directive across an octave spanning band. The effect is analytically and numerically shown using the Mie coefficients., Comment: 6 Figures

We propose a novel scheme to normalize scattering modes of the electromagnetic field. By relying on analytical solutions for Maxwell's equations in the homogenous medium outside the scatterer, we derive normalization conditions that only depend on the electromagnetic field on the surface of a sphere containing the scatterer. We pay special attention to the important cases of plane wave illumination and illumination with a multipolar field, for which an explicit and easy to use normalization condition is derived. We demonstrate the versatility of our method by normalizing scattering modes of some selected metallic and dielectric scatterers of different geometries in the context of different application scenarios. Since every quantum mechanical treatment of light-matter interaction requires the proper normalization of electromagnetic fields, we deem our proposed normalization scheme broadly applicable independent of the scatterer involved., Comment: 16 pages, 5 figures

The multipole expansion is a key tool in the study of light-matter interactions. All the information about the radiation of and coupling to electromagnetic fields of a given charge-density distribution is condensed into few numbers: The multipole moments of the source. These numbers are frequently computed with expressions obtained after the long-wavelength approximation. Here, we derive exact expressions for the multipole moments of dynamic sources that resemble in their simplicity their approximate counterparts. We validate our new expressions against analytical results for a spherical source, and then use them to calculate the induced moments for some selected sources with a non-trivial shape. The comparison of the results to those obtained with approximate expressions shows a considerable disagreement even for sources of subwavelength size. Our expressions are relevant for any scientific area dealing with the interaction between the electromagnetic field and material systems., Comment: 21 pages, 3 figures