arXiv subjects

Carsten Rockstuhl

Publications and source records attributed to Carsten Rockstuhl.

At least 55 records · Page 3Linked to original sources

arXiv2024

Analyzing the acceleration time and reflectance of light sails made from homogeneous and core-shell spheres

Deciding on appropriate materials and designs for use in light sails, like the one proposed in the Breakthrough Starshot Initiative, is a topic that requires much care and forethought. Here, we offer a feasible option in the form of metasurfaces made of periodically arranged homogeneous and core-shell spheres. Using the re-normalized T-matrix from Mie theory, we explore the reflectance, absorptance, and acceleration time of such metasurfaces. We focus on spheres made from aluminum, silicon, silicon dioxide, and combinations thereof. Since the light sails are foreseen to be accelerated using Earth-based laser arrays to 20% of the speed of light, one needs to account for relativistic effects. As a result, a high broadband reflectance is essential for effective propulsion. We identify metasurfaces that offer such properties combined with a low absorptance to reduce heating and deformation. We highlight a promising extension to the case of a metasurface made from homogeneous silicon spheres, as already discussed in the literature, by adding a layer of silicon dioxide. The high broadband reflectance of the silicon and silicon dioxide combination is explained by the favorable interference of the multipolar contributions of the outgoing field up to quadrupolar order. We also consider the impact of an embedding material characterized by different refractive indices. Refractive indices up to 1.13 maintain over 90% reflectance without re-optimizing the light sail.

physics.optics↗

arXiv2024

Inverse Design of Polaritonic Devices

Polaritons, arising from the strong coupling between excitons and photons within microcavities, hold promise for optoelectronic and all-optical devices. They have found applications in various domains, including low-threshold lasers and quantum information processing. To realize complex functionalities, non-intuitive designs for polaritonic devices are required. In this contribution, we use finite-difference time-domain simulations of the dissipative Gross-Pitaevskii equation, written in a differentiable manner, and combine it with an adjoint formulation. Such a method allows us to use topology optimization to engineer the potential landscape experienced by polariton condensates to tailor its characteristics on demand. The potential directly translates to a blueprint for a functional device, and various fabrication and optical control techniques can experimentally realize it. We inverse-design a selection of polaritonic devices, i.e., a structure that spatially shapes the polaritons into a flat-top distribution, a metalens that focuses a polariton, and a nonlinearly activated isolator. The functionalities are preserved when employing realistic fabrication constraints such as minimum feature size and discretization of the potential. Our results demonstrate the utility of inverse design techniques for polaritonic devices, providing a stepping stone toward future research in optimizing systems with complex light-matter interactions.

physics.optics↗

arXiv2024

A framework to compute resonances arising from multiple scattering

Numerous natural and technological phenomena are governed by resonances. In nanophotonics, resonances often result from the interaction of several optical elements. Controlling these resonances is an excellent opportunity to provide light with properties on demand for applications ranging from sensing to quantum technologies. The inverse design of large, distributed resonators, however, is typically challenged by high computational costs when discretizing the entire system in space. Here, this limitation is overcome by harnessing prior knowledge about the individual scatterers that form the resonator and their interaction. In particular, a transition matrix multi-scattering framework is coupled with the state-of-the-art adaptive Antoulas-Anderson (AAA) algorithm to identify complex poles of the optical response function. A sample refinement strategy suitable for accurately locating a large number of poles is introduced. We tie the AAA algorithm into an automatic differentiation framework to efficiently differentiate multi-scattering resonance calculations. The resulting resonance solver allows for efficient gradient-based optimization, demonstrated here by the inverse design of an integrated exciton-polariton cavity. This contribution serves as an important step towards efficient resonance calculations in a variety of multi-scattering scenarios, such as inclusions in stratified media, periodic lattices, and scatterers with arbitrary shapes.

physics.comp-ph↗

arXiv2024

Enhancement of the photon pair generation rate by spontaneous four-wave mixing in bent waveguides

Enhancing nonlinear optical effects is critical to improving the performance of many functional devices for nonlinear and quantum optical applications. Here we study the possibility of bending a waveguide to enhance the photon pair generation rate in a spontaneous four-wave mixing process. Whereas intuition might suggest that bending makes the process less efficient, because the waveguides are more lossy when bent, we show that the increase in the effective nonlinearity outperforms the disadvantage for moderate bending radii. That can be explained by a better localization of the guided eigenmodes, leading to a reduced mode area. By studying selected waveguide devices with a fixed length, we demonstrate an optimal improvement between 5 % and 270 % in the photon pair generation rate for an optimal bending radius. These findings have implications for the future design of integrated photonic devices for quantum optical applications, especially in cases where the chip estate tends to be a limiting factor.

physics.optics↗

arXiv2024

The electromagnetic scalar product in spatially-bounded domains

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.

physics.optics↗

arXiv2024

Polarization-dependent effects in vibrational absorption spectra of 2D finite-size adsorbate islands on dielectric substrates

In the last years, Infrared Reflection-Absorption Spectroscopy (IRRAS) became a standard technique to study vibrational excitations of molecules. These investigations are strongly motivated by perspective applications in monitoring chemical processes. For a better understanding of the adsorption mechanism of molecules on dielectrics, the polarization-dependence of an interaction of infrared light with adsorbates at dielectric surfaces is commonly used. Thus, the peak positions in absorption spectra could be different for s- and p-polarized light. This shift between the peak positions depends on both the molecule itself and the dielectric substrate. While the origin of this shift is well understood for infinite two-dimensional adsorbate layers, finite-size samples, which consist of 2D islands of a small number of molecules, have never been considered. Here, we present a study on polarization-dependent finite-size effects in the optical response of such islands on dielectric substrates. The study uses a multi-scale modeling approach that connects quantum chemistry calculations to Maxwell scattering simulations. We distinguish the optical response of a single molecule, a finite number of molecules, and a two-dimensional adsorbate layer. We analyze CO and CO$_2$ molecules deposited on CeO$_2$ and Al$_2$O$_3$ substrates. The evolution of the shift between the polarization-dependent absorbance peaks is firstly studied for a single molecule, which it does not exhibit for at all, and for finite molecular islands, which it increases with increasing island size for, as well as for an infinite two-dimensional adsorbate layer. In the latter case, the agreement between the obtained results and the experimental IRRAS data and more traditional three/four-layer-model theoretical studies supports the predictive power of the multi-scale approach.

physics.optics↗

arXiv2024

Separating the Material and Geometry Contribution to the Circular Dichroism of Chiral Objects Made from Chiral Media

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.

physics.optics↗

arXiv2024

Surface Second Harmonic Generation in Centrosymmetric Molecular Crystalline Materials: How Thick is the Surface?

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.

physics.optics↗

arXiv2023

Dynamic Control of Spontaneous Emission Using Magnetized InSb Higher-Order-Mode Antennas

We exploit InSb's magnetic-induced optical properties to propose THz sub-wavelength antenna designs that actively tune the radiative decay rates of dipole emitters at their proximity. The proposed designs include a spherical InSb antenna and a cylindrical Si-InSb hybrid antenna that demonstrate distinct behaviors; the former dramatically enhances both radiative and non-radiative decay rates in the epsilon-near-zero region due to the dominant contribution of the Zeeman splitting electric octupole mode. The latter realizes significant radiative decay rate enhancement via magnetic octupole mode, mitigating the quenching process and accelerating the photon production rate. A deep learning-based optimization of emitter positioning further enhances the quantum efficiency of the proposed hybrid system. These novel mechanisms are potentially promising for tunable THz single-photon sources in integrated quantum networks.

quant-ph↗

arXiv2023

Superradiant Broadband Magneto-electric Arrays Empowered by Meta-learning

Laws of electrodynamics constrain scattering cross-sections of resonant objects. Nevertheless, a fundamental bound that expresses how larger that scattering cross-section can be is yet to be found. Approaches based on cascading multiple resonances permitted to push the scattering responses of subwavelength structures and to exceed existing estimators, for which the Chu-Harrington criterion is, potentially, the most commonly considered one. The superradiant empirical limit, addressing scattering performances of near-field coupled resonator arrays, was subsequently developed to tighten existing estimates, setting a new bound that prompted efforts to find structures that exceed it. Here, we demonstrate that genetically designed superscattering structures, encompassing arrays of constructively interfering electric and magnetic dipoles, can build enormously high scatting cross-sections exceeding those imposed by existing criteria in electromagnetic theory including the superradiant empirical limit. After undergoing thousands of evolutionary generations, iterating sizes, mutual orientations, and locations of resonators, the structures approach their heuristically maximized performance, which is unlikely to be obtained by a random distribution given more than a billion trials. As an additional practically valuable parameter, the scattering bandwidth also underwent optimization. We demonstrate that flat wavelength-comparable structures can have significant backscattering alongside more than 40% fractional bandwidth. The result demonstrates the fundamental capability to untighten scattering cross-section from bandwidth limitations. New capabilities of genetic optimization algorithms, equipped with fast computational tools and constrained by experimentally obtainable electromagnetic parameters, allow chasing well-accepted traditional bounds, demonstrating ever-seen electromagnetic performances.

physics.app-ph↗

arXiv2023

A digital twin for a chiral sensing platform

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.

physics.optics↗

arXiv2023

treams -- A T-matrix scattering code for nanophotonic computations

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 moiré 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 .

physics.comp-ph↗

arXiv2023

A Multi-Scale Approach to Simulate the Nonlinear Optical Response of Molecular Nanomaterials

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.

physics.optics↗

arXiv2023

Inverse Design of All-dielectric Metasurfaces with Bound States in the Continuum

Metasurfaces with bound states in the continuum (BICs) have proven to be a powerful platform for drastically enhancing light-matter interactions, improving biosensing, and precisely manipulating near- and far-fields. However, engineering metasurfaces to provide an on-demand spectral and angular position for a BIC remains a prime challenge. A conventional solution involves a fine adjustment of geometrical parameters, requiring multiple time-consuming calculations. In this work, to circumvent such tedious processes, we develop a physics-inspired, inverse design method on all-dielectric metasurfaces for an on-demand spectral and angular position of a BIC. Our suggested method predicts the core-shell particles that constitute the unit cell of the metasurface, while considering practical limitations on geometry and available materials. Our method is based on a smart combination of a semi-analytical solution, for predicting the required dipolar Mie coefficients of the meta-atom, and a machine learning algorithm, for finding a practical design of the meta-atom that provides these Mie coefficients. Although our approach is exemplified in designing a metasurface sustaining a BIC, it can, also, be applied to many more objective functions. With that, we pave the way toward a general framework for the inverse design of metasurfaces in specific and nanophotonic structures in general.

physics.optics↗

arXiv2023

Identifying regions of minimal back-scattering by a relativistically-moving sphere

The far-field back-scattering amplitude of an electric field from a relativistically-moving sphere is analyzed. Contrary to prior research, we do so by expressing the fields in the helicity basis, and we highlight here its advantages when compared to the commonly-considered parity basis. With the purpose of exploring specific scattering phenomena considering relativistic effects, we identify conditions that minimize the back-scattered field, leading to a relativistic formulation of the first Kerker condition. The requirements to be satisfied by the sphere are expressed in terms of Mie angles, which constitute an effective parametrization of any possible optical response a sphere might have. We are able to identify multiple combinations of Mie angles up to octupolar order via gradient-based optimization that satisfy our newly formulated relativistic Kerker condition, yielding minima for the back-scattered energy as low as 0.016% of the average scattered energy. Our results can be extended to involve multiple particles forming a metasurface, potentially having direct implications on the design of light sails as considered by the Breakthrough Starshot Initiative.

physics.optics↗

arXiv2023

Metasurface-Based Realization of Photonic Time Crystals

Photonic time crystals are artificial materials whose electromagnetic properties are uniform in space but periodically vary in time. The synthesis of such materials and experimental observation of their physics remain very challenging due to the stringent requirement for uniform modulation of material properties in volumetric samples. In this work, we extend the concept of photonic time crystals to two-dimensional artificial structures -- metasurfaces. We demonstrate that time-varying metasurfaces not only preserve key physical properties of volumetric photonic time crystals despite their simpler topology but also host common momentum bandgaps shared by both surface and free-space electromagnetic waves. Based on a microwave metasurface design, we experimentally confirmed the exponential wave amplification inside a momentum bandgap as well as the possibility to probe bandgap physics by external (free-space) excitations. The proposed metasurface serves as a straightforward material platform for realizing emerging photonic space-time crystals and as a realistic system for the amplification of surface-wave signals in future wireless communications.

physics.app-ph↗

arXiv2023

A neural operator-based surrogate solver for free-form electromagnetic inverse design

Neural operators have emerged as a powerful tool for solving partial differential equations in the context of scientific machine learning. Here, we implement and train a modified Fourier neural operator as a surrogate solver for electromagnetic scattering problems and compare its data efficiency to existing methods. We further demonstrate its application to the gradient-based nanophotonic inverse design of free-form, fully three-dimensional electromagnetic scatterers, an area that has so far eluded the application of deep learning techniques.

physics.comp-ph↗

arXiv2023

Exploring Functional Photonic Devices made from a Chiral Metal-Organic Framework Material by a Multiscale Computational Method

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 Ångströms 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.

cond-mat.mtrl-sci↗