arXiv subjects

Benedikt Zerulla

Publications and source records attributed to Benedikt Zerulla.

10 recordsLinked to original sources

arXiv2025

Towards a fully differentiable digital twin for solar cells

Maximizing energy yield (EY) - the total electric energy generated by a solar cell within a year at a specific location - is crucial in photovoltaics (PV), especially for emerging technologies. Computational methods provide the necessary insights and guidance for future research. However, existing simulations typically focus on only isolated aspects of solar cells. This lack of consistency highlights the need for a framework unifying all computational levels, from material to cell properties, for accurate prediction and optimization of EY prediction. To address this challenge, a differentiable digital twin, Sol(Di)$^2$T, is introduced to enable comprehensive end-to-end optimization of solar cells. The workflow starts with material properties and morphological processing parameters, followed by optical and electrical simulations. Finally, climatic conditions and geographic location are incorporated to predict the EY. Each step is either intrinsically differentiable or replaced with a machine-learned surrogate model, enabling not only accurate EY prediction but also gradient-based optimization with respect to input parameters. Consequently, Sol(Di)$^2$T extends EY predictions to previously unexplored conditions. Demonstrated for an organic solar cell, the proposed framework marks a significant step towards tailoring solar cells for specific applications while ensuring maximal performance.

physics.comp-ph↗

arXiv2025

Predicting the optical properties of organometallic nanoparticles with a scale-bridging method: The importance of the embedding

It remains a prime question of how to describe the optical properties of large molecular clusters accurately. Quantum chemical methods capture essential electronic details but are infeasible for entire clusters, while optical simulations handle cluster-scale effects but miss crucial quantum effects. To overcome such limitations, we apply here a multi-scale modeling approach, combining precise quantum chemistry calculations with Maxwell scattering simulations, to study the linear and nonlinear optical response of finite-size supramolecular gold-cysteine nanoparticles dispersed in water. In this approach, every molecular unit that forms the cluster is represented by a polarizability and a hyperpolarizability, and the overall response is obtained from solving an optical multiple scattering problem. We particularly demonstrate how important it is to accurately consider the environment of the individual molecular units when computing their polarizability and hyperpolarizability. In our quantum chemical simulations, we do so at the level of a static partial charge field that represents the presence of other molecular units. Without correctly considering these effects of the embedding, predictions would deviate from experimental observations even qualitatively. Our findings pave the way for more accurate predictions of the optical response of complex molecular systems, which is crucial for advancing applications in nanophotonics, biosensing, and molecular optoelectronics.

physics.optics↗

arXiv2024

A Tensor Product Space for Studying the Interaction of Bipartite States of Light with Nanostructures

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.

physics.optics↗

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

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

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

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↗

arXiv2022

A T-matrix Based Approach to Homogenize Artificial Materials

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.

physics.optics↗