Chiral plasmonic metasurface assembled by DNA origami.

Chiral materials are essential to perceive photonic devices that control the helicity of light. However, the chirality of natural materials is rather weak, and relatively thick films are needed for noticeable effects. To overcome this limitation, artificial photonic materials were suggested to affect the chiral response in a much more substantial manner. Ideally, a single layer of such a material, a metasurface, should already be sufficient. While various structures fabricated with top-down nanofabrication technologies have already been reported, here we propose to utilize scaffolded DNA origami technology, a scalable bottom-up approach for metamolecule production, to fabricate a chiral metasurface. We introduce a chiral plasmonic metamolecule in the shape of a tripod and simulate its optical properties. By fixing the metamolecule to a rectangular planar origami, the tripods can be assembled into a 2D DNA origami crystal that forms a chiral metasurface. We simulate the optical properties but also fabricate selected devices to assess the experimental feasibility of the suggested approach critically.

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

In the last few years, infrared reflection-absorption spectroscopy (IRRAS) has become a standard technique to study vibrational excitations of molecules. These investigations are strongly motivated by potential 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 on 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 with 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 CO2 molecules deposited on CeO2 and Al2O3 substrates. The evolution of the shift between the polarization-dependent absorbance peaks is first studied for a single molecule, which does not exhibit any shifting at all, and for finite molecular islands, where it increases with increasing island size, 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.

Approximation method for fast calculation of transmission in multi-mode waveguides.

Freeform dielectric waveguides connect optical chips made of different materials in fully integrated photonic devices. With a spatial extent in the order of 100 µm, they constitute a computational challenge and make Maxwell full-wave solvers unhandy for the accelerated design. Therefore, it is of utmost importance to have tools that permit the fast prediction of waveguide loss to enable the rapid optimization of waveguide trajectories. Previously developed methods relied on the assumption that only a single mode propagates in the waveguide. However, the propagation of higher-order modes is not just unavoidable due to the geometry of the waveguides, but also, sometimes, beneficial as it increases the number of channels to transmit information. In this contribution, we present an approximate method for the fast calculation of transmission that accommodates the presence of higher-order waveguide modes, and assess its liability by describing light propagation through selected devices.

Optically tunable bianisotropy in a sphere made from an epsilon-near-zero material.

Bianisotropic media can be used to engineer absorbance, scattering, polarization, and dispersion of electromagnetic waves. However, the demonstration of a tunable light-induced bianisotropy at optical frequencies is still lacking. Here, we propose an experimentally feasible concept for a light-induced tunable bianisotropic response in a homogeneous sphere made of an epsilon-near-zero (ENZ) material. By exploiting the large linear absorption and the large possible intensity-dependent changes in the permittivity of ENZ materials, the direction-dependent scattering and absorption cross sections could be obtained. Our findings pave the way for further studies and applications in the optical regime requiring full dynamic control of the bianisotropic behavior.

Activating Electroluminescence of Charged Naphthalene Diimide Complexes Directly Adsorbed on a Metal Substrate.

Electroluminescence from single molecules adsorbed on a conducting surface imposes conflicting demands for the molecule-electrode coupling. To conduct electrons, the molecular orbitals need to be hybridized with the electrodes. To emit light, they need to be decoupled from the electrodes to prevent fluorescence quenching. Here, we show that fully quenched 2,6-core-substituted naphthalene diimide derivative in a self-assembled monolayer directly deposited on a Au(111) surface can be activated with the tip of a scanning tunneling microscope to decouple the relevant frontier orbitals from the metallic substrate. In this way, individual molecules can be driven from a strongly hybridized state with quenched luminescence to a light-emitting state. The emission performance compares in terms of quantum efficiency, stability, and reproducibility to that of single molecules deposited on thin insulating layers. Quantum chemical calculations suggest that the emitted light originates from the singly charged cationic pair of the molecules.

Quantum Plasmonic Sensors.

The extraordinary sensitivity of plasmonic sensors is well-known in the optics and photonics community. These sensors exploit simultaneously the enhancement and the localization of electromagnetic fields close to the interface between a metal and a dielectric. This enables, for example, the design of integrated biochemical sensors at scales far below the diffraction limit. Despite their practical realization and successful commercialization, the sensitivity and associated precision of plasmonic sensors are starting to reach their fundamental classical limit given by quantum fluctuations of light-known as the shot-noise limit. To improve the sensing performance of these sensors beyond the classical limit, quantum resources are increasingly being employed. This area of research has become known as "quantum plasmonic sensing", and it has experienced substantial activity in recent years for applications in chemical and biological sensing. This review aims to cover both plasmonic and quantum techniques for sensing, and it shows how they have been merged to enhance the performance of plasmonic sensors beyond traditional methods. We discuss the general framework developed for quantum plasmonic sensing in recent years, covering the basic theory behind the advancements made, and describe the important works that made these advancements. We also describe several key works in detail, highlighting their motivation, the working principles behind them, and their future impact. The intention of the review is to set a foundation for a burgeoning field of research that is currently being explored out of intellectual curiosity and for a wide range of practical applications in biochemistry, medicine, and pharmaceutical research.

Exploiting geometric biases in inverse nano-optical problems using artificial neural networks.

Solving the inverse problem is a major challenge in contemporary nano-optics. However, frequently not just a possible solution needs to be found but rather the solution that accommodates constraints imposed by the problem at hand. To select the most plausible solution for a nano-optical inverse problem additional information can be used in general, but how to specifically formulate it frequently remains unclear. Here, while studying the reconstruction of the shape of an object using the electromagnetic field in its proximity, we show how to take advantage of artificial neural networks (ANNs) to produce solutions consistent with prior assumptions concerning the structures. By preparing suitable datasets where the specific shapes of possible scatterers are defined, the ANNs learn the underlying scatterer present in the datasets. This helps to find a plausible solution to the otherwise non-unique inverse problem. We show that topology optimization, in contrast, can fail to recover the scatterer geometry meaningfully but a hybrid approach that is based on both, ANNs and a topology optimization, eventually leads to the most promising performance. Our work has direct implications in fields such as optical metrology.

Modeling four-dimensional metamaterials: a T-matrix approach to describe time-varying metasurfaces.

Exploring the interaction of light with materials periodically structured in space and time is intellectually rewarding and, simultaneously, a computational challenge. Appropriate computational tools are urgently needed to explore how such upcoming photonic materials can control light on demand. Here, we introduce a semi-analytical approach based on the transition matrix (also known as T-matrix) to analyze the optical response of a spatiotemporal metasurface. The metasurface consists of a periodic arrangement of time-varying scattering particles. In our approach, we depart from an individual scatterer's T-matrix to construct the effective T-matrix of the metasurface. From that effective T-matrix, all observable properties can reliably be predicted. We verify our semi-analytical approach with full-wave numerical simulations. We demonstrate a speed-up with our approach by a factor of more than 500 compared to a finite-element simulation. Finally, we exemplify our approach by studying the effect of time modulation on a Huygens' metasurface and discuss some emerging observable features.

Transformation-optics modeling of 3D-printed freeform waveguides.

Multi-photon lithography allows us to complement planar photonic integrated circuits (PIC) by in-situ 3D-printed freeform waveguide structures. However, design and optimization of such freeform waveguides using time-domain Maxwell's equations solvers often requires comparatively large computational volumes, within which the structure of interest only occupies a small fraction, thus leading to poor computational efficiency. In this paper, we present a solver-independent transformation-optics-(TO-) based technique that allows to greatly reduce the computational effort related to modeling of 3D freeform waveguides. The concept relies on transforming freeform waveguides with curved trajectories into equivalent waveguide structures with modified material properties but geometrically straight trajectories, that can be efficiently fit into rather small cuboid-shaped computational volumes. We demonstrate the viability of the technique and benchmark its performance using a series of different freeform waveguides, achieving a reduction of the simulation time by a factor of 3-6 with a significant potential for further improvement. We also fabricate and experimentally test the simulated waveguides by 3D-printing on a silicon photonic chip, and we find good agreement between the simulated and the measured transmission at λ = 1550 nm.

Modeling and measuring plasmonic excitations in hollow spherical gold nanoparticles.

We investigate molecular plasmonic excitations sustained in hollow spherical gold nanoparticles using time-dependent density functional theory (TD-DFT). Specifically, we consider Au60 spherical, hollow molecules as a toy model for single-shell plasmonic molecules. To quantify the plasmonic character of the excitations obtained from TD-DFT, the energy-based plasmonicity index is generalized to the framework of DFT, validated on simple systems such as the sodium Na20 chain and the silver Ag20 compound, and subsequently successfully applied to more complex molecules. We also compare the quantum mechanical TD-DFT simulations to those obtained from a classical Mie theory that relies on macroscopic electrodynamics to model the light-matter interaction. This comparison allows us to distinguish those features that can be explained classically from those that require a quantum-mechanical treatment. Finally, a double-shell system obtained by placing a C60 buckyball inside the hollow spherical gold particle is further considered. It is found that the double-shell, while increasing the overall plasmonic character of the excitations, leads to significantly lowered absorption cross sections.

Self-stabilizing curved metasurfaces as a sail for light-propelled spacecrafts.

Laser-driven spacecrafts are promising candidates for explorations to outer space. These spacecrafts should accelerate to a fraction of the speed of light upon illumination with earth-based laser systems. There are several challenges for such an ambitious mission that needs to be addressed yet. A matter of utmost importance is the stability of the spacecraft during the acceleration. Furthermore, the spacecraft sails should effectively reflect the light without absorptive-overheating. To address these requirements, we propose the design of a lightweight, low-absorbing, high-reflective, and self-stabilizing curved metasurface made from c-Si nanoparticles. A method to determine the stability is presented and, based on the multipole expansion method, the rotational stability of the curved metasurfaces is examined and the optimal operating regime is identified. The curvature is shown to be beneficial for the overall stability of the metasurface. The validity of the method is verified through numerical simulations of the time evolution of the trajectory of an identified metasurface. The results show that curved metasurfaces are a promising candidate for laser-driven spacecrafts.

Artificial neural networks used to retrieve effective properties of metamaterials.

We propose using deep neural networks for the fast retrieval of effective properties of metamaterials based on their angular-dependent reflection and transmission spectra from thin slabs. While we noticed that non-uniqueness is an issue for a successful application, we propose as a solution an automatic algorithm to subdivide the entire parameter space. Then, in each sub-space, the mapping between the optical response (complex reflection and transmission coefficients) and the corresponding material parameters (dielectric permittivity and permeability) is unique. We show that we can easily train one neural network per sub-space. For the final parameter retrieval, predictions from the different sub-networks are compared, and the one with the smallest error expresses the desired effective properties. Our approach allows a significant reduction in run-time, compared to more traditional least-squares fitting. Using deep neural networks to retrieve effective properties of metamaterials is a significant showcase for the application of AI technology to nanophotonic problems. Once trained, the nets can be applied to retrieve properties of a larger number of different metamaterials.

Light-trapping structures for planar solar cells inspired by transformation optics.

Optimal light absorption is decisive in obtaining high-efficiency solar cells. An established, if not to say the established, approach is to texture the interface of the light-absorbing layer with a suitable microstructure. However, structuring the light-absorbing layer is detrimental concerning its electrical properties due to an increased surface recombination rate (owing to enlarged surface area and surface defects) caused by the direct patterning process itself. This effect lowers the efficiency of the final solar cells. To circumvent this drawback, this work theoretically explores a transformation optics (TrO) inspired approach to map the nanopatterned texture onto a planar equivalent. This offers a pattern with the same optical functionality but with much improved electrical properties. Schwarz-Christoffel mappings are used for ensuring conformality of the maps. It leads to planar, inhomogeneous, dielectric-only materials for the light trapping structure to be placed on top of the planar light-absorbing layer. Such a design strategy paves a way towards a novel approach for implementing light-trapping structures into planar solar cells.

Annual energy yield of mono- and bifacial silicon heterojunction solar modules with high-index dielectric nanodisk arrays as anti-reflective and light trapping structures.

While various nanophotonic structures applicable to relatively thin crystalline silicon-based solar cells were proposed to ensure effective light in-coupling and light trapping in the absorber, it is of great importance to evaluate their performance on the solar module level under realistic irradiation conditions. Here, we analyze the annual energy yield of relatively thin (crystalline silicon (c-Si) wafer thickness between 5 µm and 80 µm) heterojunction (HJT) solar module architectures when optimized anti-reflective and light trapping titanium dioxide (TiO2) nanodisk square arrays are applied on the front and rear cell interfaces, respectively. Our numerical study shows that upon reducing c-Si wafer thickness down to 5 µm, the relative increase of the annual energy yield can go up to 23.3 %rel and 43.0 %rel for mono- and bifacial solar modules, respectively, when compared to the reference modules with flat optimized anti-reflective coatings of HJT solar cells.

Boosting Light Emission from Single Hydrogen Phthalocyanine Molecules by Charging.

Interest in electroluminescence of single molecules is stimulated by the prospect of possible applications in novel light emitting devices. Recent studies provide valuable insights into the mechanisms leading to single molecule electroluminescence. Concrete information on how to boost the intensity of the emitted light, however, is rare. By combining scanning tunnelling microscopy (STM) and quantum chemical calculations, we show that the light emission efficiencies of an individual hydrogen-phthalocyanine molecule can be increased by a factor of ≈19 upon charging. This boost in intensity can be explained by the development of a vertical dipole moment normal to the substrate facilitating out-coupling of the local excitation to the far field. As this effect is not related to the specific nature of hydrogen-phthalocyanine, it opens up a general way to increase light emission from molecular junctions.

Minimalist Mie coefficient model.

When considering light scattering from a sphere, the ratios between the expansion coefficients of the scattered and the incident field in a spherical basis are known as the Mie coefficients. Generally, Mie coefficients depend on many degrees of freedom, including the dimensions and electromagnetic properties of the spherical object. However, for fundamental research, it is important to have easy expressions for all possible values of Mie coefficients within the existing physical constraints and which depend on the least number of degrees of freedom. While such expressions are known for spheres made from non-absorbing materials, we present here, for the first time to our knowledge, corresponding expressions for spheres made from absorbing materials. To illustrate the usefulness of these expressions, we investigate the upper bound for the absorption cross section of a trimer made from electric dipolar spheres. Given the results, we have designed a dipolar ITO trimer that offers a maximal absorption cross section. Our approach is not limited to dipolar terms, but indeed, as demonstrated in the manuscript, can be applied to higher order terms as well. Using our model, one can scan the entire accessible parameter space of spheres for specific functionalities in systems made from spherical scatterers.

Helicity-Preserving Optical Cavity Modes for Enhanced Sensing of Chiral Molecules.

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 one to enhance the CD signal by more than 2 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.

Computation of Electromagnetic Properties of Molecular Ensembles.

We outline a methodology for efficiently computing the electromagnetic response of molecular ensembles. The methodology is based on the link that we establish between quantum-chemical simulations and the transfer matrix (T-matrix) approach, a common tool in physics and engineering. We exemplify and analyze the accuracy of the methodology by using the time-dependent Hartree-Fock theory simulation data of a single chiral molecule to compute the T-matrix of a cross-like arrangement of four copies of the molecule, and then computing the circular dichroism of the cross. The results are in very good agreement with full quantum-mechanical calculations on the cross. Importantly, the choice of computing circular dichroism is arbitrary: Any kind of electromagnetic response of an object can be computed from its T-matrix. We also show, by means of another example, how the methodology can be used to predict experimental measurements on a molecular material of macroscopic dimensions. This is possible because, 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 a large number of molecules, as well as for periodic or aperiodic molecular arrays. We identify areas of research for further improving the accuracy of the method, as well as new fundamental and technological research avenues based on the use of the T-matrices of molecules and molecular ensembles for quantifying their degrees of symmetry breaking. We provide T-matrix-based formulas for computing traditional chiro-optical properties like (oriented) circular dichroism, and also for quantifying electromagnetic duality and electromagnetic chirality. The formulas are valid for light-matter interactions of arbitrarily-high multipolar orders.

Manipulation of Magnetic Dipole Emission from Eu3+ with Mie-Resonant Dielectric Metasurfaces.

Mie-resonant high-index dielectric nanoparticles and metasurfaces have been suggested as a viable platform for enhancing both electric and magnetic dipole transitions of fluorescent emitters. While the enhancement of the electric dipole transitions by such dielectric nanoparticles has been demonstrated experimentally, the case of magnetic-dipole transitions remains largely unexplored. Here, we study the enhancement of spontaneous emission of Eu3+ ions, featuring both electric and magnetic-dominated dipole transitions, by dielectric metasurfaces composed of Mie-resonant silicon nanocylinders. By coating the metasurfaces with a layer of an Eu3+ doped polymer, we observe an enhancement of the Eu3+ emission associated with the electric (at 610 nm) and magnetic-dominated (at 590 nm) dipole transitions. The enhancement factor depends systematically on the spectral proximity of the atomic transitions to the Mie resonances as well as their multipolar order, both controlled by the nanocylinder size. Importantly, the branching ratio of emission via the electric or magnetic transition channel can be modified by carefully designing the metasurface, where the magnetic dipole transition is enhanced more than the electric transition for cylinders with radii of about 130 nm. We confirm our observations by numerical simulations based on the reciprocity principle. Our results open new opportunities for bright nanoscale light sources based on magnetic transitions.

Computational rule-based approach for corner correction of non-Manhattan geometries in mask aligner photolithography.

In proximity mask aligner photolithography, diffraction of light at the mask pattern is the predominant source for image shape distortions such as line end shortening and corner rounding. One established method to mitigate the impact of diffraction is optical proximity correction. This method relies on a deliberate sub-resolution modification of photomask features to counteract such shape distortions, with the goal to improve pattern fidelity and uniformity of printed features. While previously considered for masks featuring only rectangular shapes in horizontal or vertical orientation, called Manhatten geometries, we demonstrate here the capabilities of computational mask aligner lithography by extending optical proximity correction to non-Manhattan geometries. We combine a rigorous simulation method for light propagation with a particle-swarm optimization to identify suitable mask patterns adapt to each occurring feature in the mask. The improvement in pattern quality is demonstrated in experimental prints. Our method extends the use of proximity lithography in optical manufacturing, as required in a multitude of micro-optical devices.