High-performance designs for fiber-pigtailed quantum-light sources based on quantum dots in electrically-controlled circular Bragg gratings.

We present a numerical investigation of directly fiber-coupled hybrid circular Bragg gratings (CBGs) featuring electrical control for operation in the application relevant wavelength regimes around 930 nm as well as the telecom O- and C-band. We use a surrogate model combined with a Bayesian optimization approach to perform numerical optimization of the device performance which takes into account robustness with respect to fabrication tolerances. The proposed high-performance designs combine hybrid CBGs with a dielectric planarization and a transparent contact material, enabling > 86% direct fiber coupling efficiency (> 93% efficiency into NA 0.8) while exhibiting Purcell factors > 20. Especially the proposed designs for the telecom range prove robust and can sustain expected fiber efficiencies of more than (82.2±4.1)-5.5+2.2% and expected average Purcell factors of up to (23.2±2.3)-3.0+3.2 assuming conservative fabrication accuracies. The wavelength of maximum Purcell enhancement proves to be the most affected performance parameter by the deviations. Finally, we show that electrical field strengths suitable for Stark-tuning of an embedded quantum dot can be reached in the identified designs. Our work provides blueprints for high-performance quantum light sources based on fiber-pigtailed and electrically-controlled quantum dot CBG devices for quantum information applications.

Onset of Chirality in Plasmonic Meta-Molecules and Dielectric Coupling.

Chirality is a fundamental feature in all domains of nature, ranging from particle physics over electromagnetism to chemistry and biology. Chiral objects lack a mirror plane and inversion symmetry and therefore cannot be spatially aligned with their mirrored counterpart, their enantiomer. Both natural molecules and artificial chiral nanostructures can be characterized by their light-matter interaction, which is reflected in circular dichroism (CD). Using DNA origami, we assemble model meta-molecules from multiple plasmonic nanoparticles, representing meta-atoms accurately positioned in space. This allows us to reconstruct piece by piece the impact of varying macromolecular geometries on their surrounding optical near fields. Next to the emergence of CD signatures in the instance that we architect a third dimension, we design and implement sign-flipping signals through addition or removal of single particles in the artificial molecules. Our data and theoretical modeling reveal the hitherto unrecognized phenomenon of chiral plasmonic-dielectric coupling, explaining the intricate electromagnetic interactions within hybrid DNA-based plasmonic nanostructures.

Numerical optimization of single-mode fiber-coupled single-photon sources based on semiconductor quantum dots.

We perform extended numerical studies to maximize the overall photon coupling efficiency of fiber-coupled quantum dot single-photon sources emitting in the near-infrared and O-band and C-band. Using the finite element method, we optimize the photon extraction and fiber-coupling efficiency of quantum dot single-photon sources based on micromesas, microlenses, circular Bragg grating cavities and micropillars. The numerical simulations which consider the entire system consisting of the quantum dot source itself, the coupling lens, and the single-mode fiber, yield overall photon coupling efficiencies of up to 83%. Our work provides objectified comparability of different fiber-coupled single-photon sources and proposes optimized geometries for the realization of practical and highly efficient quantum dot single-photon sources.

Tripling the light extraction efficiency of a deep ultraviolet LED using a nanostructured p-contact.

Despite a wide array of applications, deep ultra-violet light emitting diodes offer relatively poor efficiencies compared to their optical counterparts. A contributing factor is the lower light extraction efficiency due to both highly absorbing p-contacts and total internal reflection. Here, we propose a structure consisting of a hexagonal periodic array of cylindrical nanoholes in the multi-layered p-contact which are filled with platinum. This nanostructure reduces the absorption of the p-contact layer, leading to a higher emission into the n-contact compared to a planar reference. An optimum geometry of the nanostructure allows a light extraction efficiency of 15.0%, much higher than the typical 4.6% of a planar reference. While the nanostructure strongly decreases the light absorption in the p-contact, it is still not able to considerably reduce the total internal reflection. Consequently, the nanostructured p-contact should be combined with other optical strategies, such as nanopatterned sapphire substrates to increase the efficiency even further. Despite this, the nanostructure described in this work provides a readily realizable path to enhancing the light extraction efficiency of state-of-the-art deep ultra-violet light emitting diodes.

Visible wavelength spectral tuning of absorption and circular dichroism of DNA-assembled Au/Ag core-shell nanorod assemblies.

Plasmonic nanoparticles have unique properties which can be harnessed to manipulate light at the nanoscale. With recent advances in synthesis protocols that increase their stability, gold-silver core-shell nanoparticles have become suitable building blocks for plasmonic nanostructures to expand the range of attainable optical properties. Here we tune the plasmonic response of gold-silver core-shell nanorods over the visible spectrum by varying the thickness of the silver shell. Through the chiral arrangement of the nanorods with the help of various DNA origami designs, the spectral tunability of the plasmon resonance frequencies is transferred into circular dichroism signals covering the spectrum from 400 nm to 700 nm. Our approach could aid in the construction of better sensors as well as metamaterials with a tunable optical response in the visible region.

Optical and Spin Properties of NV Center Ensembles in Diamond Nano-Pillars.

Nitrogen-vacancy (NV) color centers in diamond are excellent quantum sensors possessing high sensitivity and nano-scale spatial resolution. Their integration in photonic structures is often desired, since it leads to an increased photon emission and also allows the realization of solid-state quantum technology architectures. Here, we report the fabrication of diamond nano-pillars with diameters up to 1000 nm by electron beam lithography and inductively coupled plasma reactive ion etching in nitrogen-rich diamonds (type Ib) with [100] and [111] crystal orientations. The NV centers were created by keV-He ion bombardment and subsequent annealing, and we estimate an average number of NVs per pillar to be 4300 ± 300 and 520 ± 120 for the [100] and [111] samples, respectively. Lifetime measurements of the NVs' excited state showed two time constants with average values of τ1 ≈ 2 ns and τ2 ≈ 8 ns, which are shorter as compared to a single color center in a bulk crystal (τ ≈ 10 ns). This is probably due to a coupling between the NVs as well as due to interaction with bombardment-induced defects and substitutional nitrogen (P1 centers). Optically detected magnetic resonance measurements revealed a contrast of about 5% and average coherence and relaxation times of T2 [100] = 420 ± 40 ns, T2 [111] = 560 ± 50 ns, and T1 [100] = 162 ± 11 µs, T1 [111] = 174 ± 24 µs. These pillars could find an application for scanning probe magnetic field imaging.

Chiral Generation of Hot Carriers for Polarization-Sensitive Plasmonic Photocatalysis.

Mastering the manipulation of chirality at the nanoscale has long been a priority for chemists, physicists, and materials scientists, given its importance in the biochemical processes of the natural world and in the development of novel technologies. In this vein, the formation of novel metamaterials and sensing platforms resulting from the synergic combination of chirality and plasmonics has opened new avenues in nano-optics. Recently, the implementation of chiral plasmonic nanostructures in photocatalysis has been proposed theoretically as a means to drive polarization-dependent photochemistry. In the present work, we demonstrate that the use of inorganic nanometric chiral templates for the controlled assembly of Au and TiO2 nanoparticles leads to the formation of plasmon-based photocatalysts with polarization-dependent reactivity. The formation of plasmonic assemblies with chiroptical activities induces the asymmetric formation of hot electrons and holes generated via electromagnetic excitation, opening the door to novel photocatalytic and optoelectronic features. More precisely, we demonstrate that the reaction yield can be improved when the helicity of the circularly polarized light used to activate the plasmonic component matches the handedness of the chiral substrate. Our approach may enable new applications in the fields of chirality and photocatalysis, particularly toward plasmon-induced chiral photochemistry.

Optimizing metal grating back reflectors for III-V-on-silicon multijunction solar cells.

Multi-junction solar cells allow to utilize sunlight more effectively than single junction solar cells. In this work, we present optical simulations of III-V-on-silicon solar cells with a metal grating at the back, which experimentally have reached more than 33% power conversion efficiency. First, we perform simulations with the finite element method and compare them with experimental data to validate our model. We find that accurately modeling the investigated geometrical structure is necessary for best agreement between simulation and experimental measurements. Then, we optimize the grating for maximized light trapping using a computationally efficient Bayesian optimization algorithm. The photo current density of the limiting silicon bottom cell is improved from 13.48 mA/cm2 for the experimental grating to 13.85 mA/cm2 for the optimized metal grating. Investigation of all geometrical optimization parameters of the grating (period, height,…) shows that the structure is most sensitive towards the period, a parameter highly controllable in manufacturing by inference lithography. The results show a pathway to exceed the current world record efficiency of the III-V-on-silicon solar cell technology.

Axial localization and tracking of self-interference nanoparticles by lateral point spread functions.

Sub-diffraction limited localization of fluorescent emitters is a key goal of microscopy imaging. Here, we report that single upconversion nanoparticles, containing multiple emission centres with random orientations, can generate a series of unique, bright and position-sensitive patterns in the spatial domain when placed on top of a mirror. Supported by our numerical simulation, we attribute this effect to the sum of each single emitter's interference with its own mirror image. As a result, this configuration generates a series of sophisticated far-field point spread functions (PSFs), e.g. in Gaussian, doughnut and archery target shapes, strongly dependent on the phase difference between the emitter and its image. In this way, the axial locations of nanoparticles are transferred into far-field patterns. We demonstrate a real-time distance sensing technology with a localization accuracy of 2.8 nm, according to the atomic force microscope (AFM) characterization values, smaller than 1/350 of the excitation wavelength.

Long- and short-ranged chiral interactions in DNA-assembled plasmonic chains.

Circular dichroism (CD) has long been used to trace chiral molecular states and changes of protein configurations. In recent years, chiral plasmonic nanostructures have shown potential for applications ranging from pathogen sensing to novel optical materials. The plasmonic coupling of the individual elements of such metallic structures is a crucial prerequisite to obtain sizeable CD signals. We here identify and implement various coupling entities-chiral and achiral-to demonstrate chiral transfer over distances close to 100 nm. The coupling is realized by an achiral nanosphere situated between a pair of gold nanorods that are arranged far apart but in a chiral fashion using DNA origami. The transmitter particle causes a strong enhancement of the CD response, the emergence of an additional chiral feature at the resonance frequency of the nanosphere, and a redshift of the longitudinal plasmonic resonance frequency of the nanorods. Matching numerical simulations elucidate the intricate chiral optical fields in complex architectures.

Quasi-bound states in the continuum for deep subwavelength structural information retrieval for DUV nano-optical polarizers.

We demonstrate the retrieval of deep subwavelength structural information in nano-optical polarizers by scatterometry of quasi-bound states in the continuum (quasi-BICs). To this end, we investigate titanium dioxide wire grid polarizers for application wavelengths in the deep ultraviolet (DUV) spectral range fabricated with a self-aligned double-patterning process. In contrast to the time-consuming and elaborate measurement techniques like scanning electron microscopy, asymmetry induced quasi-BICs occurring in the near ultraviolet and visible spectral range provide an easily accessible and efficient probe mechanism. Thereby, dimensional parameters are retrieved with uncertainties in the sub-nanometer range. Our results show that BICs are a promising tool for process control in optics and semiconductor technology.

General design formalism for highly efficient flat optics for broadband applications.

The use of flat diffractive optical elements (DOEs) for broadband applications, e.g. conventional optical systems, requires DOEs that maintain high efficiencies across the required range of wavelengths, angles of incidence, and grating periods. Here we introduce a general framework for how dispersion engineering can be used to design DOEs that fulfill these requirements and use our approach to determine design rules for broadband DOEs. Our analysis shows that the key to making échelette-type gratings (EGs) suitable for broadband optical systems is the development of new optical materials with specific uncommon dispersion properties. Subsequently, we use our framework to design a representative range of prototype EGs, which allows us to link the specifications of an optical system to the requirements on the EGs' materials. Finally, we show that our design rules apply to all DOEs based on propagation delays including GRIN DOEs and metagratings. Our design rules therefore guide the way towards unlocking the full potential of DOEs for different kinds of broadband applications.

Nanopatterned sapphire substrates in deep-UV LEDs: is there an optical benefit?

Light emitting diodes (LEDs) in the deep ultra-violet (DUV) offer new perspectives for multiple applications ranging from 3D printing to sterilization. However, insufficient light extraction severely limits their efficiency. Nanostructured sapphire substrates in aluminum nitride based LED devices have recently shown to improve crystal growth properties, while their impact on light extraction has not been fully verified. We present a model for understanding the impact of nanostructures on the light extraction capability of DUV-LEDs. The model assumes an isotropic light source in the semiconductor layer stack and combines rigorously computed scattering matrices with a multilayer solver. We find that the optical benefit of using a nanopatterned as opposed to a planar sapphire substrate to be negligible, if parasitic absorption in the p-side of the LED is dominant. If losses in the p-side are reduced to 20%, then for a wavelength of 265 nm an increase of light extraction efficiency from 7.8% to 25.0% is possible due to nanostructuring. We introduce a concept using a diffuse ('Lambertian') reflector as p-contact, further increasing the light extraction efficiency to 34.2%. The results underline that transparent p-sides and reflective p-contacts in DUV-LEDs are indispensable for enhanced light extraction regardless of the interface texture between semiconductor and sapphire substrate. The optical design guidelines presented in this study will accelerate the development of high-efficiency DUV-LEDs. The model can be extended to other multilayer opto-electronic nanostructured devices such as photovoltaics or photodetectors.

Hot Electrons Generated in Chiral Plasmonic Nanocrystals as a Mechanism for Surface Photochemistry and Chiral Growth.

The realization of chiral photochemical reactions at the molecular level has proven to be a challenging task, with invariably low efficiencies originating from very small optical circular dichroism signals. On the contrary, colloidal nanocrystals offer a very large differential response to circularly polarized light when designed with chiral geometries. We propose taking advantage of this capability, introducing a novel mechanism driving surface photochemistry in a chiral nanocrystal. Plasmonic nanocrystals exhibit anomalously large asymmetry factors in optical circular dichroism (CD), and the related hot-electron generation shows in turn a very strong asymmetry, serving as a mechanism for chiral growth. Through theoretical modeling, we show that chiral plasmonic nanocrystals can enable chiral surface growth based on the generation of energetic (hot) electrons. Using simple and realistic phenomenological models, we illustrate how this kind of surface photochemistry can be observed experimentally. The proposed mechanism is efficient if it operates on an already strongly chiral nanocrystal, whereas our proposed mechanism does not show chiral growth for initially nonchiral structures in a solution. The asymmetry factors for the chiral effects, driven by hot electrons, exceed the values observed in chiral molecular photophysics at least 10-fold. The proposed chiral-growth mechanism for the transformation of plasmonic colloids is fundamentally different to the traditional schemes of chiral photochemistry at the molecular level.

Method for direct coupling of a semiconductor quantum dot to an optical fiber for single-photon source applications.

We present an effective method for direct fiber coupling of a quantum dot (QD) that is deterministically incorporated into a cylindrical mesa. For precise positioning of the fiber with respect to the QD-mesa, we use a scanning procedure relying on interference of light reflected back from the fiber end-face and the top surface of the mesa, applicable for both single-mode and multi-mode fibers. The central part of the fiber end-face is etched to control the required distance between the top surface of the mesa and the fiber core. Emission around 1260 nm from a fiber-coupled InGaAs/GaAs QD is demonstrated and its stability is proven over multiple cooling cycles. Moreover, a single photon character of emission from such system for a line emitting above 1200 nm is proven experimentally by photon autocorrelation measurements with an obtained value of the second order correlation function at zero time-delay well below 0.5.

Correlation of circular differential optical absorption with geometric chirality in plasmonic meta-atoms.

We report a strong correlation between the calculated broadband circular differential optical absorption (CDOA) and the geometric chirality of plasmonic meta-atoms with two-dimensional chirality. We investigate this correlation using three common gold meta-atom geometries: L-shapes, triangles, and nanorod dimers, over a broad range of geometric parameters. We show that this correlation holds for both contiguous plasmonic meta-atoms and non-contiguous structures which support plasmonic coupling effects. A potential application for this correlation is the rapid optimization of plasmonic nanostructure for maximum broadband CDOA.

Numerical optimization of the extraction efficiency of a quantum-dot based single-photon emitter into a single-mode fiber.

We present a numerical method for the accurate and efficient simulation of strongly localized light sources, such as quantum dots, embedded in dielectric micro-optical structures. We apply the method in order to optimize the photon extraction efficiency of a single-photon emitter consisting of a quantum dot embedded into a multi-layer stack with further lateral structures. Furthermore, we present methods to study the robustness of the extraction efficiency with respect to fabrication errors and defects.

Benchmarking five numerical simulation techniques for computing resonance wavelengths and quality factors in photonic crystal membrane line defect cavities.

We present numerical studies of two photonic crystal membrane microcavities, a short line-defect cavity with a relatively low quality (Q) factor and a longer cavity with a high Q. We use five state-of-the-art numerical simulation techniques to compute the cavity Q factor and the resonance wavelength λ for the fundamental cavity mode in both structures. For each method, the relevant computational parameters are systematically varied to estimate the computational uncertainty. We show that some methods are more suitable than others for treating these challenging geometries.

Deterministic Integration of Quantum Dots into on-Chip Multimode Interference Beamsplitters Using in Situ Electron Beam Lithography.

The development of multinode quantum optical circuits has attracted great attention in recent years. In particular, interfacing quantum-light sources, gates, and detectors on a single chip is highly desirable for the realization of large networks. In this context, fabrication techniques that enable the deterministic integration of preselected quantum-light emitters into nanophotonic elements play a key role when moving forward to circuits containing multiple emitters. Here, we present the deterministic integration of an InAs quantum dot into a 50/50 multimode interference beamsplitter via in situ electron beam lithography. We demonstrate the combined emitter-gate interface functionality by measuring triggered single-photon emission on-chip with g(2)(0) = 0.13 ± 0.02. Due to its high patterning resolution as well as spectral and spatial control, in situ electron beam lithography allows for integration of preselected quantum emitters into complex photonic systems. Being a scalable single-step approach, it paves the way toward multinode, fully integrated quantum photonic chips.

On accurate simulations of thin-film solar cells with a thick glass superstrate.

The optical response of periodically nanotextured layer stacks with dimensions comparable to the wavelength of the incident light can be computed with rigorous Maxwell solvers, such as the finite element method (FEM). Experimentally, such layer stacks are often prepared on glass superstrates with a thickness, which is orders of magnitude larger than the wavelength. For many applications, light in these thick superstrates can be treated incoherently. The front side of thick superstrate is located far away from the computational domain of the Maxwell solvers. Nonetheless, it has to be considered in order to achieve accurate results. In this contribution, we discuss how solutions of rigorous Maxwell solvers can be corrected for flat front sides of the superstrates with an incoherent a posteriori approach. We test these corrections for hexagonal sinusoidal nanotextured silica-silicon interfaces, which are applied in certain silicon thin-film solar cells. These corrections are determined via a scattering matrix, which contains the full scattering information of the periodically nanotextured structure. A comparison with experimental data reveals that higher-order corrections can predict the measured reflectivity of the samples much better than an often-applied zeroth-order correction.