Dynamic circular birefringence response with fractured geometric phase metasurface systems.

Control over symmetry breaking in three-dimensional electromagnetic systems offers a pathway to tailoring their optical activity. We introduce fractured Pancharatnam­Berry-phase metasurface systems, in which a full-waveplate geometric phase metasurface is fractured into two half-waveplate-based metasurfaces and actively configured using shear displacement. Local relative rotations between stacked half-nanowaveplates within the metasurface system are transduced by shear displacement, leading to dynamic modulation of their collective geometric phase properties. We apply this concept to pairs of periodic Pancharatnam­Berry-phase metasurfaces and experimentally show that these systems support arbitrary and reconfigurable broadband circular birefringence response. High-speed circular birefringence modulation is demonstrated with modest shearing speeds, indicating the potential for these concepts to dynamically control polarization states with fast temporal responses. We anticipate that fractured geometric phase metasurface systems will serve as a nanophotonic platform that leverages systems-level symmetry breaking to enable active electromagnetic wave control.

Thermoelectric response from grain boundaries and lattice distortions in crystalline gold devices.

The electronic Seebeck response in a conductor involves the energy-dependent mean free path of the charge carriers and is affected by crystal structure, scattering from boundaries and defects, and strain. Previous photothermoelectric (PTE) studies have suggested that the thermoelectric properties of polycrystalline metal nanowires are related to grain structure, although direct evidence linking crystal microstructure to the PTE response is difficult to elucidate. Here, we show that room temperature scanning PTE measurements are sensitive probes that can detect subtle changes in the local Seebeck coefficient of gold tied to the underlying defects and strain that mediate crystal deformation. This connection is revealed through a combination of scanning PTE and electron microscopy measurements of single-crystal and bicrystal gold microscale devices. Unexpectedly, the photovoltage maps strongly correlate with gradually varying crystallographic misorientations detected by electron backscatter diffraction. The effects of individual grain boundaries and differing grain orientations on the PTE signal are minimal. This scanning PTE technique shows promise for identifying minor structural distortions in nanoscale materials and devices.

Electrically Driven Hyperbolic Nanophotonic Resonators as High Speed, Spectrally Selective Thermal Radiators.

We introduce and experimentally demonstrate electrically driven, spectrally selective thermal emitters based on globally aligned carbon nanotube metamaterials. The self-assembled metamaterial supports a high degree of nanotube ordering, enabling nanoscale ribbons patterned in the metamaterial to function both as Joule-heated incandescent filaments and as infrared hyperbolic resonators imparting spectral selectivity to the thermal radiation. Devices batch-fabricated on a single chip emit polarized thermal radiation with peak wavelengths dictated by their hyperbolic resonances, and their nanoscale heated dimensions yield modulation rates as high as 1 MHz. As a proof of concept, we show that two sets of thermal emitters on the same chip, operating with different peak wavelengths and modulation rates, can be used to sense carbon dioxide with one detector. We anticipate that the combination of batch fabrication, modulation bandwidth, and spectral tuning with chip-based nanotube thermal emitters will enable new modalities in multiplexed infrared sources.

Single-crystal metal growth on amorphous insulating substrates.

Metal structures on insulators are essential components in advanced electronic and nanooptical systems. Their electronic and optical properties are closely tied to their crystal quality, due to the strong dependence of carrier transport and band structure on defects and grain boundaries. Here we report a method for creating patterned single-crystal metal microstructures on amorphous insulating substrates, using liquid phase epitaxy. In this process, the patterned metal microstructures are encapsulated in an insulating crucible, together with a small seed of a differing material. The system is heated to temperatures above the metal melting point, followed by cooling and metal crystallization. During the heating process, the metal and seed form a high-melting-point solid solution, which directs liquid epitaxial metal growth. High yield of single-crystal metal with different sizes is confirmed with electron backscatter diffraction images, after removing the insulating crucible. Unexpectedly, the metal microstructures crystallize with the [Formula: see text] direction normal to the plane of the film. This platform technology will enable the large-scale integration of high-performance plasmonic and electronic nanosystems.

MetaNet: a new paradigm for data sharing in photonics research.

Optimization methods are playing an increasingly important role in all facets of photonics engineering, from integrated photonics to free space diffractive optics. However, efforts in the photonics community to develop optimization algorithms remain uncoordinated, which has hindered proper benchmarking of design approaches and access to device designs based on optimization. We introduce MetaNet, an online database of photonic devices and design codes intended to promote coordination and collaboration within the photonics community. Using metagratings as a model system, we have uploaded over one hundred thousand device layouts to the database, as well as source code for implementations of local and global topology optimization methods. Further analyses of these large datasets allow the distribution of optimized devices to be visualized for a given optimization method. We expect that the coordinated research efforts enabled by MetaNet will expedite algorithm development for photonics design.

Global Optimization of Dielectric Metasurfaces Using a Physics-Driven Neural Network.

We present a global optimizer, based on a conditional generative neural network, which can output ensembles of highly efficient topology-optimized metasurfaces operating across a range of parameters. A key feature of the network is that it initially generates a distribution of devices that broadly samples the design space and then shifts and refines this distribution toward favorable design space regions over the course of optimization. Training is performed by calculating the forward and adjoint electromagnetic simulations of outputted devices and using the subsequent efficiency gradients for backpropagation. With metagratings operating across a range of wavelengths and angles as a model system, we show that devices produced from the trained generative network have efficiencies comparable to or better than the best devices produced by adjoint-based topology optimization, while requiring less computational cost. Our reframing of adjoint-based optimization to the training of a generative neural network applies generally to physical systems that can utilize gradients to improve performance.

Tunable Hyperbolic Metamaterials Based on Self-Assembled Carbon Nanotubes.

We show that packed, horizontally aligned films of single-walled carbon nanotubes are hyperbolic metamaterials with ultrasubwavelength unit cells and dynamic tunability. Using Mueller matrix ellipsometry, we characterize the films' optical properties, which are doping level dependent, and find a broadband hyperbolic region tunable in the mid-infrared. To characterize the dispersion of in-plane hyperbolic plasmon modes, we etch the nanotube films into nanoribbons with differing widths and orientations relative to the nanotube axis, and we observe that the hyperbolic modes support strong light localization. An agreement between the experiments and theoretical models using the ellipsometry data indicates that the packed carbon nanotubes support bulk anisotropic responses at the nanoscale. Self-assembled films of carbon nanotubes are well-suited for applications in thermal emission and photodetection, and they serve as model systems for studying light-matter interactions in the deep subwavelength regime.

Large-Angle, Multifunctional Metagratings Based on Freeform Multimode Geometries.

We show that silicon-based metagratings capable of large-angle, multifunctional performance can be realized using inverse freeform design. These devices consist of nonintuitive nanoscale patterns and support a large number of spatially overlapping optical modes per unit area. The quantity of modes, in combination with their optimized responses, provides the degrees of freedom required to produce high-efficiency devices. To demonstrate the power and versatility of our approach, we fabricate metagratings that can efficiently deflect light to 75° angles and multifunctional devices that can steer beams to different diffraction orders based on wavelength. A theoretical analysis of the Bloch modes supported by these devices elucidates the spatial mode profiles and coupling dynamics that make high-performance beam deflection possible. This approach represents a new paradigm in nano-optical mode engineering and utilizes different physics from the current state-of-the-art, which is based on the stitching of noninteracting waveguide structures. We envision that inverse design will enable new classes of high-performance photonic systems and new strategies toward the nanoscale control of light fields.

Analysis of material selection on dielectric metasurface performance.

Dielectric metasurfaces are ultra-thin devices that can shape optical wavefronts with extreme control. While an assortment of materials possessing a wide range of dielectric constants have been proposed and implemented, the minimum dielectric contrast required for metasurfaces to achieve high-efficiency performance, for a given device function and feature size constraint, is unclear. In this Article, we examine the impact of dielectric material selection on metasurface efficiency at optical frequencies. As a model system, we design transmissive, single-layer periodic metasurfaces (i.e., metagratings) using topology optimization, and we sweep device thickness and light deflection angle for differing material types. We find that for modest deflection angles below 40 degrees, materials with relatively low dielectric constants near 4 can be used to produce metagratings with efficiencies over 80%. However, ultra-high-efficiency devices designed for large deflection angles and multiple functions require materials with high dielectric constants comparable to silicon. We also identify, for all materials, a minimum device thickness required for optimal metagrating performance that scales inversely with dielectric constant. Our work presents materials selection guidelines for high-performance metasurfaces operating at visible and infrared wavelengths.

Topology-optimized metasurfaces: impact of initial geometric layout.

Topology optimization is a powerful iterative inverse design technique in metasurface engineering and can transform an initial layout into a high-performance device. With this method, devices are optimized within a local design phase space, making the identification of suitable initial geometries essential. In this Letter, we examine the impact of initial geometric layout on the performance of large-angle (75 deg) topology-optimized metagrating deflectors. We find that when conventional metasurface designs based on dielectric nanoposts are used as initial layouts for topology optimization, the final devices have efficiencies around 65%. In contrast, when random initial layouts are used, the final devices have ultra-high efficiencies that can reach 94%. Our numerical experiments suggest that device topologies based on conventional metasurface designs may not be suitable to produce ultra-high-efficiency, large-angle metasurfaces. Rather, initial geometric layouts with non-trivial topologies and shapes are required.

Oxygen vacancy promoted methane partial oxidation over iron oxide oxygen carriers in the chemical looping process.

We perform ab initio DFT+U calculations and experimental studies of the partial oxidation of methane to syngas on iron oxide oxygen carriers to elucidate the role of oxygen vacancies in oxygen carrier reactivity. In particular, we explore the effect of oxygen vacancy concentration on sequential processes of methane dehydrogenation, and oxidation with lattice oxygen. We find that when CH4 adsorbs onto Fe atop sites without neighboring oxygen vacancies, it dehydrogenates with CHx radicals remaining on the same site and evolves into CO2via the complete oxidation pathway. In the presence of oxygen vacancies, on the other hand, the formed methyl (CH3) prefers to migrate onto the vacancy site while the H from CH4 dehydrogenation remains on the original Fe atop site, and evolves into CO via the partial oxidation pathway. The oxygen vacancies created in the oxidation process can be healed by lattice oxygen diffusion from the subsurface to the surface vacancy sites, and it is found that the outward diffusion of lattice oxygen atoms is more favorable than the horizontal diffusion on the same layer. Based on the proposed mechanism and energy profile, we identify the rate-limiting steps of the partial oxidation and complete oxidation pathways. Also, we find that increasing the oxygen vacancy concentration not only lowers the barriers of CH4 dehydrogenation but also the cleavage energy of Fe-C bonds. However, the barrier of the rate-limiting step cannot further decrease when the oxygen vacancy concentration reaches 2.5%. The fundamental insight into the oxygen vacancy effect on CH4 oxidation with iron oxide oxygen carriers can help guide the design and development of more efficient oxygen carriers and CLPO processes.

Methane adsorption and dissociation on iron oxide oxygen carriers: the role of oxygen vacancies.

We performed ab initio DFT+U calculations to explore the interaction between methane and iron oxide oxygen carriers for chemical looping reaction systems. The adsorption of CH4 and CHx (x = 0-3) radicals on α-Fe2O3(001), and the influence of oxygen vacancies at the top surface and on the subsurface on the adsorption properties of the radicals was investigated. The adsorption strength for CH4 and C radicals at the top of the α-Fe2O3(001) surface in the presence of oxygen vacancies is lower than that on the stoichiometric surface. However, for methyl (CH3), methylene (CH2) and methine (CH) radicals, it is correspondingly higher. In contrast, the oxygen vacancy formation on the subsurface not only increases the adsorption strength of CH3, CH2 and CH radicals, but also facilitates C radical adsorption. We found that oxygen vacancies significantly affect the adsorption configuration of CHx radicals, and determine the probability of finding an adsorbed species in the stoichiometric region and the defective region at the surface. With the obtained adsorption geometries and energetics of these species adsorbed on the surface, we extend the analysis to CH4 dissociation under chemical looping reforming conditions. The distribution of adsorbed CH4 and CHx (x = 0-3) radicals is calculated and analyzed which reveals the relationship between adsorbed CHx radical configuration and oxygen vacancies in iron oxide. Also, the oxygen vacancies can significantly facilitate CH4 activation by lowering the dissociation barriers of CH3, CH2 and CH radicals. However, when the oxygen vacancy concentration reaches 2.67%, increasing the oxygen vacancy concentration cannot continue to lower the CH dissociation barrier. The study provides fundamental insights into the mechanism of CH4 dissociation on iron based oxygen carriers and also provide guidance to design more efficient oxygen carriers.

Elasticity of fractal inspired interconnects.

The use of fractal-inspired geometric designs in electrical interconnects represents an important approach to simultaneously achieve large stretchability and high aerial coverage of active devices for stretchable electronics. The elastic stiffness of fractal interconnects is determined analytically in this paper. Specifically, the elastic energy and the tensile stiffness for an order n fractal interconnect of arbitrary shape are obtained, and are verified by the finite element analysis and experiments.

Tunable Phonon Polariton Hybridization in a Van der Waals Hetero-Bicrystal.

Phonon polaritons, the hybrid quasiparticles resulting from the coupling of photons and lattice vibrations, have gained significant attention in the field of layered van der Waals heterostructures. Particular interest has been paid to hetero-bicrystals composed of molybdenum oxide (MoO3) and hexagonal boron nitride (hBN), which feature polariton dispersion tailorable via avoided polariton mode crossings. In this work, the polariton eigenmodes in MoO3-hBN hetero-bicrystals self-assembled on ultrasmooth gold are systematically studied using synchrotron infrared nanospectroscopy. It is experimentally demonstrated that the spectral gap in bicrystal dispersion and corresponding regimes of negative refraction can be tuned by material layer thickness, and these results are quantitatively matched with a simple analytic model. Polaritonic cavity modes and polariton propagation along "forbidden" directions are also investigated in microscale bicrystals, which arise from the finite in-plane dimension of the synthesized MoO3 micro-ribbons. The findings shed light on the unique dispersion properties of polaritons in van der Waals heterostructures and pave the way for applications leveraging deeply sub-wavelength mid-infrared light-matter interactions.

Roadmap for Optical Metasurfaces.

Metasurfaces have recently risen to prominence in optical research, providing unique functionalities that can be used for imaging, beam forming, holography, polarimetry, and many more, while keeping device dimensions small. Despite the fact that a vast range of basic metasurface designs has already been thoroughly studied in the literature, the number of metasurface-related papers is still growing at a rapid pace, as metasurface research is now spreading to adjacent fields, including computational imaging, augmented and virtual reality, automotive, display, biosensing, nonlinear, quantum and topological optics, optical computing, and more. At the same time, the ability of metasurfaces to perform optical functions in much more compact optical systems has triggered strong and constantly growing interest from various industries that greatly benefit from the availability of miniaturized, highly functional, and efficient optical components that can be integrated in optoelectronic systems at low cost. This creates a truly unique opportunity for the field of metasurfaces to make both a scientific and an industrial impact. The goal of this Roadmap is to mark this "golden age" of metasurface research and define future directions to encourage scientists and engineers to drive research and development in the field of metasurfaces toward both scientific excellence and broad industrial adoption.

Tetrahedral colloidal clusters from random parking of bidisperse spheres.

Using experiments and simulations, we investigate the clusters that form when colloidal spheres stick irreversibly to--or "park" on--smaller spheres. We use either oppositely charged particles or particles labeled with complementary DNA sequences, and we vary the ratio α of large to small sphere radii. Once bound, the large spheres cannot rearrange, and thus the clusters do not form dense or symmetric packings. Nevertheless, this stochastic aggregation process yields a remarkably narrow distribution of clusters with nearly 90% tetrahedra at α = 2.45. The high yield of tetrahedra, which reaches 100% in simulations at α = 2.41, arises not simply because of packing constraints, but also because of the existence of a long-time lower bound that we call the "minimum parking" number. We derive this lower bound from solutions to the classic mathematical problem of spherical covering, and we show that there is a critical size ratio α(c) = (1 + sqrt[2]) ≈ 2.41, close to the observed point of maximum yield, where the lower bound equals the upper bound set by packing constraints. The emergence of a critical value in a random aggregation process offers a robust method to assemble uniform clusters for a variety of applications, including metamaterials.

Plasmonic mode engineering with templated self-assembled nanoclusters.

Plasmonic nanoparticle assemblies are a materials platform in which optical modes, resonant frequencies, and near-field intensities can be specified by the number and position of nanoparticles in a cluster. A current challenge is to achieve clusters with higher yields and new types of shapes. In this Letter, we show that a broad range of plasmonic nanoshell nanoclusters can be assembled onto a lithographically defined elastomeric substrate with relatively high yields using templated assembly. We assemble and measure the optical properties of three cluster types: Fano-resonant heptamers, linear chains, and rings of nanoparticles. The yield of heptamer clusters is measured to be over 30%. The assembly of plasmonic nanoclusters on an elastomer paves the way for new classes of plasmonic nanocircuits and colloidal metamaterials that can be transfer-printed onto various substrate media.

Near-normal incidence dark-field microscopy: applications to nanoplasmonic spectroscopy.

The spectroscopic characterization of individual nanostructures is of fundamental importance to understanding a broad range of physical and chemical processes. One general and powerful technique that addresses this aim is dark-field microscopy, with which the scattered light from an individual structure can be analyzed with minimal background noise. We present the spectroscopic analysis of individual plasmonic nanostructures using dark-field illumination with incidence nearly normal to the substrate. We show that, compared to large incidence angle approaches, the near-normal incidence approach provides significantly higher signal-to-background ratios and reduced retardation field effects. To demonstrate the utility of this technique, we characterize an individual chemically synthesized gold nanoshell and a lithographically defined heptamer exhibiting a pronounced Fano-like resonance. We show that the line shape of the latter strongly depends on the incidence angle. Near-normal incidence dark-field microscopy can be used to characterize a broad range of molecules and nanostructures and can be adapted to most microscopy setups.

Polychromatic metasurfaces for complete control of phase and polarization in the mid-infrared.

Multifunctional metasurfaces based on wavelength-decoupled supercells are experimentally demonstrated, enabling new regimes of optical control for arbitrary orthogonal polarizations at different wavelengths.

Conformal Volumetric Grayscale Metamaterials.

Conformal artificial electromagnetic media that feature tailorable responses as a function of incidence wavelength and angle represent universal components for optical engineering. Conformal grayscale metamaterials are introduced as a new class of volumetric electromagnetic media capable of supporting highly multiplexed responses and arbitrary, curvilinear form factors. Subwavelength-scale voxels based on irregular shapes are designed to accommodate a continuum of dielectric values, enabling the freeform design process to reliably converge to exceptionally high figures of merit (FOMs) for a given multi-objective design problem. Through additive manufacturing of ceramic-polymer composites, microwave metamaterials, designed for the radio-frequency range of 8-12 GHz, are experimentally fabricated and devices with extreme dispersion profiles, an airfoil-shaped beam-steering device, and a broadband, broad-angle conformal carpet cloak, are demonstrated. It is anticipated that conformal volumetric metamaterials will lead to new classes of compact and multifunctional imaging, sensing, and communications systems.