Metasurface Light-Emitting Diodes with Directional and Focused Emission.

Phased-array metasurfaces enable the imprinting of complex beam structures onto coherent incident light. Recent demonstrations of photoluminescent phased-array metasurfaces highlight possibilities for achieving similar control in electroluminescent light-emitting diodes (LEDs). However, phased-array metasurface LEDs have not yet been demonstrated owing to the complexities of integrating device stacks and electrodes within nanopatterned metasurfaces. Here, we demonstrate metasurface LEDs that emit directional or focused light. We first design nanoribbon elements that achieve the requisite phase control within typical LED device constraints. Subsequently, we demonstrate unidirectional emission that can be engineered at will via phased-array concepts. This control is further exhibited in metasurface LEDs that directly emit focused beams. Finally, we show that these metasurface LEDs exhibit external quantum efficiencies (EQEs) superior to those of unpatterned LEDs. These results demonstrate metasurface designs that are compatible with high-EQE metal-free LED devices and portend opportunities for new classes of metasurface LEDs that directly produce complex beam structures.

Optical-Frequency Magnetic Polarizability in a Layered Semiconductor.

The optical response of crystals is most commonly attributed to electric dipole interactions between light and matter. Although metamaterials support "artificial" magnetic resonances supported by mesoscale structuring, there are no naturally occurring materials known to exhibit a nonzero optical-frequency magnetic polarizability. Here, we experimentally demonstrate and quantify a naturally occurring nonzero magnetic polarizability in a layered semiconductor system: two-dimensional (Ruddlesden-Popper phase) hybrid organic-inorganic perovskites. These results demonstrate the only known material with an optical-frequency permeability that differs appreciably from vacuum, informing future efforts to find, synthesize, or exploit atomic-scale optical magnetism for novel optical phenomena such as negative index of refraction and electromagnetic cloaking.

Chemical and Structural Diversity of Hybrid Layered Double Perovskite Halides.

Hybrid halide double perovskites are a class of compounds attracting growing interest because of their richness of structure and property. Two-dimensional (2D) derivatives of hybrid double perovskites are formed by the incorporation of organic spacer cations into three-dimensional (3D) double perovskites. Here, we report a series of seven new layered double perovskite halides with propylammonium (PA), octylammonium (OCA), and 1,4-butyldiammonium (BDA) cations. The general formulas of the compounds are AmMIMIIIX8 (single-layered Ruddlesden-Popper type with m = 4 and A = PA or OCA, and single-layered Dion-Jacobson type with m = 2 and A = BDA, MI = Ag, MIII= In or Bi, X = Cl or Br) and PA2CsMIMIIIBr7 (bilayered, with MI = Ag, MIII = In or Bi). These families of compounds demonstrate great versatility, with tunable layer thickness, the ability to vary the interlayer spacing, and the ability to selectively tune the band gap by varying the MI and MIII cations along with the halide anions. The band gap of the single-layered materials varies from 2.41 eV for PA4AgBiBr8 to 3.96 eV for PA4AgInCl8. Photoluminescent emission spectra of the layered double perovskites at low-temperature (100 K) are reported, and density functional theory electronic structure calculations are presented to understand the nature of the band gap evolution. The development of new structural and compositions in layered double perovskite halides enhances the understanding of structure-property relations in this important family.

Ultrawide Thermo-optic Tuning of PbTe Meta-Atoms.

Subwavelength Mie resonators have enabled new classes of optical antenna and nanophotonic devices and can act as the basic meta-atom constituents of low-loss dielectric metasurfaces. In any application, tunable Mie resonances are key to achieving a dynamic and reconfigurable operation. However, the active tuning of these nanoantennas is still limited and usually results in sub-linewidth resonance tuning. Here, we demonstrate the ultrawide dynamic tuning of PbTe Mie resonators fabricated via both laser ablation and a novel solution-processing approach. Taking advantage of the extremely large thermo-optic (TO) coefficient and a high refractive index of PbTe, we demonstrate high-quality factor Mie resonances that are tuned by several linewidths with temperature modulations as small as ΔT ∼ 10 K. We reveal that the origin for this exceptional tunability is due to an increased TO coefficient of PbTe at low temperatures. When combined into metasurface arrays, these effects can be exploited in ultranarrow active notch filers and metasurface phase shifters that require only a few kelvin modulation. These findings demonstrate the enabling potential of PbTe as a versatile, solution-processable, and highly tunable nanophotonic material that suggests new possibilities for meta-atom paints, coatings, and 3D metamaterials fabrication.

Enhancing Organic Semiconductor-Surface Plasmon Polariton Coupling with Molecular Orientation.

Due to strong electric field enhancements, surface plasmon polaritons (SPPs) are capable of drastically increasing light-molecule coupling in organic optoelectronic devices. The electric field enhancement, however, is anisotropic, offering maximal functional benefits if molecules are oriented perpendicular to the interface. To provide a clear demonstration of this orientation dependence, we study SPP dispersion and SPP-mediated photoluminescence at a model Au/small-molecule interface where identical molecules can be deposited with two very different molecular backbone orientations depending on processing conditions. First, we demonstrate that thin films of p-SIDT(FBTTh2)2 can be deposited with either all "in-plane" (parallel to substrate) or a 50/50 mix of in-plane/"out-of-plane" (perpendicular to substrate) optical transition dipoles by the absence or presence, respectively, of diiodooctane during spin-coating. In contrast to typical orientation control observed in organic thin films, for this particular molecule, this corresponds to films with conjugated backbones purely in-plane, or with a 50/50 mix of in-plane/out-of-plane backbones. Then, using momentum-resolved reflectometry and momentum-resolved photoluminescence, we study and quantify changes in SPP dispersion and photoluminescence intensity arising solely from changes in molecular orientation. We demonstrate increased SPP momentum and a 2-fold enhancement in photoluminescence for systems with out-of-plane oriented transition dipoles. These results agree well with theory and have direct implications for the design and analysis of organic optoelectronic devices.

Model-blind characterization of thin-film optical constants with momentum-resolved reflectometry.

Determining optical constants of thin material films is important for characterizing their electronic excitations and for the design of optoelectronic devices. Spectroscopic ellipsometry techniques have emerged as the predominant approach for measuring thin-film optical constants. However, ellipsometry methods suffer from complications associated with highly model-dependent, multi-parameter spectral fitting procedures. Here, we present a model-blind, momentum-resolved reflectometry technique that yields accurate and precise optical constants, with quantifiable error estimates, even for film thicknesses less than 50 nm. These capabilities are demonstrated by interrogating an optical absorption resonance in films of the polymer P(NDI2OD-T2). We show that this approach produces exceptional agreement with UV-Vis-NIR absorption measurements, while simultaneously avoiding the need to construct complicated multi-oscillator spectral models. Finally, we use this procedure to resolve subtle differences in the out-of-plane optical properties of different film morphologies that were previously obscured in ellipsometry measurements.

Widely Tunable Infrared Antennas Using Free Carrier Refraction.

We demonstrate tuning of infrared Mie resonances by varying the carrier concentration in doped semiconductor antennas. We fabricate spherical silicon and germanium particles of varying sizes and doping concentrations. Single-particle infrared spectra reveal electric and magnetic dipole, quadrupole, and hexapole resonances. We subsequently demonstrate doping-dependent frequency shifts that follow simple Drude models, culminating in the emergence of plasmonic resonances at high doping levels and long wavelengths. These findings demonstrate the potential for actively tuning infrared Mie resonances by optically or electrically modulating charge carrier densities, thus providing an excellent platform for tunable metamaterials.

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.

Morphology-dependent light trapping in thin-film organic solar cells.

The active layer materials used in organic photovoltaic (OPV) cells often self-assemble into highly ordered morphologies, resulting in significant optical anisotropies. However, the impact of these anisotropies on light trapping in nanophotonic OPV architectures has not been considered. In this paper, we show that optical anisotropies in a canonical OPV material, P3HT, strongly affect absorption enhancements in ultra-thin textured OPV cells. In particular we show that plasmonic and gap-mode solar cell architectures redistribute electromagnetic energy into the out-of-plane field component, independent of the active layer orientation. Using analytical and numerical calculations, we demonstrate how the absorption in these solar cell designs can be significantly increased by reorienting polymer domains such that strongly absorbing axes align with the direction of maximum field enhancement.

Nanophotonic light trapping with patterned transparent conductive oxides.

Transparent conductive oxides (TCOs) play a crucial role in solar cells by efficiently transmitting sunlight and extracting photo-generated charge. Here, we show how nanophotonics concepts can be used to transform TCO films into effective photon management layers for solar cells. This is accomplished by patterning the TCO layer present on virtually every thin-film solar cell into an array of subwavelength beams that support optical (Mie) resonances. These resonances can be exploited to concentrate randomly polarized sunlight or to effectively couple it to guided and diffracted modes. We first demonstrate these concepts with a model system consisting of a patterned TCO layer on a thin silicon (Si) film and outline a design methodology for high-performance, TCO-based light trapping coatings. We then show that the short circuit current density from a 300 nm thick amorphous silicon (a-Si) cell with an optimized TCO anti-reflection coating can be enhanced from 19.9 mA/cm2 to 21.1 mA/cm2, out of a possible 26.0 mA/cm2, by using an optimized nanobeam array. The key differences and advantages over plasmonic light trapping layers will be discussed.

Designing Highly Directional Luminescent Phased-Array Metasurfaces with Reciprocity-Based Simulations.

Phased-array metasurfaces grant the ability to arbitrarily shape the wavefront of light. As such, they have been used as various optical elements including waveplates, lenses, and beam deflectors. Luminescent metasurfaces, on the other hand, have largely comprised uniform arrays and are therefore unable to provide the same control over the wavefront of emitted light. Recently, phased-array control of the wavefront of spontaneous emission has been experimentally demonstrated in luminescent phased-array metalenses and beam deflectors. However, current luminescent metasurface beam deflectors exhibit unidirectional emission for only p-polarized light. In this paper, we use a reciprocal simulation strategy to explain the polarization disparity and improve the directionality of incoherent emission from current quantum-well emitting phased-array metasurfaces. We also design complementary metasurfaces to direct emission from systems where emission originates from alternate quantum mechanical processes.

Plasmonics for extreme light concentration and manipulation.

The unprecedented ability of nanometallic (that is, plasmonic) structures to concentrate light into deep-subwavelength volumes has propelled their use in a vast array of nanophotonics technologies and research endeavours. Plasmonic light concentrators can elegantly interface diffraction-limited dielectric optical components with nanophotonic structures. Passive and active plasmonic devices provide new pathways to generate, guide, modulate and detect light with structures that are similar in size to state-of-the-art electronic devices. With the ability to produce highly confined optical fields, the conventional rules for light-matter interactions need to be re-examined, and researchers are venturing into new regimes of optical physics. In this review we will discuss the basic concepts behind plasmonics-enabled light concentration and manipulation, make an attempt to capture the wide range of activities and excitement in this area, and speculate on possible future directions.

Dielectric particle and void resonators for thin film solar cell textures.

Using Mie theory and Rigorous Coupled Wave Analysis (RCWA) we compare the properties of dielectric particle and void resonators. We show that void resonators-low refractive index inclusions within a high index embedding medium-exhibit larger bandwidth resonances, reduced peak scattering intensity, different polarization anisotropies, and enhanced forward scattering when compared to their particle (high index inclusions in a low index medium) counterparts. We evaluate amorphous silicon solar cell textures comprising either arrays of voids or particles. Both designs support substantial absorption enhancements (up to 45%) relative to a flat cell with anti-reflection coating, over a large range of cell thicknesses. By leveraging void-based textures 90% of above-bandgap photons are absorbed in cells with maximal vertical dimension of 100 nm.

Semiconductor nanowire optical antenna solar absorbers.

Photovoltaic (PV) cells can serve as a virtually unlimited clean source of energy by converting sunlight into electrical power. Their importance is reflected in the tireless efforts that have been devoted to improving the electrical and structural properties of PV materials. More recently, photon management (PM) has emerged as a powerful additional means to boost energy conversion efficiencies. Here, we demonstrate an entirely new PM strategy that capitalizes on strong broad band optical antenna effects in one-dimensional semiconductor nanostructures to dramatically enhance absorption of sunlight. We show that the absorption of sunlight in Si nanowires (Si NWs) can be significantly enhanced over the bulk. The NW's optical properties also naturally give rise to an improved angular response. We propose that by patterning the silicon layer in a thin film PV cell into an array of NWs, one can boost the absorption for solar radiation by 25% while utilizing less than half of the semiconductor material (250% increase in the light absorption per unit volume of material). These results significantly advance our understanding of the way sunlight is absorbed by one-dimensional semiconductor nanostructures and provide a clear, intuitive guidance for the design of efficient NW solar cells. The presented approach is universal to any semiconductor and a wide range of nanostructures; as such, it provides a new PV platform technology.

Light-emitting metalenses and meta-axicons for focusing and beaming of spontaneous emission.

Phased-array metasurfaces have been extensively used for wavefront shaping of coherent incident light. Due to the incoherent nature of spontaneous emission, the ability to similarly tailor photoluminescence remains largely unexplored. Recently, unidirectional photoluminescence from InGaN/GaN quantum-well metasurfaces incorporating one-dimensional phase profiles has been shown. However, the possibility of generating arbitrary two-dimensional waveforms-such as focused beams-is not yet realized. Here, we demonstrate two-dimensional metasurface axicons and lenses that emit collimated and focused beams, respectively. First, we develop off-axis meta-axicon/metalens equations designed to redirect surface-guided waves that dominate the natural emission pattern of quantum wells. Next, we show that photoluminescence properties are well predicted by passive transmission results using suitably engineered incident light sources. Finally, we compare collimating and focusing performances across a variety of different light-emitting metasurface axicons and lenses. These generated two-dimensional phased-array photoluminescence waveforms facilitate future development of light sources with arbitrary functionalities.

Engineering light absorption in semiconductor nanowire devices.

The use of quantum and photon confinement has enabled a true revolution in the development of high-performance semiconductor materials and devices. Harnessing these powerful physical effects relies on an ability to design and fashion structures at length scales comparable to the wavelength of electrons (approximately 1 nm) or photons (approximately 1 microm). Unfortunately, many practical optoelectronic devices exhibit intermediate sizes where resonant enhancement effects seem to be insignificant. Here, we show that leaky-mode resonances, which can gently confine light within subwavelength, high-refractive-index semiconductor nanostructures, are ideally suited to enhance and spectrally engineer light absorption in this important size regime. This is illustrated with a series of individual germanium nanowire photodetectors. This notion, together with the ever-increasing control over nanostructure synthesis opens up tremendous opportunities for the realization of a wide range of high-performance, nanowire-based optoelectronic devices, including solar cells, photodetectors, optical modulators and light sources.

Even-Parity Self-Trapped Excitons Lead to Magnetic Dipole Radiation in Two-Dimensional Lead Halide Perovskites.

Recently, unconventional bright magnetic dipole (MD) radiation was observed from two-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs). According to commonly accepted HOIP band structure calculations, such MD light emission from the ground-state exciton should be strictly symmetry forbidden. These results suggest that MD emission arises in conjunction with an as-yet unidentified symmetry-breaking mechanism. In this paper, we show that MD light emission originates from a self-trapped p-like exciton stabilized at energies below the primary electric dipole (ED)-emitting 1s exciton. Using suitable combinations of sample and collection geometries, we isolate the distinct temperature-dependent properties of the ED and MD photoluminescence (PL). We show that the ED emission wavelength is nearly constant with temperature, whereas the MD emission wavelength exhibits substantial red shifts with heating. To explain these results, we derive a microscopic model comprising two distinct parity exciton states coupled to lattice distortions. The model explains many experimental observations, including the thermal red shift, the difference in emission wavelengths, and the relative intensities of the ED and MD emission. Thermodynamic analysis of temperature-dependent PL reveals that the MD emission originates from a locally distorted structure. Finally, we demonstrate unusual hysteresis effects of the MD-emitting state near structural phase transitions. We hypothesize that this is another manifestation of the local distortions, indicating that they are insensitive to phase changes in the equilibrium lattice structure.

Bright magnetic dipole radiation from two-dimensional lead-halide perovskites.

Light-matter interactions in semiconductors are uniformly treated within the electric dipole approximation; multipolar interactions are considered "forbidden." We experimentally demonstrate that this approximation inadequately describes light emission in two-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs), solution processable semiconductors with promising optoelectronic properties. By exploiting the highly oriented crystal structure, we use energy-momentum spectroscopies to demonstrate that an exciton-like sideband in 2D HOIPs exhibits a multipolar radiation pattern with highly directed emission. Electromagnetic and quantum-mechanical analyses indicate that this emission originates from an out-of-plane magnetic dipole transition arising from the 2D character of electronic states. Symmetry arguments and temperature-dependent measurements suggest a dynamic symmetry-breaking mechanism that is active over a broad temperature range. These results challenge the paradigm of electric dipole-dominated light-matter interactions in optoelectronic materials, provide new perspectives on the origins of unexpected sideband emission in HOIPs, and tease the possibility of metamaterial-like scattering phenomena at the quantum-mechanical level.

General properties of dielectric optical antennas.

Using Mie theory we derive a number of general results concerning the resonances of spherical and cylindrical dielectric antennas. Specifically, we prove that the peak scattering cross-section of radiation-limited antennas depends only on the resonance frequency and thus is independent of refractive index and size, a result which is valid even when the resonator is atomic-scale. Furthermore, we derive scaling limits for the bandwidth of dielectric antennas and describe a cylindrical mode which is unique in its ability to support extremely large bandwidths even when the particle size is deeply subwavelength. Finally, we show that higher Q antennas may couple more efficiently to an external load, but the optimal absorption cross-section depends only on the resonance frequency.

Optical Constants and Effective-Medium Origins of Large Optical Anisotropies in Layered Hybrid Organic/Inorganic Perovskites.

Hybrid organic/inorganic perovskites (HOIPs) are of great interest for optoelectronic applications due to their quality electronic and optical properties and the exceptional ease of room-temperature synthesis. Layered HOIP structures, e.g., Ruddlesden-Popper phases, offer additional synthetic means to define self-assembling multiple quantum well structures. Measurements of Ruddlesden-Popper HOIP optical constants are currently lacking, but are critical for both a fundamental understanding as well as optoelectronic device design. Here, we use momentum-resolved optical techniques to measure error-constrained complex uniaxial optical constants of layered lead-iodide perovskites incorporating a variety of organic spacer molecules. We demonstrate how large optical anisotropies measured in these materials arise primarily from classical dielectric inhomogeneities rather than the two-dimensional nature of the electronic states. We subsequently show how variations among these materials can be understood within a classical effective-medium model that accounts for dielectric inhomogeneity. We find agreement between experimentally inferred dielectric properties and quantum-mechanical calculations only after accounting for these purely classical effects. This work provides a library of optical constants for this class of materials and clarifies the origins of large absorption and photoluminescence anisotropies witnessed in these and other layered nanomaterials.