Temperature-Dependent Excitonic Light Manipulation with Atomically Thin Optical Elements.

Monolayer 2D semiconductors, such as WS2, exhibit uniquely strong light-matter interactions due to exciton resonances that enable atomically thin optical elements. Similar to geometry-dependent plasmon and Mie resonances, these intrinsic material resonances offer coherent and tunable light scattering. Thus far, the impact of the excitons' temporal dynamics on the performance of such excitonic metasurfaces remains unexplored. Here, we show how the excitonic decay rates dictate the focusing efficiency of an atomically thin lens carved directly out of exfoliated monolayer WS2. By isolating the coherent exciton radiation from the incoherent background in the focus of the lens, we obtain a direct measure of the role of exciton radiation in wavefront shaping. Furthermore, we investigate the influence of exciton-phonon scattering by characterizing the focusing efficiency as a function of temperature, demonstrating an increased optical efficiency at cryogenic temperatures. Our results provide valuable insights into the role of excitonic light scattering in 2D nanophotonic devices.

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.

Determining hot-carrier transport dynamics from terahertz emission.

Understanding the ultrafast excitation and transport dynamics of plasmon-driven hot carriers is critical to the development of optoelectronics, photochemistry, and solar-energy harvesting. However, the ultrashort time and length scales associated with the behavior of these highly out-of-equilibrium carriers have impaired experimental verification of ab initio quantum theories. Here, we present an approach to studying plasmonic hot-carrier dynamics that analyzes the temporal waveform of coherent terahertz bursts radiated by photo-ejected hot carriers from designer nano-antennas with a broken symmetry. For ballistic carriers ejected from gold antennas, we find an ~11-femtosecond timescale composed of the plasmon lifetime and ballistic transport time. Polarization- and phase-sensitive detection of terahertz fields further grant direct access to their ballistic transport trajectory. Our approach opens explorations of ultrafast carrier dynamics in optically excited nanostructures.

Off-axis metasurfaces for folded flat optics.

The overall size of an optical system is limited by the volume of the components and the internal optical path length. To reach the limits of miniaturization, it is possible to reduce both component volume and path length by combining the concepts of metasurface flat optics and folded optics. In addition to their subwavelength component thickness, metasurfaces enable bending conventional folded geometries off axis beyond the law of reflection. However, designing metasurfaces for highly off-axis illumination with visible light in combination with a high numerical aperture is non-trivial. In this case, traditional designs with gradient metasurfaces exhibit low diffraction efficiencies and require the use of deep-subwavelength, high-index, and high-aspect-ratio semiconductor nanostructures that preclude inexpensive, large-area nanofabrication. Here, we describe a design approach that enables the use of low-index (n ≈ 1.5), low-aspect ratio structures for off-axis metagratings that can redirect and focus visible light (λ = 532 nm) with near-unity efficiency. We show that fabricated optical elements offer a very large angle-of-view (110°) and lend themselves to scalable fabrication by nano-imprint lithography.

Controlling Valley-Specific Light Emission from Monolayer MoS2 with Achiral Dielectric Metasurfaces.

Excitons in two-dimensional transition metal dichalcogenides have a valley degree of freedom that can be optically manipulated for quantum information processing. Here, we integrate MoS2 monolayers with achiral silicon disk array metasurfaces to enhance and control valley-specific absorption and emission. Through the coupling to the metasurface electric and magnetic Mie modes, the intensity and lifetime of the emission of neutral excitons, trions, and defect bound excitons can be enhanced and shortened, respectively, while the spectral shape can be modified. Additionally, the degree of polarization (DOP) of exciton and trion emission from the valley can be symmetrically enhanced at 100 K. The DOP increase is attributed to both the metasurface-enhanced chiral absorption of light and the metasurface-enhanced exciton emission from the Purcell effect. Combining Si-compatible photonic design with large-scale 2D materials integration, our work makes an important step toward on-chip valleytronic applications approaching room-temperature operation.

Dynamically Tunable Optical Cavities with Embedded Nematic Liquid Crystalline Networks.

Tunable metal-insulator-metal (MIM) Fabry-Pérot (FP) cavities that can dynamically control light enable novel sensing, imaging and display applications. However, the realization of dynamic cavities incorporating stimuli-responsive materials poses a significant engineering challenge. Current approaches rely on refractive index modulation and suffer from low dynamic tunability, high losses, and limited spectral ranges, and require liquid and hazardous materials for operation. To overcome these challenges, a new tuning mechanism employing reversible mechanical adaptations of a polymer network is proposed, and dynamic tuning of optical resonances is demonstrated. Solid-state temperature-responsive optical coatings are developed by preparing a monodomain nematic liquid crystalline network (LCN) and are incorporated between metallic mirrors to form active optical microcavities. LCN microcavities offer large, reversible and highly linear spectral tuning of FP resonances reaching wavelength-shifts up to 40 nm via thermomechanical actuation while featuring outstanding repeatability and precision over more than 100 heating-cooling cycles. This degree of tunability allows for reversible switching between the reflective and the absorbing states of the device over the entire visible and near-infrared spectral regions, reaching large changes in reflectance with modulation efficiency ΔR = 79%.

Quantitative phase contrast imaging with a nonlocal angle-selective metasurface.

Phase contrast microscopy has played a central role in the development of modern biology, geology, and nanotechnology. It can visualize the structure of translucent objects that remains hidden in regular optical microscopes. The optical layout of a phase contrast microscope is based on a 4 f image processing setup and has essentially remained unchanged since its invention by Zernike in the early 1930s. Here, we propose a conceptually new approach to phase contrast imaging that harnesses the non-local optical response of a guided-mode-resonator metasurface. We highlight its benefits and demonstrate the imaging of various phase objects, including biological cells, polymeric nanostructures, and transparent metasurfaces. Our results showcase that the addition of this non-local metasurface to a conventional microscope enables quantitative phase contrast imaging with a 0.02π phase accuracy. At a high level, this work adds to the growing body of research aimed at the use of metasurfaces for analog optical computing.

Creating the ultimate virtual reality display.

Scientists are exploring new material designs to make smaller and denser pixel displays.

Metasurface optofluidics for dynamic control of light fields.

The ability to manipulate light and liquids on integrated optofluidics chips has spurred a myriad of important developments in biology, medicine, chemistry and display technologies. Here we show how the convergence of optofluidics and metasurface optics can lead to conceptually new platforms for the dynamic control of light fields. We first demonstrate metasurface building blocks that display an extreme sensitivity in their scattering properties to their dielectric environment. These blocks are then used to create metasurface-based flat optics inside microfluidic channels where liquids with different refractive indices can be directed to manipulate their optical behaviour. We demonstrate the intensity and spectral tuning of metasurface colour pixels as well as on-demand optical elements. We finally demonstrate automated control in an integrated meta-optofluidic platform to open up new display functions. Combined with large-scale microfluidic integration, our dynamic-metasurface flat-optics platform could open up the possibility of dynamic display, imaging, holography and sensing applications.

High-specific-power flexible transition metal dichalcogenide solar cells.

Semiconducting transition metal dichalcogenides (TMDs) are promising for flexible high-specific-power photovoltaics due to their ultrahigh optical absorption coefficients, desirable band gaps and self-passivated surfaces. However, challenges such as Fermi-level pinning at the metal contact-TMD interface and the inapplicability of traditional doping schemes have prevented most TMD solar cells from exceeding 2% power conversion efficiency (PCE). In addition, fabrication on flexible substrates tends to contaminate or damage TMD interfaces, further reducing performance. Here, we address these fundamental issues by employing: (1) transparent graphene contacts to mitigate Fermi-level pinning, (2) MoOx capping for doping, passivation and anti-reflection, and (3) a clean, non-damaging direct transfer method to realize devices on lightweight flexible polyimide substrates. These lead to record PCE of 5.1% and record specific power of 4.4 W g-1 for flexible TMD (WSe2) solar cells, the latter on par with prevailing thin-film solar technologies cadmium telluride, copper indium gallium selenide, amorphous silicon and III-Vs. We further project that TMD solar cells could achieve specific power up to 46 W g-1, creating unprecedented opportunities in a broad range of industries from aerospace to wearable and implantable electronics.

Non-local metasurfaces for spectrally decoupled wavefront manipulation and eye tracking.

Metasurface-based optical elements typically manipulate light waves by imparting space-variant changes in the amplitude and phase with a dense array of scattering nanostructures. The highly localized and low optical-quality-factor (Q) modes of nanostructures are beneficial for wavefront shaping as they afford quasi-local control over the electromagnetic fields. However, many emerging imaging, sensing, communication, display and nonlinear optics applications instead require flat, high-Q optical elements that provide substantial energy storage and a much higher degree of spectral control over the wavefront. Here, we demonstrate high-Q, non-local metasurfaces with atomically thin metasurface elements that offer notably enhanced light-matter interaction and fully decoupled optical functions at different wavelengths. We illustrate a possible use of such a flat optic in eye tracking for eyewear. Here, a metasurface patterned on a regular pair of eye glasses provides an unperturbed view of the world across the visible spectrum and redirects near-infrared light to a camera to allow imaging of the eye.

Electrical tuning of phase-change antennas and metasurfaces.

The success of semiconductor electronics is built on the creation of compact, low-power switching elements that offer routing, logic and memory functions. The availability of nanoscale optical switches could have a similarly transformative impact on the development of dynamic and programmable metasurfaces, optical neural networks and quantum information processing. Phase-change materials are uniquely suited to enable their creation as they offer high-speed electrical switching between amorphous and crystalline states with notably different optical properties. Their high refractive index has already been harnessed to fashion them into compact optical antennas. Here, we take the next important step, by showing electrically-switchable phase-change antennas and metasurfaces that offer strong, reversible, non-volatile, multi-phase switching and spectral tuning of light scattering in the visible and near-infrared spectral ranges. Their successful implementation relies on a careful joint thermal and optical optimization of the antenna elements that comprise a silver strip that simultaneously serves as a plasmonic resonator and a miniature heating stage. Our metasurface affords electrical modulation of the reflectance by more than fourfold at 755 nm.

High-Performance p-n Junction Transition Metal Dichalcogenide Photovoltaic Cells Enabled by MoOx Doping and Passivation.

Layered semiconducting transition metal dichalcogenides (TMDs) are promising materials for high-specific-power photovoltaics due to their excellent optoelectronic properties. However, in practice, contacts to TMDs have poor charge carrier selectivity, while imperfect surfaces cause recombination, leading to a low open-circuit voltage (VOC) and therefore limited power conversion efficiency (PCE) in TMD photovoltaics. Here, we simultaneously address these fundamental issues with a simple MoOx (x ≈ 3) surface charge-transfer doping and passivation method, applying it to multilayer tungsten disulfide (WS2) Schottky-junction solar cells with initially near-zero VOC. Doping and passivation turn these into lateral p-n junction photovoltaic cells with a record VOC of 681 mV under AM 1.5G illumination, the highest among all p-n junction TMD solar cells with a practical design. The enhanced VOC also leads to record PCE in ultrathin (<90 nm) WS2 photovoltaics. This easily scalable doping and passivation scheme is expected to enable further advances in TMD electronics and optoelectronics.

Nanoelectromechanical modulation of a strongly-coupled plasmonic dimer.

The ability of two nearly-touching plasmonic nanoparticles to squeeze light into a nanometer gap has provided a myriad of fundamental insights into light-matter interaction. In this work, we construct a nanoelectromechanical system (NEMS) that capitalizes on the unique, singular behavior that arises at sub-nanometer particle-spacings to create an electro-optical modulator. Using in situ electron energy loss spectroscopy in a transmission electron microscope, we map the spectral and spatial changes in the plasmonic modes as they hybridize and evolve from a weak to a strong coupling regime. In the strongly-coupled regime, we observe a very large mechanical tunability (~250 meV/nm) of the bonding-dipole plasmon resonance of the dimer at ~1 nm gap spacing, right before detrimental quantum effects set in. We leverage our findings to realize a prototype NEMS light-intensity modulator operating at ~10 MHz and with a power consumption of only 4 fJ/bit.

All-solid-state spatial light modulator with independent phase and amplitude control for three-dimensional LiDAR applications.

Spatial light modulators are essential optical elements in applications that require the ability to regulate the amplitude, phase and polarization of light, such as digital holography, optical communications and biomedical imaging. With the push towards miniaturization of optical components, static metasurfaces are used as competent alternatives. These evolved to active metasurfaces in which light-wavefront manipulation can be done in a time-dependent fashion. The active metasurfaces reported so far, however, still show incomplete phase modulation (below 360°). Here we present an all-solid-state, electrically tunable and reflective metasurface array that can generate a specific phase or a continuous sweep between 0 and 360° at an estimated rate of 5.4 MHz while independently adjusting the amplitude. The metasurface features 550 individually addressable nanoresonators in a 250 × 250 µm2 area with no micromechanical elements or liquid crystals. A key feature of our design is the presence of two independent control parameters (top and bottom gate voltages) in each nanoresonator, which are used to adjust the real and imaginary parts of the reflection coefficient independently. To demonstrate this array's use in light detection and ranging, we performed a three-dimensional depth scan of an emulated street scene that consisted of a model car and a human figure up to a distance of 4.7 m.

Direct laser writing of volumetric gradient index lenses and waveguides.

Direct laser writing (DLW) has been shown to render 3D polymeric optical components, including lenses, beam expanders, and mirrors, with submicrometer precision. However, these printed structures are limited to the refractive index and dispersive properties of the photopolymer. Here, we present the subsurface controllable refractive index via beam exposure (SCRIBE) method, a lithographic approach that enables the tuning of the refractive index over a range of greater than 0.3 by performing DLW inside photoresist-filled nanoporous silicon and silica scaffolds. Adjusting the laser exposure during printing enables 3D submicron control of the polymer infilling and thus the refractive index and chromatic dispersion. Combining SCRIBE's unprecedented index range and 3D writing accuracy has realized the world's smallest (15 µm diameter) spherical Luneburg lens operating at visible wavelengths. SCRIBE's ability to tune the chromatic dispersion alongside the refractive index was leveraged to render achromatic doublets in a single printing step, eliminating the need for multiple photoresins and writing sequences. SCRIBE also has the potential to form multicomponent optics by cascading optical elements within a scaffold. As a demonstration, stacked focusing structures that generate photonic nanojets were fabricated inside porous silicon. Finally, an all-pass ring resonator was coupled to a subsurface 3D waveguide. The measured quality factor of 4600 at 1550 nm suggests the possibility of compact photonic systems with optical interconnects that traverse multiple planes. SCRIBE is uniquely suited for constructing such photonic integrated circuits due to its ability to integrate multiple optical components, including lenses and waveguides, without additional printed supports.

Monolithic Full-Stokes Near-Infrared Polarimetry with Chiral Plasmonic Metasurface Integrated Graphene-Silicon Photodetector.

The ability to detect the full-Stokes polarization of light is vital for a variety of applications that often require complex and bulky optical systems. Here, we report an on-chip polarimeter comprising four metasurface-integrated graphene-silicon photodetectors. The geometric chirality and anisotropy of the metasurfaces result in circular and linear polarization-resolved photoresponses, from which the full-Stokes parameters, including the intensity, orientation, and ellipticity of arbitrarily polarized incident infrared light (1550 nm), can be obtained. The design presents an ultracompact architecture while excluding the standard bulky optical components and structural redundancy. Computational extraction of full-Stokes parameters from mutual information among four detectors eliminates the need for a large absorption contrast between different polarization states. Our monolithic plasmonic metasurface integrated polarimeter is ideal for a variety of polarization-based applications including biological sensing, quantum information processing, and polarization photography.

Metasurface-driven OLED displays beyond 10,000 pixels per inch.

Optical metasurfaces are starting to find their way into integrated devices, where they can enhance and control the emission, modulation, dynamic shaping, and detection of light waves. In this study, we show that the architecture of organic light-emitting diode (OLED) displays can be completely reenvisioned through the introduction of nanopatterned metasurface mirrors. In the resulting meta-OLED displays, different metasurface patterns define red, green, and blue pixels and ensure optimized extraction of these colors from organic, white light emitters. This new architecture facilitates the creation of devices at the ultrahigh pixel densities (>10,000 pixels per inch) required in emerging display applications (for instance, augmented reality) that use scalable nanoimprint lithography. The fabricated pixels also offer twice the luminescence efficiency and superior color purity relative to standard color-filtered white OLEDs.

High quality factor phase gradient metasurfaces.

Dielectric microcavities with quality factors (Q-factors) in the thousands to billions markedly enhance light-matter interactions, with applications spanning high-efficiency on-chip lasing, frequency comb generation and modulation and sensitive molecular detection. However, as the dimensions of dielectric cavities are reduced to subwavelength scales, their resonant modes begin to scatter light into many spatial channels. Such enhanced scattering is a powerful tool for light manipulation, but also leads to high radiative loss rates and commensurately low Q-factors, generally of order ten. Here, we describe and experimentally demonstrate a strategy for the generation of high Q-factor resonances in subwavelength-thick phase gradient metasurfaces. By including subtle structural perturbations in individual metasurface elements, resonances are created that weakly couple free-space light into otherwise bound and spatially localized modes. Our metasurface can achieve Q-factors >2,500 while beam steering light to particular directions. High-Q beam splitters are also demonstrated. With high-Q metasurfaces, the optical transfer function, near-field intensity and resonant line shape can all be rationally designed, providing a foundation for efficient, free-space-reconfigurable and nonlinear nanophotonics.

Electrotunable liquid sulfur microdroplets.

Manipulating liquids with tunable shape and optical functionalities in real time is important for electroactive flow devices and optoelectronic devices, but remains a great challenge. Here, we demonstrate electrotunable liquid sulfur microdroplets in an electrochemical cell. We observe electrowetting and merging of sulfur droplets under different potentiostatic conditions, and successfully control these processes via selective design of sulfiphilic/sulfiphobic substrates. Moreover, we employ the electrowetting phenomena to create a microlens based on the liquid sulfur microdroplets and tune its characteristics in real time through changing the shape of the liquid microdroplets in a fast, repeatable, and controlled manner. These studies demonstrate a powerful in situ optical battery platform for unraveling the complex reaction mechanism of sulfur chemistries and for exploring the rich material properties of the liquid sulfur, which shed light on the applications of liquid sulfur droplets in devices such as microlenses, and potentially other electrotunable and optoelectronic devices.