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.

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.

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.

Dynamic Tuning of Gap Plasmon Resonances Using a Solid-State Electrochromic Device.

Plasmonic antennas and metasurfaces can effectively control light-matter interactions, and this facilitates a deterministic design of optical materials properties, including structural color. However, these optical properties are generally fixed after synthesis and fabrication, while many modern-day optics applications require active, low-power, and nonvolatile tuning. These needs have spurred broad research activities aimed at identifying materials and resonant structures capable of achieving large, dynamic changes in optical properties, especially in the challenging visible spectral range. In this work, we demonstrate dynamic tuning of polarization-dependent gap plasmon resonators that contain the electrochromic oxide WO3. Its refractive index in the visible changes continuously from n = 2.1 to 1.9 upon electrochemical lithium insertion and removal in a solid-state device. By incorporating WO3 into a gap plasmon resonator, the resonant wavelength can be shifted continuously and reversibly by up to 58 nm with less than 2 V electrochemical bias voltage. The resonator can remain in a tuned state for tens of minutes under open circuit conditions.

A Light-Field Metasurface for High-Resolution Single-Particle Tracking.

Three-dimensional (3D) single-particle tracking (SPT) is a key tool for studying dynamic processes in the life sciences. However, conventional optical elements utilizing light fields impose an inherent trade-off between lateral and axial resolution, preventing SPT with high spatiotemporal resolution across an extended volume. We overcome the typical loss in spatial resolution that accompanies light-field-based approaches to obtain 3D information by placing a standard microscope coverslip patterned with a multifunctional, light-field metasurface on a specimen. This approach enables an otherwise unmodified microscope to gather 3D information at an enhanced spatial resolution. We demonstrate simultaneous tracking of multiple fluorescent particles within a large 0.5 × 0.5 × 0.3 mm3 volume using a standard epi-fluorescent microscope with submicron lateral and micron-level axial resolution.

Probing the Band Structure of Topological Silicon Photonic Lattices in the Visible Spectrum.

We study two-dimensional hexagonal photonic lattices of silicon Mie resonators with a topological optical band structure in the visible spectral range. We use 30 keV electrons focused to nanoscale spots to map the local optical density of states in topological photonic lattices with deeply subwavelength resolution. By slightly shrinking or expanding the unit cell, we form hexagonal superstructures and observe the opening of a band gap and a splitting of the double-degenerate Dirac cones, which correspond to topologically trivial and nontrivial phases. Optical transmission spectroscopy shows evidence of topological edge states at the domain walls between topological and trivial lattices.

Metasurface Mirrors for External Control of Mie Resonances.

The ability to control and structurally tune the optical resonances of semiconductor nanostructures has far-reaching implications for a wide range of optical applications, including photodetectors, (bio)sensors, and photovoltaics. Such control is commonly obtained by tailoring the nanostructure's geometry, material, or dielectric environment. Here, we combine insights from the field of coherent optics and metasurface mirrors to effectively turn Mie resonances on and off with high spatial control and in a polarization-dependent fashion. We illustrate this in an integrated device by manipulating the photocurrent spectra of a single-nanowire photodetector placed on a metasurface mirror. This approach can be generalized to control spectral, angle-dependent, absorption, and scattering properties of semiconductor nanostructures with an engineered metasurface and without a need to alter their geometric or materials properties.

Thermoplasmonic Ignition of Metal Nanoparticles.

Explosives, propellants, and pyrotechnics are energetic materials that can store and quickly release tremendous amounts of chemical energy. Aluminum (Al) is a particularly important fuel in many applications because of its high energy density, which can be released in a highly exothermic oxidation process. The diffusive oxidation mechanism (DOM) and melt-dispersion mechanism (MDM) explain the ways powders of Al nanoparticles (NPs) can burn, but little is known about the possible use of plasmonic resonances in NPs to manipulate photoignition. This is complicated by the inhomogeneous nature of powders and very fast heating and burning rates. Here, we generate Al NPs with well-defined sizes, shapes, and spacings by electron beam lithography and demonstrate that their plasmonic resonances can be exploited to heat and ignite them with a laser. By combining simulations with thermal-emission, electron-, and optical-microscopy studies, we reveal how an improved control over NP ignition can be attained.

DNA-Assembled Plasmonic Waveguides for Nanoscale Light Propagation to a Fluorescent Nanodiamond.

Plasmonic waveguides consisting of metal nanoparticle chains can localize and guide light well below the diffraction limit, but high propagation losses due to lithography-limited large interparticle spacing have impeded practical applications. Here, we demonstrate that DNA-origami-based self-assembly of monocrystalline gold nanoparticles allows the interparticle spacing to be decreased to ∼2 nm, thus reducing propagation losses to 0.8 dB per 50 nm at a deep subwavelength confinement of 62 nm (∼λ/10). We characterize the individual waveguides with nanometer-scale resolution by electron energy-loss spectroscopy. Light propagation toward a fluorescent nanodiamond is directly visualized by cathodoluminescence imaging spectroscopy on a single-device level, thereby realizing nanoscale light manipulation and energy conversion. Simulations suggest that longitudinal plasmon modes arising from the narrow gaps are responsible for the efficient waveguiding. With this scalable DNA origami approach, micrometer-long propagation lengths could be achieved, enabling applications in information technology, sensing, and quantum optics.

Polarization-independent metasurface lens employing the Pancharatnam-Berry phase.

Metasurface optical elements, optical phased arrays constructed from a dense arrangement of nanoscale antennas, are promising candidates for the next generation of flat optical components. Metasurfaces that rely on the Pancharatnam-Berry phase facilitate complete and efficient wavefront control. However, their operation typically requires control over the polarization state of the incident light to achieve a desired optical function. Here, we circumvent this inherent sensitivity to the incident polarization by multiplexing two metasurfaces that were designed to achieve the same optical function with incident light of opposite helicity. We analyze the optical performance of different multiplexing approaches, and demonstrate a subwavelength random interleaved polarization-independent metasurface lens operating in the visible spectrum, providing a diffraction-limited spot size for the shared-aperture.

Spectrally interleaved topologies using geometric phase metasurfaces.

Metasurfaces facilitate the interleaving of multiple topologies in an ultra-thin photonic system. Here, we report on the spectral interleaving of topological states of light using a geometric phase metasurface. We realize that a dielectric spectrally interleaved metasurface generates multiple interleaved vortex beams at different wavelengths. By harnessing the space-variant polarization manipulations that are enabled by the geometric phase mechanism, a vectorial vortex array is implemented. The presented interleaved topologies concept can greatly enhance the functionality of advanced microscopy and communication systems.

Dynamic Reflection Phase and Polarization Control in Metasurfaces.

Optical metasurfaces are two-dimensional optical elements composed of dense arrays of subwavelength optical antennas and afford on-demand manipulation of the basic properties of light waves. Following the pioneering works on active metasurfaces capable of modulating wave amplitude, there is now a growing interest to dynamically control other fundamental properties of light. Here, we present metasurfaces that facilitate electrical tuning of the reflection phase and polarization properties. To realize these devices, we leverage the properties of actively controlled plasmonic antennas and fundamental insights provided by coupled mode theory. Indium-tin-oxide is embedded into gap-plasmon resonator-antennas as it offers electrically tunable optical properties. By judiciously controlling the resonant properties of the antennas from under- to overcoupling regimes, we experimentally demonstrate tuning of the reflection phase over 180°. This work opens up new design strategies for active metasurfaces for displacement measurements and tunable waveplates.

Active flat optics using a guided mode resonance.

Dynamically-controlled flat optics relies on achieving active and effective control over light-matter interaction in ultrathin layers. A variety of metasurface designs have achieved efficient amplitude and phase modulation. Particularly, noteworthy progress has been made with the incorporation of newly emerging electro-optical materials into such metasurfaces, including graphene, phase change materials, and transparent conductive oxides. In this Letter, we demonstrate dynamic light-matter interaction in a silicon-based subwavelength grating that supports a guided mode resonance. By overcoating the grating with indium tin oxide as an electrically tunable material, its reflectance can be tuned from 4% to 86%. Guided mode resonances naturally afford higher optical quality factors than the optical antennas used in the construction of metasurfaces. As such, they facilitate more effective control over the flow of light within the same layer thickness.

Photonic Multitasking Interleaved Si Nanoantenna Phased Array.

Metasurfaces provide unprecedented control over light propagation by imparting local, space-variant phase changes on an incident electromagnetic wave. They can improve the performance of conventional optical elements and facilitate the creation of optical components with new functionalities and form factors. Here, we build on knowledge from shared aperture phased array antennas and Si-based gradient metasurfaces to realize various multifunctional metasurfaces capable of achieving multiple distinct functions within a single surface region. As a key point, we demonstrate that interleaving multiple optical elements can be accomplished without reducing the aperture of each subelement. Multifunctional optical elements constructed from Si-based gradient metasurface are realized, including axial and lateral multifocus geometric phase metasurface lenses. We further demonstrate multiwavelength color imaging with a high spatial resolution. Finally, optical imaging functionality with simultaneous color separation has been obtained by using multifunctional metasurfaces, which opens up new opportunities for the field of advanced imaging and display.

Superabsorbing, Artificial Metal Films Constructed from Semiconductor Nanoantennas.

In 1934, Wilhelm Woltersdorff demonstrated that the absorption of light in an ultrathin, freestanding film is fundamentally limited to 50%. He concluded that reaching this limit would require a film with a real-valued sheet resistance that is exactly equal to R = η/2 ≈ 188.5Ω/□, where [Formula: see text] is the impedance of free space. This condition can be closely approximated over a wide frequency range in metals that feature a large imaginary relative permittivity εr″, that is, a real-valued conductivity σ = ε0εr″ω. A thin, continuous sheet of semiconductor material does not facilitate such strong absorption as its complex-valued permittivity with both large real and imaginary components preclude effective impedance matching. In this work, we show how a semiconductor metafilm constructed from optically resonant semiconductor nanostructures can be created whose optical response mimics that of a metallic sheet. For this reason, the fundamental absorption limit mentioned above can also be reached with semiconductor materials, opening up new opportunities for the design of ultrathin optoelectronic and light harvesting devices.

Porous Silicon Gradient Refractive Index Micro-Optics.

The emergence and growth of transformation optics over the past decade has revitalized interest in how a gradient refractive index (GRIN) can be used to control light propagation. Two-dimensional demonstrations with lithographically defined silicon (Si) have displayed the power of GRIN optics and also represent a promising opportunity for integrating compact optical elements within Si photonic integrated circuits. Here, we demonstrate the fabrication of three-dimensional Si-based GRIN micro-optics through the shape-defined formation of porous Si (PSi). Conventional microfabrication creates Si square microcolumns (SMCs) that can be electrochemically etched into PSi elements with nanoscale porosity along the shape-defined etching pathway, which imparts the geometry with structural birefringence. Free-space characterization of the transmitted intensity distribution through a homogeneously etched PSi SMC exhibits polarization splitting behavior resembling that of dielectric metasurfaces that require considerably more laborious fabrication. Coupled birefringence/GRIN effects are studied by way of PSi SMCs etched with a linear (increasing from edge to center) GRIN profile. The transmitted intensity distribution shows polarization-selective focusing behavior with one polarization focused to a diffraction-limited spot and the orthogonal polarization focused into two laterally displaced foci. Optical thickness-based analysis readily predicts the experimentally observed phenomena, which strongly match finite-element electromagnetic simulations.

Backward phase-matching for nonlinear optical generation in negative-index materials.

Metamaterials have enabled the realization of unconventional electromagnetic properties not found in nature, which provokes us to rethink the established rules of optics in both the linear and nonlinear regimes. One of the most intriguing phenomena in nonlinear metamaterials is 'backward phase-matching', which describes counter-propagating fundamental and harmonic waves in a negative-index medium. Predicted nearly a decade ago, this process is still awaiting a definitive experimental confirmation at optical frequencies. Here, we report optical measurements showing backward phase-matching by exploiting two distinct modes in a nonlinear plasmonic waveguide, where the real parts of the mode refractive indices are 3.4 and -3.4 for the fundamental and the harmonic waves respectively. The observed peak conversion efficiency at the excitation wavelength of ∼780 nm indicates the fulfilment of the phase-matching condition of k(2ω) = 2k(ω) and n(2ω) = -n(ω), where the coherent harmonic wave emerges along a direction opposite to that of the incoming fundamental light.

Fabry-Perot description for Mie resonances of rectangular dielectric nanowire optical resonators.

We show that a dielectric nanowire (NW) with a rectangular cross section can effectively be modeled as a Fabry-Perot cavity formed by truncating a dielectric slab waveguide. By calculating the mode indices of the supported waveguide modes and the reflection phase pickup of the guided waves from the end facets, we can numerically predict the spectral locations of optical, Mie-like resonances for such NWs. This type of analysis must be performed twice in order to account for all resonances of these structures, corresponding to light propagating in the vertical or horizontal directions. The model shows excellent agreement with full-field simulations. We show how the refractive index of both the NW itself and neighboring materials and substrates impact the resonant properties. Our results can aid the development of NW-based optoelectronic devices, for which rectangular cross sections are much simpler to fabricate using top-down fabrication procedures.

Picosecond Electric-Field-Induced Threshold Switching in Phase-Change Materials.

Many chalcogenide glasses undergo a breakdown in electronic resistance above a critical field strength. Known as threshold switching, this mechanism enables field-induced crystallization in emerging phase-change memory. Purely electronic as well as crystal nucleation assisted models have been employed to explain the electronic breakdown. Here, picosecond electric pulses are used to excite amorphous Ag_{4}In_{3}Sb_{67}Te_{26}. Field-dependent reversible changes in conductivity and pulse-driven crystallization are observed. The present results show that threshold switching can take place within the electric pulse on subpicosecond time scales-faster than crystals can nucleate. This supports purely electronic models of threshold switching and reveals potential applications as an ultrafast electronic switch.

Gap Plasmon Resonance in a Suspended Plasmonic Nanowire Coupled to a Metallic Substrate.

We present an experimental demonstration of nanoscale gap plasmon resonators that consist of an individual suspended plasmonic nanowire (NW) over a metallic substrate. Our study demonstrates that the NW supports strong gap plasmon resonances of various gap sizes including single-nanometer-scale gaps. The obtained resonance features agree well with intuitive resonance models for near- and far-field regimes. We also illustrate that our suspended NW geometry is capable of constructing plasmonic coupled systems dominated by quasi-electrostatics.