Dynamically stable radiation pressure propulsion of flexible lightsails for interstellar exploration.

Meter-scale, submicron-thick lightsail spacecraft, propelled to relativistic velocities via photon pressure using high-power density laser radiation, offer a potentially new route to space exploration within and beyond the solar system, posing substantial challenges for materials science and engineering. We analyze the structural and photonic design of flexible lightsails by developing a mesh-based multiphysics simulator based on linear elastic theory. We observe spin-stabilized flexible lightsail shapes and designs that are immune to shape collapse during acceleration and exhibit beam-riding stability despite deformations caused by photon pressure and thermal expansion. Excitingly, nanophotonic lightsails based on planar silicon nitride membranes patterned with suitable optical metagratings exhibit both mechanically and dynamically stable propulsion along the pump laser axis. These advances suggest that laser-driven acceleration of membrane-like lightsails to the relativistic speeds needed to access interstellar distances is conceptually feasible, and that their fabrication could be achieved by scaling up modern microfabrication technology.

Electrode Surface Heating with Organic Films Improves CO2 Reduction Kinetics on Copper.

Management of the electrode surface temperature is an understudied aspect of (photo)electrode reactor design for complex reactions, such as CO2 reduction. In this work, we study the impact of local electrode heating on electrochemical reduction of CO2 reduction. Using the ferri/ferrocyanide open circuit voltage as a reporter of the effective reaction temperature, we reveal how the interplay of surface heating and convective cooling presents an opportunity for cooptimizing mass transport and thermal assistance of electrochemical reactions, where we focus on reduction of CO2 to carbon-coupled (C2+) products. The introduction of an organic coating on the electrode surface facilitates well-behaved electrode kinetics with near-ambient bulk electrolyte temperature. This approach helps to probe the fundamentals of thermal effects in electrochemical reactions, as demonstrated through Bayesian inference of Tafel kinetic parameters from a suite of high throughput experiments, which reveal a decrease in overpotential for C2+ products by 0.1 V on polycrystalline copper via 60 °C surface heating.

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.

Third Harmonic Generation Enhancement and Wavefront Control Using a Local High-Q Metasurface.

High quality factor optical nanostructures provide a great opportunity to enhance nonlinear optical processes such as third harmonic generation. However, the field enhancement in these high quality factor structures is typically accompanied by optical mode nonlocality. As a result, the enhancement of nonlinear processes comes at the cost of their local control as needed for nonlinear wavefront shaping, imaging, and holography. Here we show simultaneous strong enhancement and spatial control over third harmonic generation with a local high-Q metasurface relying on higher-order Mie resonant modes. Our results demonstrate third harmonic generation at an efficiency of up to 3.25 × 10-5, high quality wavefront shaping as illustrated by a third harmonic metalens, and a flatband, angle independent, third harmonic response up to ±11° incident angle. The demonstrated high level of local control and efficient frequency conversion offer promising prospects for realizing novel nonlinear optical devices.

Molecular Additives Improve the Selectivity of CO2 Photoelectrochemical Reduction over Gold Nanoparticles on Gallium Nitride.

Photoelectrochemical CO2 reduction (CO2R) is an appealing solution for converting carbon dioxide into higher-value products. However, CO2R in aqueous electrolytes suffers from poor selectivity due to the competitive hydrogen evolution reaction that is dominant on semiconductor surfaces in aqueous electrolytes. We demonstrate that functionalizing gold/p-type gallium nitride devices with a film derived from diphenyliodonium triflate suppresses hydrogen generation from 90% to 18%. As a result, we observe increases in the Faradaic efficiency and partial current density for carbon monoxide of 50% and 3-fold, respectively. Furthermore, we demonstrate through optical absorption measurements that the molecular film employed herein, regardless of thickness, does not affect the photocathode's light absorption. Altogether, this study provides a rigorous platform for elucidating the catalytic structure-property relationships to enable engineering of active, stable, and selective materials for photoelectrochemical CO2R.

Dramatically Enhanced Valley-Polarized Emission by Alloying and Electrical Tuning of Monolayer WTe2 x S2(1- x ) Alloys at Room Temperature with 1T'-WTe2 -Contact.

Monolayer ternary tellurides based on alloying different transition metal dichalcogenides (TMDs) can result in new two-dimensional (2D) materials ranging from semiconductors to metals and superconductors with tunable optical and electrical properties. Semiconducting WTe2 x S2(1- x ) monolayer possesses two inequivalent valleys in the Brillouin zone, each valley coupling selectively with circularly polarized light (CPL). The degree of valley polarization (DVP) under the excitation of CPL represents the purity of valley polarized photoluminescence (PL), a critical parameter for opto-valleytronic applications. Here, new strategies to efficiently tailor the valley-polarized PL from semiconducting monolayer WTe2 x S2(1- x ) at room temperature (RT) through alloying and back-gating are presented. The DVP at RT is found to increase drastically from < 5% in WS2 to 40% in WTe0.12 S1.88 by Te-alloying to enhance the spin-orbit coupling. Further enhancement and control of the DVP from 40% up to 75% is demonstrated by electrostatically doping the monolayer WTe0.12 S1.88 via metallic 1T'-WTe2 electrodes, where the use of 1T'-WTe2 substantially lowers the Schottky barrier height (SBH) and weakens the Fermi-level pinning of the electrical contacts. The demonstration of drastically enhanced DVP and electrical tunability in the valley-polarized emission from 1T'-WTe2 /WTe0.12 S1.88 heterostructures paves new pathways towards harnessing valley excitons in ultrathin valleytronic devices for RT applications.

High quality factor metasurfaces for two-dimensional wavefront manipulation.

The strong interaction of light with micro- and nanostructures plays a critical role in optical sensing, nonlinear optics, active optical devices, and quantum optics. However, for wavefront shaping, the required local control over light at a subwavelength scale limits this interaction, typically leading to low-quality-factor optical devices. Here, we demonstrate an avenue towards high-quality-factor wavefront shaping in two spatial dimensions based on all-dielectric higher-order Mie-resonant metasurfaces. We design and experimentally realize transmissive band stop filters, beam deflectors and high numerical aperture radial lenses with measured quality factors in the range of 202-1475 at near-infrared wavelengths. The excited optical mode and resulting wavefront control are both local, allowing versatile operation with finite apertures and oblique illumination. Our results represent an improvement in quality factor by nearly two orders of magnitude over previous localized mode designs, and provide a design approach for a new class of compact optical devices.

Edge-Confined Excitons in Monolayer Black Phosphorus.

Quantum confinement of two-dimensional excitons in van der Waals materials via electrostatic trapping, lithographic patterning, Moiré potentials, and chemical implantation has enabled significant advances in tailoring light emission from nanostructures. While such approaches rely on complex preparation of materials, natural edges are a ubiquitous feature in layered materials and provide a different approach for investigating quantum-confined excitons. Here, we observe that certain edge sites of monolayer black phosphorus (BP) strongly localize the intrinsic quasi-one-dimensional excitons, yielding sharp spectral lines in photoluminescence, with nearly an order of magnitude line width reduction. Through structural characterization of BP edges using transmission electron microscopy and first-principles GW plus Bethe-Salpeter equation (GW-BSE) calculations of exemplary BP nanoribbons, we find that certain atomic reconstructions can strongly quantum-confine excitons resulting in distinct emission features, mediated by local strain and screening. We observe linearly polarized luminescence emission from edge reconstructions that preserve the mirror symmetry of the parent BP lattice, in agreement with calculations. Furthermore, we demonstrate efficient electrical switching of localized edge excitonic luminescence, whose sites act as excitonic transistors for emission. Localized emission from BP edges motivates exploration of nanoribbons and quantum dots as hosts for tunable narrowband light generation, with future potential to create atomic-like structures for quantum information processing applications as well as exploration of exotic phases that may reside in atomic edge structures.

Detecting, Distinguishing, and Spatiotemporally Tracking Photogenerated Charge and Heat at the Nanoscale.

Since dissipative processes are ubiquitous in semiconductors, characterizing how electronic and thermal energy transduce and transport at the nanoscale is vital for understanding and leveraging their fundamental properties. For example, in low-dimensional transition metal dichalcogenides (TMDCs), excess heat generation upon photoexcitation is difficult to avoid since even with modest injected exciton densities exciton-exciton annihilation still occurs. Both heat and photoexcited electronic species imprint transient changes in the optical response of a semiconductor, yet the distinct signatures of each are difficult to disentangle in typical spectra due to overlapping resonances. In response, we employ stroboscopic optical scattering microscopy (stroboSCAT) to simultaneously map both heat and exciton populations in few-layer MoS2 on relevant nanometer and picosecond length- and time scales and with 100-mK temperature sensitivity. We discern excitonic contributions to the signal from heat by combining observations close to and far from exciton resonances, characterizing the photoinduced dynamics for each. Our approach is general and can be applied to any electronic material, including thermoelectrics, where heat and electronic observables spatially interplay, and it will enable direct and quantitative discernment of different types of coexisting energy without recourse to complex models or underlying assumptions.

Thermal metasurface with tunable narrowband absorption from a hybrid graphene/silicon photonic crystal resonance.

We report the design of a tunable, narrowband, thermal metasurface that employs a hybrid resonance generated by coupling a tunable permittivity graphene ribbon to a silicon photonic crystal. The gated graphene ribbon array, proximitized to a high quality factor Si photonic crystal supporting a guided mode resonance, exhibits tunable narrowband absorbance lineshapes (Q > 10,000). Actively tuned Fermi level modulation in graphene with applied gate voltage between high absorptivity and low absorptivity states gives rise to absorbance on/off ratios exceeding 60. We employ coupled-mode theory as a computationally efficient approach to elements of the metasurface design, demonstrating an orders of magnitude speedup over typical finite element computational methods.

Quasiparticle and Optical Properties of Carrier-Doped Monolayer MoTe2 from First Principles.

The intrinsic weak and highly nonlocal dielectric screening of two-dimensional materials is well-known to lead to high sensitivity of their optoelectronic properties to environment. Less studied theoretically is the role of free carriers in those properties. Here, we use ab initio GW and Bethe-Salpeter equation calculations, with a rigorous treatment of dynamical screening and local-field effects, to study the doping dependence of the quasiparticle and optical properties of a monolayer transition-metal dichalcogenide, 2H MoTe2. We predict a quasiparticle band gap renormalization of several hundreds of meV for experimentally attainable carrier densities and a similarly sizable decrease in the exciton binding energy. This results in an almost constant excitation energy for the lowest-energy exciton resonance with an increasing doping density. Using a newly developed and generally applicable plasmon-pole model and a self-consistent solution of the Bethe-Salpeter equation, we reveal the importance of accurately capturing both dynamical and local-field effects to understand detailed photoluminescence measurements.

Rydberg Excitons and Trions in Monolayer MoTe2.

Monolayer transition metal dichalcogenide (TMDC) semiconductors exhibit strong excitonic optical resonances, which serve as a microscopic, noninvasive probe into their fundamental properties. Like the hydrogen atom, such excitons can exhibit an entire Rydberg series of resonances. Excitons have been extensively studied in most TMDCs (MoS2, MoSe2, WS2, and WSe2), but detailed exploration of excitonic phenomena has been lacking in the important TMDC material molybdenum ditelluride (MoTe2). Here, we report an experimental investigation of excitonic luminescence properties of monolayer MoTe2 to understand the excitonic Rydberg series, up to 3s. We report a significant modification of emission energies with temperature (4 to 300 K), thereby quantifying the exciton-phonon coupling. Furthermore, we observe a strongly gate-tunable exciton-trion interplay for all the Rydberg states governed mainly by free-carrier screening, Pauli blocking, and band gap renormalization in agreement with the results of first-principles GW plus Bethe-Salpeter equation approach calculations. Our results help bring monolayer MoTe2 closer to its potential applications in near-infrared optoelectronics and photonic devices.

Photovoltaics at multi-terawatt scale: Waiting is not an option.

25% annual PV growth is possible over the next decade.

Excitonic Beam Steering in an Active van der Waals Metasurface.

Two-dimensional transition metal dichalcogenides (2D TMDCs) are promising candidates for ultrathin active nanophotonic elements due to the strong tunable excitonic resonances that dominate their optical response. Here, we demonstrate dynamic beam steering by an active van der Waals metasurface that leverages large complex refractive index tunability near excitonic resonances in monolayer molybdenum diselenide (MoSe2). Through varying the radiative and nonradiative rates of the excitons, we can dynamically control both the reflection amplitude and phase profiles, resulting in an excitonic phased array metasurface. Our experiments show reflected light steering to angles between -30° and 30° at different resonant wavelengths corresponding to the A exciton and B exciton. This active van der Waals metasurface relies solely on the excitonic resonances of the monolayer MoSe2 material rather than geometric resonances of patterned nanostructures, suggesting the potential to harness the tunability of excitonic resonances for wavefront shaping in emerging photonic applications.

A Single-Step Bottom-up Approach for Synthesis of Highly Uniform Mie-Resonant Crystalline Semiconductor Particles at Visible Wavelengths.

Optically Mie-resonant crystalline silicon nanoparticles have long attracted interest for their unique scattering behaviors. Here, we report a bottom-up nonthermal plasma process that produces highly monodisperse particles, with diameters controllable between 60 and 214 nm, by temporarily electrostatically trapping nanoparticles inside a continuous-flow plasma reactor. The particle size is tuned by adjusting the gas residence time in the reactor. By dispersing the nanoparticles in water, optical extinction measurements indicate colloidal solutions of a particle-based metafluid in which particles support both strong magnetic and electric dipole resonances at visible wavelengths. The spectral overlap of the electric and magnetic resonances gives rise to directional Kerker scattering. The extinction measurements show excellent agreement with Mie theory, supporting the idea that the fabrication process enables particles with narrow distributions in size, shape, and composition. This single-step gas-phase process can also produce Mie-resonant nanoparticles of dielectric materials other than silicon and directly deposit them on the desired substrates.

Amorphous silicon carbide high contrast gratings as highly efficient spectrally selective visible reflectors.

We report spectrally selective visible wavelength reflectors using hydrogenated amorphous silicon carbide (a-SiC:H) as a high index contrast material. Beyond 610nm and through the near infrared spectrum, a-SiC:H exhibits very low loss and exhibits an wavelength averaged index of refraction of n = 3.1. Here we design, fabricate, and characterize such visible reflectors using a hexagonal array of a-SiC:H nanopillars as wavelength-selective mirrors with a stop-band of approximately 40 nm full-width at half maximum. The fabricated high contrast grating exhibits reflectivity R >94% at a resonance wavelength of 642nm with a single layer of a-SiC:H nanopillars. The resonance wavelength is tunable by adjusting the geometrical parameters of the a-SiC:H nanopillar array, and we observe a stop-band spectral center shift from 635 nm up to 642 nm. High contrast gratings formed from a-SiC:H nanopillars are a promising platform for various visible wavelength nanophotonics applications.

Ultra-lightweight mirrors with high solar reflectivity and high infrared emissivity for sun-facing radiative thermal management in space.

We report the design, fabrication, and characterization of ultralight coatings that employ Salisbury screen principles and the unique nature of ITO to achieve frequency selective broadband emissivity. Our coating comprises 60 nm SiO2, 10 nm ITO, 2.3 µm NeXolv LaRC CP1 polyimide and 300 nm Ag, and achieves an aerial mass of 4.07 gm-2. It has a calculated and measured visible spectrum reflectivity of R = 0.893 and R = 0.896 respectively when weighted against AM0 from 300 nm to 1800nm; and a calculated and measured IR spectrum emissivity of e = 0.574 and e = 0.554 weighted against a 300 K blackbody respectively. This simple coating design, fabricated on the centimeter scale, achieves broadband frequency selectivity, with the highest reported thermal performance for an ultralight sun-facing radiative energy management structure.

Lifetime-Limited and Tunable Quantum Light Emission in h-BN via Electric Field Modulation.

Color-center-based single-photon emitters in hexagonal boron nitride (h-BN) have shown promising photophysical properties as sources for quantum light emission. Despite significant advances toward such a goal, achieving lifetime-limited quantum light emission in h-BN has proven to be challenging, primarily due to various broadening mechanisms, including spectral diffusion. Here, we propose and experimentally demonstrate suppression of spectral diffusion by applying an electrostatic field. We observe both Stark shift tuning of the resonant emission wavelength and emission line width reduction (down to 89 MHz) nearly to the homogeneously broadened lifetime limit. Finally, we find a cubic dependence of the line width with respect to temperature at the homogeneous broadening regime. Our results suggest that field tuning in electrostatically gated heterostructures is promising as an approach to control the emission characteristics of h-BN color centers, removing spectral diffusion and providing the energy tunability necessary for integrate of quantum light emission in nanophotonic architectures.

Broadband, Angle- and Polarization-Invariant Antireflective and Absorbing Films by a Scalable Synthesis of Monodisperse Silicon Nanoparticles.

Optically induced magnetic resonances (OMRs) are highly tunable scattering states that cannot be reproduced in systems that only support electric resonances, such as in metals, lossy, or low-index materials. Despite offering unique scattering and coupling behavior, the study of OMRs in thin films has been limited by synthesis and simulation constraints. We report on the absorption and scattering response of OMR-based thin films composed of monodisperse crystalline silicon nanoparticles synthesized using a scalable nonthermal plasma growth technique and tractable simulation framework. The synthesis is solvent and ligand free, ensuring minimal contamination, and crystalline particles form with high yield and a narrow size distribution at close to room temperature. Using a scalable high-throughput deposition method, we deposit random particle films, without the need of a solid host matrix, showing near complete blackbody absorption at the collective OMR. This is achieved using 70% less material than an optimized antireflective-coated crystalline silicon thin film. The film exhibits strongly directional forward scattering with very low reflectivity, thus giving rise to angle- and polarization-insensitive antireflection properties across the visible spectrum. We find that, while commonly used effective medium models cannot capture the optical response, a modified effective medium accounting for multipole resonances and interparticle coupling shows excellent agreement with experiment. The effective permittivity and permeability are written in a mode and cluster resolved form, providing useful insight into how individual resonances and nanoparticle clusters affect the overall film response. Electric and magnetic-mode coupling show dramatically different behavior, resulting in uniquely different spectral broadening.

Nonreciprocal infrared absorption via resonant magneto-optical coupling to InAs.

Nonreciprocal elements are a vital building block of electrical and optical systems. In the infrared regime, there is a particular interest in structures that break reciprocity because their thermal absorptive (and emissive) properties should not obey the Kirchhoff thermal radiation law. In this work, we break time-reversal symmetry and reciprocity in n-type-doped magneto-optic InAs with a static magnetic field where light coupling is mediated by a guided-mode resonator structure, whose resonant frequency coincides with the epsilon-near-zero resonance of the doped indium arsenide. Using this structure, we observe the nonreciprocal absorptive behavior as a function of magnetic field and scattering angle in the infrared. Accounting for resonant and nonresonant optical scattering, we reliably model experimental results that break reciprocal absorption relations in the infrared. The ability to design these nonreciprocal absorbers opens an avenue to explore devices with unequal absorptivity and emissivity in specific channels.