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.

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.

Glucose-responsive enzymatic biomimetic nanodots for H2O2 self-supplied catalytic photothermal/chemodynamic anticancer therapy.

Photothermal therapy (PTT) combined with chemodynamic therapy (CDT) presents an appealing complementary anti-tumor strategy, wherein PTT accelerates the production of reactive oxygen species (ROS) in CDT and CDT eliminates residual tumor tissues that survive from PTT treatment. However, nanomaterials utilized in PTT/CDT are limited by non-specific damage to the entire organism. Herein, a glucose-responsive enzymatic Fe@HRP-ABTS/GOx nanodot is judiciously designed for tumor-specific PTT/CDT via a simple and clean protein-templated biomimetic mineralization synthesis. By oxidizing glucose in tumor cells, glucose oxidase (GOx) activates glucose-responsive tumor therapy and increases the concentration of H2O2 at the tumor site. More importantly, the self-supplied peroxide hydrogen (H2O2) can convert ABTS (2,2'-Hydrazine-bis(3-ethylbenzothiazoline-6-sulfonic acid) diamine salt) into oxidized ABTS (oxABTS) through horseradish peroxidase (HRP) catalysis for PTT and photoacoustic (PA) imaging. Furthermore, the Fe2+ arising from the reduction of Fe3+ by overexpressed GSH reacts with H2O2 to generate intensely reactive •OH through the Fenton reaction, concurrently depleting GSH and inducing efficient tumor CDT. The in vitro and in vivo experiments demonstrate superior cancer cell killing and tumor eradication effect of Fe@HRP-ABTS/GOx nanodot under near-infrared (NIR) laser irradiation. Collectively, the nanodots provide mutually reinforcing catalytic PTT/CDT anti-tumor strategies for treating liver cancer and potentially other malignancies. STATEMENT OF SIGNIFICANCE: Combinatorial antitumor therapy with nanomedicines presents great prospects for development. However, the limitation of non-specific damage to normal tissues hinders its further clinical application. In this work, we fabricated tumor-selective biomimetic Fe@HRP-ABTS/GOx nanodots for H2O2 self-supplied catalytic photothermal/chemodynamic therapy of tumors. The biomimetic synthesis strategy provides the nanodots with enzymatic activity in response to glucose to produce H2O2. The self-supplied H2O2 initiates photothermal therapy with oxidized ABTS and enhances chemodynamic therapy through simultaneous •OH generation and GSH depletion. Our work provides a new paradigm for developing tumor-selective catalytic nanomedicines and will guide further clinical translation of the enzymatic biomimetic synthesis strategy.

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.

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.

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.

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.

Transparent multispectral photodetectors mimicking the human visual system.

Compact and lightweight photodetection elements play a critical role in the newly emerging augmented reality, wearable and sensing technologies. In these technologies, devices are preferred to be transparent to form an optical interface between a viewer and the outside world. For this reason, it is of great value to create detection platforms that are imperceptible to the human eye directly onto transparent substrates. Semiconductor nanowires (NWs) make ideal photodetectors as their optical resonances enable parsing of the multi-dimensional information carried by light. Unfortunately, these optical resonances also give rise to strong, undesired light scattering. In this work, we illustrate how a new optical resonance arising from the radiative coupling between arrayed silicon NWs can be harnessed to remove reflections from dielectric interfaces while affording spectro-polarimetric detection. The demonstrated transparent photodetector concept opens up promising platforms for transparent substrates as the base for opto-electronic devices and in situ optical measurement systems.

Reversible and selective ion intercalation through the top surface of few-layer MoS2.

Electrochemical intercalation of ions into the van der Waals gap of two-dimensional (2D) layered materials is a promising low-temperature synthesis strategy to tune their physical and chemical properties. It is widely believed that ions prefer intercalation into the van der Waals gap through the edges of the 2D flake, which generally causes wrinkling and distortion. Here we demonstrate that the ions can also intercalate through the top surface of few-layer MoS2 and this type of intercalation is more reversible and stable compared to the intercalation through the edges. Density functional theory calculations show that this intercalation is enabled by the existence of natural defects in exfoliated MoS2 flakes. Furthermore, we reveal that sealed-edge MoS2 allows intercalation of small alkali metal ions (e.g., Li+ and Na+) and rejects large ions (e.g., K+). These findings imply potential applications in developing functional 2D-material-based devices with high tunability and ion selectivity.

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.

Visible-Frequency Dielectric Metasurfaces for Multiwavelength Achromatic and Highly Dispersive Holograms.

Dielectric metasurfaces built up with nanostructures of high refractive index represent a powerful platform for highly efficient flat optical devices due to their easy-tuning electromagnetic scattering properties and relatively high transmission efficiencies. Here we show visible-frequency silicon metasurfaces formed by three kinds of nanoblocks multiplexed in a subwavelength unit to constitute a metamolecule, which are capable of wavefront manipulation for red, green, and blue light simultaneously. Full phase control is achieved for each wavelength by independently changing the in-plane orientations of the corresponding nanoblocks to induce the required geometric phases. Achromatic and highly dispersive meta-holograms are fabricated to demonstrate the wavefront manipulation with high resolution. This technique could be viable for various practical holographic applications and flat achromatic devices.

Polarization-independent and high-efficiency dielectric metasurfaces for visible light.

Dielectric metasurfaces are capable of completely manipulating the phase, amplitude, and polarization of light with high spatial resolutions. The emerging design based on high-index and low-loss dielectrics has led to the realization of novel metasurfaces with high transmissions, but these devices usually operate at the limited bandwidth, and are sensitive to the incident polarization. Here, we report the realization of the polarization-independent and high-efficiency silicon metasurfaces spanning the visible wavelengths about 200 nm. The fabricated computer-generated meta-holograms exhibit a 90% diffraction efficiency, which are verified by gradient metasurfaces with measured efficiencies up to 93% at 670 nm, and exceeding 75% at the wavelengths from 600 to 800 nm for the two orthogonally polarized incidences. These dielectric metasurfaces effectively decouple the phase modulation from the polarization states and frequencies for visible light, which hold great potential for novel flat optical devices operating over a broad spectrum.

Excitation and propagation of surface plasmon polaritons on a non-structured surface with a permittivity gradient.

Accompanied by the rise of plasmonic materials beyond those based on noble metals and the development of advanced materials processing techniques, it is important to understand the plasmonic behavior of materials with large-scale inhomogeneity (such as gradient permittivity materials) because they cannot be modeled simply as scatterers. In this paper, we theoretically analyze the excitation and propagation of surface plasmon polaritons (SPPs) on a planar interface between a homogeneous dielectric and a material with a gradient of negative permittivity. We demonstrate the following: (i) free-space propagating waves and surface waves can be coupled by a gradient negative-permittivity material and (ii) the coupling can be enhanced if the material permittivity variation is suitably designed. This theory is then verified by numerical simulations. A direct application of this theory, 'rainbow trapping', is also proposed, considering a realistic design based on doped indium antimonide. This theory may lead to various applications, such as ultracompact spectroscopy and dynamically controllable generation of SPPs.