Scalable and robust beam shaping using apodized fish-bone grating couplers.

Efficient power coupling between on-chip guided and free-space optical modes requires precision spatial mode matching with apodized grating couplers. Yet, grating apodizations are often limited by the minimum feature size of the fabrication approach. This is especially challenging when small feature sizes are required to fabricate gratings at short wavelengths or to achieve weakly scattered light for large-area gratings. Here, we demonstrate a fish-bone grating coupler for precision beam shaping and the generation of millimeter-scale beams at 461 nm wavelength. Our design decouples the minimum feature size from the minimum achievable optical scattering strength, allowing smooth turn-on and continuous control of the emission. Our approach is compatible with commercial foundry photolithography and has reduced sensitivity to both the resolution and the variability of the fabrication approach compared to subwavelength meta-gratings, which often require electron beam lithography.

Integrating planar photonics for multi-beam generation and atomic clock packaging on chip.

The commercialization of atomic technologies requires replacing laboratory-scale laser setups with compact and manufacturable optical platforms. Complex arrangements of free-space beams can be generated on chip through a combination of integrated photonics and metasurface optics. In this work, we combine these two technologies using flip-chip bonding and demonstrate an integrated optical architecture for realizing a compact strontium atomic clock. Our planar design includes twelve beams in two co-aligned magneto-optical traps. These beams are directed above the chip to intersect at a central location with diameters as large as 1 cm. Our design also includes two co-propagating beams at lattice and clock wavelengths. These beams emit collinearly and vertically to probe the center of the magneto-optical trap, where they will have diameters of ≈100 µm. With these devices we demonstrate that our integrated photonic platform is scalable to an arbitrary number of beams, each with different wavelengths, geometries, and polarizations.

Surface-Normal Free-Space Beam Projection via Slow-Light Standing-Wave Resonance Photonic Gratings.

On-chip grating couplers directly connect photonic circuits to free-space light. The commonly used photonic gratings have been specialized for small areas, specific intensity profiles, and nonvertical beam projection. This falls short of the precise and flexible wavefront control over large beam areas needed to empower emerging integrated miniaturized optical systems that leverage volumetric light-matter interactions, including trapping, cooling, and interrogation of atoms, bio- and chemi- sensing, and complex free-space interconnect. The large coupler size challenges general inverse design techniques, and solutions obtained by them are often difficult to physically understand and generalize. Here, by posing the problem to a carefully constrained computational inverse-design algorithm capable of large area structures, we discover a qualitatively new class of grating couplers. The numerically found solutions can be understood as coupling an incident photonic slab mode to a spatially extended slow-light (near-zero refractive index) region, backed by a reflector. The structure forms a spectrally broad standing wave resonance at the target wavelength, radiating vertically into free space. A reflectionless adiabatic transition critically couples the incident photonic mode to the resonance, and the numerically optimized lower cladding provides 70% overall theoretical conversion efficiency. We have experimentally validated an efficient surface normal collimated emission of ≈90 µm full width at half-maximum Gaussian at the thermally tunable operating wavelength of ≈780 nm. The variable-mesh-deformation inverse design approach scales to extra large photonic devices, while directly implementing the fabrication constraints. The deliberate choice of smooth parametrization resulted in a novel type of solution, which is both efficient and physically comprehensible.

Exceptional points in lossy media lead to deep polynomial wave penetration with spatially uniform power loss.

Waves entering a spatially uniform lossy medium typically undergo exponential intensity decay, arising from either the energy loss of the Beer-Lambert-Bouguer transmission law or the evanescent penetration during reflection. Recently, exceptional point singularities in non-Hermitian systems have been linked to unconventional wave propagation. Here, we theoretically propose and experimentally demonstrate exponential decay free wave propagation in a purely lossy medium. We observe up to 400-wave deep polynomial wave propagation accompanied by a uniformly distributed energy loss across a nanostructured photonic slab waveguide with exceptional points. We use coupled-mode theory and fully vectorial electromagnetic simulations to predict deep wave penetration manifesting spatially constant radiation losses through the entire structured waveguide region regardless of its length. The uncovered exponential decay free wave phenomenon is universal and holds true across all domains supporting physical waves, finding immediate applications for generating large, uniform and surface-normal free-space plane waves directly from dispersion-engineered photonic chip surfaces.

Meta-grating outcouplers for optimized beam shaping in the visible.

Accurate coupling between optical modes at the interface between photonic chips and free space is required for the development of many on-chip devices. This control is critical in quantum technologies where large-diameter beams with designed mode profiles are required. Yet, these designs are often difficult to achieve at shorter wavelengths where fabrication limits the resolution of designed devices. In this work we demonstrate optimized outcoupling of free-space beams at 461 nm using a meta-grating approach that achieves a 16 dB improvement in the apodized outcoupling strength. We design and fabricate devices, demonstrating accurate reproduction of beams with widths greater than 100 µm.

Probing Electrified Liquid-Solid Interfaces with Scanning Electron Microscopy.

Electrical double layers play a key role in a variety of electrochemical systems. The mean free path of secondary electrons in aqueous solutions is on the order of a nanometer, making them suitable for probing ultrathin electrical double layers at solid-liquid electrolyte interfaces. Employing graphene as an electron-transparent electrode in a two-electrode electrochemical system, we show that the secondary electron yield of the graphene-liquid interface depends on the ionic strength and concentration of the electrolyte and the applied bias at the remote counter electrode. These observations have been related to polarization-induced changes in the potential distribution within the electrical double layer and demonstrate the feasibility of using scanning electron microscopy to examine and map electrified liquid-solid interfaces.

Nanoscale Mapping of the Double Layer Potential at the Graphene-Electrolyte Interface.

The electrical double layer (EDL) governs the operation of multiple electrochemical devices, determines reaction potentials, and conditions ion transport through cellular membranes in living organisms. The few existing methods of EDL probing have low spatial resolution, usually only providing spatially averaged information. On the other hand, traditional Kelvin probe force microscopy (KPFM) is capable of mapping potential with nanoscale lateral resolution but cannot be used in electrolytes with concentrations higher than several mmol/L. Here, we resolve this experimental impediment by combining KPFM with graphene-capped electrolytic cells to quantitatively measure the potential drop across the EDL in aqueous electrolytes of decimolar and molar concentrations with a high lateral resolution. The surface potential of graphene in contact with deionized water and 0.1 mol/L solutions of CuSO4 and MgSO4 as a function of counter electrode voltage is reported. The measurements are supported by numerical modeling to reveal the role of the graphene membrane in potential screening and to determine the EDL potential drop. The proposed approach proves to be especially useful for imaging spatially inhomogeneous systems, such as nanoparticles submerged in an electrolyte solution. It could be suitable for in operando and in vivo measurements of the potential drop in the EDL on the surfaces of nanocatalysts and biological cells in equilibrium with liquid solutions.

Metasurface-Integrated Photonic Platform for Versatile Free-Space Beam Projection with Polarization Control.

Densely integrated photonic circuits enable scalable, complex processing of optical signals, including modulation, multiplexing, wavelength conversion, and detection. Directly interfacing such integrated circuits to free-space optical modes will enable novel optical functions, such as chip-scale sensing, interchip free-space interconnect and cooling, trapping, and interrogation of atoms. However, doing this within the limits of planar batch fabrication requires new approaches for bridging the large mode scale mismatch. Here, by integrating a dielectric metasurface with an extreme photonic mode converter, we create a versatile nanophotonic platform for efficient coupling to arbitrary-defined free-space radiation of 780 nm wavelength with well-controlled spatially-dependent polarization, phase, and intensity. Without leaving the chip, the high index photonic mode is converted first to a ≈ 200 µm wide, precisely collimated, linearly-polarized Gaussian beam, which is then modified by a planar, integrated, low-loss metasurface. We demonstrate high numerical aperture, diffraction limited focusing to an ≈ 473 nm spot at an ≈ 75 µm working distance, and combine it with simultaneous conversion from linear to elliptical polarization. All device components are lithographically defined and can be batch fabricated, facilitating future chip-scale low-cost hybrid photonic systems for bio-sensing, nonlinear signal processing and atomic quantum sensing, frequency references and memory.

Photonic waveguide to free-space Gaussian beam extreme mode converter.

Integration of photonic chips with millimeter-scale atomic, micromechanical, chemical, and biological systems can advance science and enable new miniaturized hybrid devices and technology. Optical interaction via small evanescent volumes restricts performance in applications such as gas spectroscopy, and a general ability to photonically access optical fields in large free-space volumes is desired. However, conventional inverse tapers and grating couplers do not directly scale to create wide, high-quality collimated beams for low-loss diffraction-free propagation over many millimeters in free space, necessitating additional bulky collimating optics and expensive alignment. Here, we develop an extreme mode converter, which is a compact planar photonic structure that efficiently couples a 300 nm × 250 nm silicon nitride high-index single-mode waveguide to a well-collimated near surface-normal Gaussian beam with an ≈160 µm waist, which corresponds to an increase in the modal area by a factor of >105. The beam quality is thoroughly characterized, and propagation over 4 mm in free space and coupling back into a single-mode photonic waveguide with low loss via a separate identical mode converter is demonstrated. To achieve low phase error over a beam area that is >100× larger than that of a typical grating coupler, our approach separates the two-dimensional mode expansion into two sequential separately optimized stages, which create a fully expanded and well-collimated Gaussian slab mode before out-coupling it into free space. Developed at 780 nm for integration with chip-scale atomic vapor cell cavities, our design can be adapted for visible, telecommunication, or other wavelengths. The technique can be expanded to more arbitrary phase and intensity control of both large-diameter, free-space optical beams and wide photonic slab modes.

From Microparticles to Nanowires and Back: Radical Transformations in Plated Li Metal Morphology Revealed via in Situ Scanning Electron Microscopy.

Li metal is the preferred anode material for all-solid-state Li batteries. However, a stable plating and stripping of Li metal at the anode-solid electrolyte interface remains a significant challenge particularly at practically feasible current densities. This problem usually relates to high and/or inhomogeneous Li-electrode-electrolyte interfacial impedance and formation and growth of high-aspect-ratio dendritic Li deposits at the electrode-electrolyte interface, which eventually shunt the battery. To better understand details of Li metal plating, we use operando electron microscopy and Auger spectroscopy to probe nucleation, growth, and stripping of Li metal during cycling of a model solid-state Li battery as a function of current density and oxygen pressure. We find a linear correlation between the nucleation density of Li clusters and the charging rate in an ultrahigh vacuum, which agrees with a classical nucleation and growth model. Moreover, the trace amount of oxidizing gas (≈10-6 Pa of O2) promotes the Li growth in a form of nanowires due to a fine balance between the ion current density and a growth rate of a thin lithium-oxide shell on the surface of the metallic Li. Interestingly, increasing the partial pressure of O2 to 10-5 Pa resumes Li plating in a form of 3D particles. Our results demonstrate the importance of trace amounts of preexisting or ambient oxidizing species on lithiation processes in solid-state batteries.

Interfacial Electrochemistry in Liquids Probed with Photoemission Electron Microscopy.

Studies of the electrified solid-liquid interfaces are crucial for understanding biological and electrochemical systems. Until recently, use of photoemission electron microscopy (PEEM) for such purposes has been hampered by incompatibility of the liquid samples with ultrahigh vacuum environment of the electron optics and detector. Here we demonstrate that the use of ultrathin electron transparent graphene membranes, which can sustain large pressure differentials and act as a working electrode, makes it possible to probe electrochemical reactions in operando in liquid environments with PEEM.

Imaging and Analysis of Encapsulated Objects through Self-Assembled Electron and Optically Transparent Graphene Oxide Membranes.

We demonstrate a technique for facile encapsulation and adhesion of micro- and nano objects on arbitrary substrates, stencils, and micro structured surfaces by ultrathin graphene oxide membranes via a simple drop casting of graphene oxide solution. A self-assembled encapsulating membrane forms during the drying process at the liquid-air and liquid-solid interfaces and consists of a water-permeable quasi-2D network of overlapping graphene oxide flakes. Upon drying and interlocking between the flakes, the encapsulating coating around the object becomes mechanically robust, chemically protective, and yet highly transparent to electrons and photons in a wide energy range, enabling microscopic and spectroscopic access to encapsulated objects. The characteristic encapsulation scenarios were demonstrated on a set of representative inorganic and organic micro and nano-objects and microstructured surfaces. Different coating regimes can be achieved by controlling the pH of the supporting solution, and the hydrophobicity and morphology of interfaces. Several specific phenomena such as compression of encased objects by contracting membranes as well as hierarchical encapsulations were observed. Finally, electron as well as optical microscopy and analysis of encapsulated objects along with the membrane effect on the image contrast formation, and signal attenuation are discussed.

Graphene Microcapsule Arrays for Combinatorial Electron Microscopy and Spectroscopy in Liquids.

Atomic-scale thickness, molecular impermeability, low atomic number, and mechanical strength make graphene an ideal electron-transparent membrane for material characterization in liquids and gases with scanning electron microscopy and spectroscopy. Here, we present a novel sample platform made of an array of thousands of identical isolated graphene-capped microchannels with high aspect ratio. A combination of a global wide field of view with high resolution local imaging of the array allows for high throughput in situ studies as well as for combinatorial screening of solutions, liquid interfaces, and immersed samples. We demonstrate the capabilities of this platform by studying a pure water sample in comparison with alkali halide solutions, a model electrochemical plating process, and beam-induced crystal growth in liquid electrolyte. Spectroscopic characterization of liquid interfaces and immersed objects with Auger and X-ray fluorescence analysis through the graphene membrane are also demonstrated.

Enabling Photoemission Electron Microscopy in Liquids via Graphene-Capped Microchannel Arrays.

Photoelectron emission microscopy (PEEM) is a powerful tool to spectroscopically image dynamic surface processes at the nanoscale, but it is traditionally limited to ultrahigh or moderate vacuum conditions. Here, we develop a novel graphene-capped multichannel array sample platform that extends the capabilities of photoelectron spectromicroscopy to routine liquid and atmospheric pressure studies with standard PEEM setups. Using this platform, we show that graphene has only a minor influence on the electronic structure of water in the first few layers and thus will allow for the examination of minimally perturbed aqueous-phase interfacial dynamics. Analogous to microarray screening technology in biomedical research, our platform is highly suitable for applications in tandem with large-scale data mining, pattern recognition, and combinatorial methods for spectro-temporal and spatiotemporal analyses at solid-liquid interfaces. Applying Bayesian linear unmixing algorithm to X-ray induced water radiolysis process, we were able to discriminate between different radiolysis scenarios and observe a metastable "wetting" intermediate water layer during the late stages of bubble formation.

Toward Clean Suspended CVD Graphene.

The application of suspended graphene as electron transparent supporting media in electron microscopy, vacuum electronics, and micromechanical devices requires the least destructive and maximally clean transfer from their original growth substrate to the target of interest. Here, we use thermally evaporated anthracene films as the sacrificial layer for graphene transfer onto an arbitrary substrate. We show that clean suspended graphene can be achieved via desorbing the anthracene layer at temperatures in the 100 °C to 150 °C range, followed by two sequential annealing steps for the final cleaning, using Pt catalyst and activated carbon. The cleanliness of the suspended graphene membranes was analyzed employing the high surface sensitivity of low energy scanning electron microscopy and x-ray photoelectron spectroscopy. A quantitative comparison with two other commonly used transfer methods revealed the superiority of the anthracene approach to obtain larger area of clean, suspended CVD graphene. Our graphene transfer method based on anthracene paves the way for integrating cleaner graphene in various types of complex devices, including the ones that are heat and humidity sensitive.

Photoelectron spectroscopy of wet and gaseous samples through graphene membranes.

Photoelectron spectroscopy (PES) and microscopy are highly important for exploring morphologically and chemically complex liquid-gas, solid-liquid and solid-gas interfaces under realistic conditions, but the very small electron mean free path inside dense media imposes serious experimental challenges. Currently, near ambient pressure PES is conducted using dexterously designed electron energy analyzers coupled with differentially pumped electron lenses which make it possible to conduct PES measurements at a few hPa. This report proposes an alternative ambient pressure approach that can be applied to a broad class of samples and be implemented in conventional PES instruments. It uses ultrathin electron transparent but molecular impermeable membranes to isolate the high pressure sample environment from the high vacuum PES detection system. We demonstrate that the separating graphene membrane windows are both mechanically robust and sufficiently transparent for electrons in a wide energy range to allow soft X-ray PES of liquid and gaseous water. The performed proof-of-principle experiments confirm the possibility to probe vacuum-incompatible toxic or reactive samples placed inside such hermetic, gas flow or fluidic environmental cells.

Harmonic modulation of light by means of collinear acousto-optic interaction.

The collinear anisotropic interaction of light with a standing acoustic wave generated in a lithium niobate crystal is discussed. Diffraction may be applied for harmonic modulation of laser light. The analysis of the light modulation is based on the concept of vector diagrams. A set of differential equations is derived to describe up to five interacting optic waves in the material. It is shown that solution of the equations by the method of successive approximations yields amplitudes of electric fields corresponding to diffracted and transmitted optical beams at the output of the crystal. Dependences of the amplitudes of the interacting waves on the acoustic frequency and length of the acousto-optic interaction are also discussed.