Solution-Based Synthesis of Layered Two-Dimensional Oxides as Broadband Emitters.

Preparing transition-metal oxides in their two-dimensional (2D) form is the key to exploring their unrevealed low-dimensional properties, such as the p-type transparent superconductivity, topological Mott insulator state, existence of the condensed 2D electron/hole gas, and strain-tunable catalysis. However, existing approaches suffer from the specific constraint techniques and precursors that limit their product types. Here, we report a solution-based method to directly synthesize KNbO2 in 2D by an out-of-the-pot growth process at low temperature, which is observed directly in real time. The developed method can also be applied to other 2D ternary oxide syntheses, including CsNbO2 and composited NaxK1-xNbO2, and it can be extended to the preparation of self-assembled nanofilms. In addition, We demonstrate the emission of broadband photoluminescence (PL, λ ∼ 350-800 nm) from as-synthesized single-crystal 2D KNbO2 sheets down to a single unit cell thickness. The ultra-broadband emission is ascribed to the self-trapped excitation state (STEs) from the in-phase distortion of the NbO6 octahedrons in 2D NbO2- layers. Beyond the broader luminescent range and the robust material thermal stability of niobates, the absence of sample size restrictions and the large aspect ratio of the 2D oxide sheets will provide opportunities in miniaturizing and advancing 2D-materials integrated optoelectronic devices.

Helical van der Waals crystals with discretized Eshelby twist.

The ability to manipulate the twisting topology of van der Waals structures offers a new degree of freedom through which to tailor their electrical and optical properties. The twist angle strongly affects the electronic states, excitons and phonons of the twisted structures through interlayer coupling, giving rise to exotic optical, electric and spintronic behaviours1-5. In twisted bilayer graphene, at certain twist angles, long-range periodicity associated with moiré patterns introduces flat electronic bands and highly localized electronic states, resulting in Mott insulating behaviour and superconductivity3,4. Theoretical studies suggest that these twist-induced phenomena are common to layered materials such as transition-metal dichalcogenides and black phosphorus6,7. Twisted van der Waals structures are usually created using a transfer-stacking method, but this method cannot be used for materials with relatively strong interlayer binding. Facile bottom-up growth methods could provide an alternative means to create twisted van der Waals structures. Here we demonstrate that the Eshelby twist, which is associated with a screw dislocation (a chiral topological defect), can drive the formation of such structures on scales ranging from the nanoscale to the mesoscale. In the synthesis, axial screw dislocations are first introduced into nanowires growing along the stacking direction, yielding van der Waals nanostructures with continuous twisting in which the total twist rates are defined by the radii of the nanowires. Further radial growth of those twisted nanowires that are attached to the substrate leads to an increase in elastic energy, as the total twist rate is fixed by the substrate. The stored elastic energy can be reduced by accommodating the fixed twist rate in a series of discrete jumps. This yields mesoscale twisting structures consisting of a helical assembly of nanoplates demarcated by atomically sharp interfaces with a range of twist angles. We further show that the twisting topology can be tailored by controlling the radial size of the structure.

All-Silicon Broadband Ultraviolet Metasurfaces.

Featuring high photon energy and short wavelength, ultraviolet (UV) light enables numerous applications such as high-resolution imaging, photolithography, and sensing. In order to manipulate UV light, bulky optics are usually required, and hence do not meet the fast-growing requirements of integration in compact systems. Recently, metasurfaces have shown unprecedented control of light, enabling substantial miniaturization of photonic devices from terahertz to visible regions. However, material challenges have hampered the realization of such functionalities at shorter wavelengths. Herein, it is experimentally demonstrated that all-silicon (Si) metasurfaces with thicknesses of only one-tenth of the working wavelength can be designed and fabricated to manipulate broadband UV light with efficiencies comparable to plasmonic metasurface performance in infrared (IR). Also, for the first time, photolithography enabled by metasurface-generated UV holograms is shown. Such performance enhancement is attributed to increased scattering cross sections of Si antennas in the UV range, which is adequately modeled via a circuit. The new platform introduced here will deepen the understanding of light-matter interactions and introduce even more material options to broadband metaphotonic applications, including those in integrated photonics and holographic lithography technologies.

Solution-Based, Template-Assisted Realization of Large-Scale Graphitic ZnO.

With a honeycomb single-atomic-layer structure similar to those of graphene and hexagonal boron nitride (hBN), the graphitic phase of ZnO (gZnO) have been predicted to offer many advantages for engineering, including high-temperature stability in ambient conditions and great potential in heterostructure applications. However, there is little experimental data about this hexagonal phase due to the difficulty of synthesizing large-area gZnO for characterization and applications. In this work, we demonstrate a solution-based approach to realize gZnO nanoflakes with thicknesses down to a monolayer and sizes up to 20 µm. X-ray photoelectron spectroscopy, X-ray absorption near-edge spectroscopy, photoluminescence, atomic force microscopy, and electron microscopy characterizations are conducted on synthesized gZnO samples. Measurements show significant changes to the electronic band structure compared to its bulk phase, including an increase of the band gap to 4.8 eV. The gZnO nanosheets also exhibit excellent stability at temperatures as high as 800 °C in ambient environment. This wide band gap layered material provides us with a platform for harsh environment electronic devices, deep ultraviolet optical applications, and a practical alternative for hBN. Our synthesis method may also be applied to achieve other types of 2D oxides.

Subwavelength light confinement and enhancement enabled by dissipative dielectric nanostructures.

Dissipative loss in optical materials is considered one of the major challenges in nano-optics. Here we show that, counter-intuitively, a large imaginary part of material permittivity contributes positively to subwavelength light enhancement and confinement. The Purcell factor and the fluorescence enhancement of dissipative dielectric bowtie nanoantennas, such as Si in ultraviolet (UV), are demonstrated to be orders of magnitude higher than their lossless dielectric counterparts, which is particularly favorable in deep UV applications where metals are plasmonically inactive. The loss-facilitated field enhancement is the result of a large material property contrast and an electric field discontinuity. These dissipative dielectric nanostructures can be easily achieved with a great variety of dielectrics at their Lorentz oscillation frequencies, thus having the potential to build a completely new material platform boosting light-matter interaction over broader frequency ranges, with advantages such as bio-compatibility, CMOS compatibility, and harsh environment endurance.

Three-dimensional Architecture Enabled by Strained Two-dimensional Material Heterojunction.

Engineering the structure of materials endows them with novel physical properties across a wide range of length scales. With high in-plane stiffness and strength, but low flexural rigidity, two-dimensional (2D) materials are excellent building blocks for nanostructure engineering. They can be easily bent and folded to build three-dimensional (3D) architectures. Taking advantage of the large lattice mismatch between the constituents, we demonstrate a 3D heterogeneous architecture combining a basal Bi2Se3 nanoplate and wavelike Bi2Te3 edges buckling up and down forming periodic ripples. Unlike 2D heterostructures directly grown on substrates, the solution-based synthesis allows the heterostructures to be free from substrate influence during the formation process. The balance between bending and in-plane strain energies gives rise to controllable rippling of the material. Our experimental results show clear evidence that the wavelengths and amplitudes of the ripples are dependent on both the widths and thicknesses of the rippled material, matching well with continuum mechanics analysis. The rippled Bi2Se3/Bi2Te3 heterojunction broadens the horizon for the application of 2D materials heterojunction and the design and fabrication of 3D architectures based on them, which could provide a platform to enable nanoscale structure generation and associated photonic/electronic properties manipulation for optoelectronic and electromechanic applications.

A 0.2 V Micro-Electromechanical Switch Enabled by a Phase Transition.

Micro-electromechanical (MEM) switches, with advantages such as quasi-zero leakage current, emerge as attractive candidates for overcoming the physical limits of complementary metal-oxide semiconductor (CMOS) devices. To practically integrate MEM switches into CMOS circuits, two major challenges must be addressed: sub 1 V operating voltage to match the voltage levels in current circuit systems and being able to deliver at least millions of operating cycles. However, existing sub 1 V mechanical switches are mostly subject to significant body bias and/or limited lifetimes, thus failing to meet both limitations simultaneously. Here 0.2 V MEM switching devices with ≳106 safe operating cycles in ambient air are reported, which achieve the lowest operating voltage in mechanical switches without body bias reported to date. The ultralow operating voltage is mainly enabled by the abrupt phase transition of nanolayered vanadium dioxide (VO2 ) slightly above room temperature. The phase-transition MEM switches open possibilities for sub 1 V hybrid integrated devices/circuits/systems, as well as ultralow power consumption sensors for Internet of Things applications.

Multifunctional Microelectro-Opto-mechanical Platform Based on Phase-Transition Materials.

Along with the rapid development of hybrid electronic-photonic systems, multifunctional devices with dynamic responses have been widely investigated for improving many optoelectronic applications. For years, microelectro-opto-mechanical systems (MEOMS), one of the major approaches to realizing multifunctionality, have demonstrated profound reconfigurability and great reliability. However, modern MEOMS still suffer from limitations in modulation depth, actuation voltage, or miniaturization. Here, we demonstrate a new MEOMS multifunctional platform with greater than 50% optical modulation depth over a broad wavelength range. This platform is realized by a specially designed cantilever array, with each cantilever consisting of vanadium dioxide, chromium, and gold nanolayers. The abrupt structural phase transition of the embedded vanadium dioxide enables the reconfigurability of the platform. Diverse stimuli, such as temperature variation or electric current, can be utilized to control the platform, promising CMOS-compatible operating voltage. Multiple functionalities, including an active enhanced absorber and a reprogrammable electro-optic logic gate, are experimentally demonstrated to address the versatile applications of the MEOMS platform in fields such as communication, energy harvesting, and optical computing.

A Lithography-Free and Field-Programmable Photonic Metacanvas.

The unique correspondence between mathematical operators and photonic elements in wave optics enables quantitative analysis of light manipulation with individual optical devices. Phase-transition materials are able to provide real-time reconfigurability of these devices, which would create new optical functionalities via (re)compilation of photonic operators, as those achieved in other fields such as field-programmable gate arrays (FPGA). Here, by exploiting the hysteretic phase transition of vanadium dioxide, an all-solid, rewritable metacanvas on which nearly arbitrary photonic devices can be rapidly and repeatedly written and erased is presented. The writing is performed with a low-power laser and the entire process stays below 90 °C. Using the metacanvas, dynamic manipulation of optical waves is demonstrated for light propagation, polarization, and reconstruction. The metacanvas supports physical (re)compilation of photonic operators akin to that of FPGA, opening up possibilities where photonic elements can be field programmed to deliver complex, system-level functionalities.