Topological polaritons and photonic magic angles in twisted α-MoO3 bilayers.

Twisted two-dimensional bilayer materials exhibit many exotic electronic phenomena. Manipulating the 'twist angle' between the two layers enables fine control of the electronic band structure, resulting in magic-angle flat-band superconductivity1,2, the formation of moiré excitons3-8 and interlayer magnetism9. However, there are limited demonstrations of such concepts for photons. Here we show how analogous principles, combined with extreme anisotropy, enable control and manipulation of the photonic dispersion of phonon polaritons in van der Waals bilayers. We experimentally observe tunable topological transitions from open (hyperbolic) to closed (elliptical) dispersion contours in bilayers of α-phase molybdenum trioxide (α-MoO3), arising when the rotation between the layers is at a photonic magic twist angle. These transitions are induced by polariton hybridization and are controlled by a topological quantity. At the transitions the bilayer dispersion flattens, exhibiting low-loss tunable polariton canalization and diffractionless propagation with a resolution of less than λ0/40, where λ0 is the free-space wavelength. Our findings extend twistronics10 and moiré physics to nanophotonics and polaritonics, with potential applications in nanoimaging, nanoscale light propagation, energy transfer and quantum physics.

In-plane anisotropic and ultra-low-loss polaritons in a natural van der Waals crystal.

Polaritons-hybrid light-matter excitations-enable nanoscale control of light. Particularly large polariton field confinement and long lifetimes can be found in graphene and materials consisting of two-dimensional layers bound by weak van der Waals forces1,2 (vdW materials). These polaritons can be tuned by electric fields3,4 or by material thickness5, leading to applications including nanolasers6, tunable infrared and terahertz detectors7, and molecular sensors8. Polaritons with anisotropic propagation along the surface of vdW materials have been predicted, caused by in-plane anisotropic structural and electronic properties9. In such materials, elliptic and hyperbolic in-plane polariton dispersion can be expected (for example, plasmon polaritons in black phosphorus9), the latter leading to an enhanced density of optical states and ray-like directional propagation along the surface. However, observation of anisotropic polariton propagation in natural materials has so far remained elusive. Here we report anisotropic polariton propagation along the surface of α-MoO3, a natural vdW material. By infrared nano-imaging and nano-spectroscopy of semiconducting α-MoO3 flakes and disks, we visualize and verify phonon polaritons with elliptic and hyperbolic in-plane dispersion, and with wavelengths (up to 60 times smaller than the corresponding photon wavelengths) comparable to those of graphene plasmon polaritons and boron nitride phonon polaritons3-5. From signal oscillations in real-space images we measure polariton amplitude lifetimes of 8 picoseconds, which is more than ten times larger than that of graphene plasmon polaritons at room temperature10. They are also a factor of about four larger than the best values so far reported for phonon polaritons in isotopically engineered boron nitride11 and for graphene plasmon polaritons at low temperatures12. In-plane anisotropic and ultra-low-loss polaritons in vdW materials could enable directional and strong light-matter interactions, nanoscale directional energy transfer and integrated flat optics in applications ranging from bio-sensing to quantum nanophotonics.

Interfacial engineering of halide perovskites and two-dimensional materials.

Recently, halide perovskites (HPs) and layered two-dimensional (2D) materials have received significant attention from industry and academia alike. HPs are emerging materials that have exciting photoelectric properties, such as a high absorption coefficient, rapid carrier mobility and high photoluminescence quantum yields, making them excellent candidates for various optoelectronic applications. 2D materials possess confined carrier mobility in 2D planes and are widely employed in nanostructures to achieve interfacial modification. HP/2D material interfaces could potentially reveal unprecedented interfacial properties, including light absorbance with desired spectral overlap, tunable carrier dynamics and modified stability, which may lead to several practical applications. In this review, we attempt to provide a comprehensive perspective on the development of interfacial engineering of HP/2D material interfaces. Specifically, we highlight the recent progress in HP/2D material interfaces considering their architectures, electronic energetics tuning and interfacial properties, discuss the potential applications of these interfaces and analyze the challenges and future research directions of interfacial engineering of HP/2D material interfaces. This review links the fields of HPs and 2D materials through interfacial engineering to provide insights into future innovations and their great potential applications in optoelectronic devices.

Shear polaritons from transformation optics.

Natural in-plane hyperbolic crystals (such as α-MoO3) and natural monoclinic crystals (such as ß-Ga2O3) have recently drawn great research focus. Despite their obvious similarities, however, these two kinds of materials are usually studied as separate topics. In this Letter, we explore the intrinsic relationship between materials like α-MoO3 and ß-Ga2O3 under the framework of transformation optics, providing another perspective to understand the asymmetry of hyperbolic shear polaritons. It is worth mentioning that we demonstrate this novel, to the best of our knowledge, method from theoretical analysis and numerical simulations, which maintain a high degree of consistency. Our work not only combines natural hyperbolic materials with the theory of classical transformation optics, but also opens new avenues for future studies of various natural materials.

Tailoring Topological Transitions of Anisotropic Polaritons by Interface Engineering in Biaxial Crystals.

Polaritons in polar biaxial crystals with extreme anisotropy offer a promising route to manipulate nanoscale light-matter interactions. The dynamic modulation of their dispersion is of great significance for future integrated nano-optics but remains challenging. Here, we report tunable topological transitions in biaxial crystals enabled by interface engineering. We theoretically demonstrate such tailored polaritons at the interface of heterostructures between graphene and α-phase molybdenum trioxide (α-MoO3). The interlayer coupling can be modulated by both the stack of graphene and α-MoO3 and the magnitude of the Fermi level in graphene enabling a dynamic topological transition. More interestingly, we found that the wavefront transition occurs at a constant Fermi level when the thickness of α-MoO3 is tuned. Furthermore, we also experimentally verify the hybrid polaritons in the graphene/α-MoO3 heterostructure with different thicknesses of α-MoO3. The interface engineering offers new insights into optical topological transitions, which may shed new light on programmable polaritonics, energy transfer, and neuromorphic photonics.

Nonlinear microscopy of lead iodide nanosheets.

Lead iodide (PbI2) is a van der Waals layered semiconductor with a direct bandgap in its bulk form and a hexagonal layered crystalline structure. The recently developed PbI2 nanosheets have shown great promise for high-performance optoelectronic devices, including nanolasers and photodetectors. However, despite being widely used as a precursor for perovskite materials, the optical properties of PbI2 nanomaterials remain largely unexplored. Here, we determine the nonlinear optical properties of PbI2 nanosheets by utilising nonlinear microscopy as a non-invasive optical technique. We demonstrate the nonlinearity enhancement dependent on excitonic resonances, crystalline orientation, thickness, and influence of the substrate. Our results allow for estimating the second- and third-order nonlinear susceptibilities of the nanosheets, opening new opportunities for the use of PbI2 nanosheets as nonlinear and quantum light sources.

Tunable Cherenkov radiation based on a van der Waals semiconductor α-MoO3 and graphene hybrid.

In this Letter, we explore the Cherenkov radiation properties of α-phase molybdenum trioxide (α-MoO3). We demonstrate that the asymmetric, forward, and reverse Cherenkov radiation can simultaneously exist by rotating the α-MoO3 slab at the same working frequency and structure. In addition, thanks to the tunable functionalities of graphene, the conversion of forward and reverse Cherenkov radiation can be actualized by altering the Fermi level of graphene. These dynamically adjustable features provide a novel, to the best of our knowledge, and intuitive way for tunable Cherenkov radiation in the mid-infrared range, which opens up new opportunities in designing and manufacturing tunable radiation sources in future.

Artificial Metaphotonics Born Naturally in Two Dimensions.

Recently, two rich and exciting research fields, layered two-dimensional (2D) materials and metamaterials, have started overlapping. Metamaterials are artificial, engineered materials with broad metaphotonic prospects such as negative refraction, perfect lensing, subwavelength imaging, and cloaking. The possibility of achieving metaphotonic properties using metamaterials based on layered 2D materials has been extensively exploited. Because they are highly tunable and adjustable with the ease of micro- and nanofabrication, 2D materials exhibit diverse optical properties such as natural negative refraction, natural anisotropic behavior, and even hyperbolic dispersion. A combination of 2D materials with conventional metamaterials promises a variety of prospective applications. In this review, we illustrate how the concept of metamaterials and their associated metaphotonic capabilities are naturally born in 2D materials. The multifunctionality of 2D materials may enable the manufacture of novel optical devices that work in a broad frequency range, from visible to terahertz, with particularly low loss, high speed, gated tunability, and miniaturized sizes. This new area of research links the fields of photonics, optoelectronics, and plasmonics with that of metamaterials and may provide insights to future innovations for 2D-material-inspired metaphotonic devices.

Hybridized Hyperbolic Surface Phonon Polaritons at α-MoO3 and Polar Dielectric Interfaces.

Surface phonon polaritons (SPhPs) in polar dielectrics offer new opportunities for infrared nanophotonics. However, bulk SPhPs inherently propagate isotropically with limited photon confinement, and how to collectively realize ultralarge confinement, in-plane hyperbolicity, and unidirectional propagation remains elusive. Here, we report an approach to solve the aforementioned issues of bulk SPhPs in one go by constructing a heterostructural interface between biaxial van der Waals material (e.g., α-MoO3) and bulk polar dielectric (e.g., SiC, AlN, and GaN). Because of anisotropy-oriented mode couplings, the hybridized SPhPs with a large confinement factor (>100) show in-plane hyperbolicity that has been switched to the orthogonal direction as compared to that in natural α-MoO3. More interestingly, this proof of concept allows steerable and unidirectional polariton excitation by suspending α-MoO3 on patterned SiC air cavities. Our finding exemplifies a generalizable framework to manipulate the flow of nanolight in many other hybrid systems consisting of anisotropic materials and polar dielectrics.

Broad spectral tuning of ultra-low-loss polaritons in a van der Waals crystal by intercalation.

Phonon polaritons-light coupled to lattice vibrations-in polar van der Waals crystals are promising candidates for controlling the flow of energy on the nanoscale due to their strong field confinement, anisotropic propagation and ultra-long lifetime in the picosecond range1-5. However, the lack of tunability of their narrow and material-specific spectral range-the Reststrahlen band-severely limits their technological implementation. Here, we demonstrate that intercalation of Na atoms in the van der Waals semiconductor α-V2O5 enables a broad spectral shift of Reststrahlen bands, and that the phonon polaritons excited show ultra-low losses (lifetime of 4 ± 1 ps), similar to phonon polaritons in a non-intercalated crystal (lifetime of 6 ± 1 ps). We expect our intercalation method to be applicable to other van der Waals crystals, opening the door for the use of phonon polaritons in broad spectral bands in the mid-infrared domain.

Ideal type-II Weyl points in twisted one-dimensional dielectric photonic crystals.

We proposed an one-dimensional layer-stacked photonic crystal using anisotropic materials to realize ideal type-II Weyl points. The topological transition from Dirac to Weyl points can be clearly observed by tuning the twist angle between layers. Also, on the interface between the photonic type-II Weyl material and air, gapless surface states have been demonstrated in an incomplete bulk bandgap. By breaking parameter symmetry, these ideal type-II Weyl points would transform into the non-ideal ones, exhibiting topological surface states with single group velocity. Our work may provide a new idea for the realization of photonic semimetal phases by utilizing naturally anisotropic materials.

A graphene-Mo2C heterostructure for a highly responsive broadband photodetector.

Photodetectors based on intrinsic graphene can operate over a broad wavelength range with ultrafast response, but their responsivity is much lower than commercial silicon photodiodes. The combination of graphene with two-dimensional (2D) semiconductors may enhance the light absorption, but there is still a cutoff wavelength originating from the bandgap of semiconductors. Here, we report a highly responsive broadband photodetector based on the heterostructure of graphene and transition metal carbides (TMCs, more specifically Mo2C). The graphene-Mo2C heterostructure enhanced light absorption over a broad wavelength range from ultraviolet to infrared. In addition, there is very small resistance for photoexcited carriers in both graphene and Mo2C. Consequently, photodetectors based on the graphene-Mo2C heterostructure deliver a very high responsivity from visible to infrared telecommunication wavelengths.

Atomically Thin Noble Metal Dichalcogenides for Phase-Regulated Meta-optics.

Owing to its good air stability and high refractive index, two-dimensional (2D) noble metal dichalcogenide shows intriguing potential for versatile flat optics applications. However, light field manipulation at the atomic scale is conventionally considered unattainable because the small thickness and intrinsic losses of 2D materials completely suppress both resonances and phase accumulation effects. Here, we demonstrate that losses of structured atomically thick PtSe2 films integrated on top of a uniform substrate can be utilized to create the spots of critical coupling, enabling singular phase behaviors with a remarkable π phase jump. This finding enables the experimental demonstration of atomically thick binary meta-optics that allows an angle-robust and high unit thickness diffraction efficiency of 0.96%/nm in visible frequencies (given its thickness of merely 4.3 nm). Our results unlock the potential of a new class of 2D flat optics for light field manipulation at an atomic thickness.

Infrared Polaritonic Biosensors Based on Two-Dimensional Materials.

In recent years, polaritons in two-dimensional (2D) materials have gained intensive research interests and significant progress due to their extraordinary properties of light-confinement, tunable carrier concentrations by gating and low loss absorption that leads to long polariton lifetimes. With additional advantages of biocompatibility, label-free, chemical identification of biomolecules through their vibrational fingerprints, graphene and related 2D materials can be adapted as excellent platforms for future polaritonic biosensor applications. Extreme spatial light confinement in 2D materials based polaritons supports atto-molar concentration or single molecule detection. In this article, we will review the state-of-the-art infrared polaritonic-based biosensors. We first discuss the concept of polaritons, then the biosensing properties of polaritons on various 2D materials, then lastly the impending applications and future opportunities of infrared polaritonic biosensors for medical and healthcare applications.

High Efficiency Mesoscopic Solar Cells Using CsPbI3 Perovskite Quantum Dots Enabled by Chemical Interface Engineering.

All-inorganic α-CsPbI3 perovskite quantum dots (QDs) are attracting great interest as solar cell absorbers due to their appealing light harvesting properties and enhanced stability due to the absence of volatile organic constituents. Moreover, ex situ synthesized QDs significantly reduce the variability of the perovskite layer deposition process. However, the incorporation of α-CsPbI3 QDs into mesoporous TiO2 (m-TiO2) is highly challenging, but these constitute the best performing electron transport materials in state-of-the-art perovskite solar cells. Herein, the m-TiO2 surface is engineered using an electron-rich cesium-ion containing methyl acetate solution. As one effect of this treatment, the solid-liquid interfacial tension at the TiO2 surface is reduced and the wettability is improved, facilitating the migration of the QDs into m-TiO2. As a second effect, Cs+ ions passivate the QD surface and promote the charge transfer at the m-TiO2/QD interface, leading to an enhancement of the electron injection rate by a factor of 3. In combination with an ethanol-environment smoothing route that significantly reduces the surface roughness of the m-TiO2/QD layer, optimized devices exhibit highly reproducible power conversion efficiencies exceeding 13%. The best cell with an efficiency of 14.32% (reverse scan) reaches a short-circuit current density of 17.77 mA cm-2, which is an outstanding value for QD-based perovskite solar cells.

High Performance Lithium-Ion Batteries Using Layered 2H-MoTe2 as Anode.

The major challenges faced by candidate electrode materials in lithium-ion batteries (LIBs) include their low electronic and ionic conductivities. 2D van der Waals materials with good electronic conductivity and weak interlayer interaction have been intensively studied in the electrochemical processes involving ion migrations. In particular, molybdenum ditelluride (MoTe2 ) has emerged as a new material for energy storage applications. Though 2H-MoTe2 with hexagonal semiconducting phase is expected to facilitate more efficient ion insertion/deinsertion than the monoclinic semi-metallic phase, its application as an anode in LIB has been elusive. Here, 2H-MoTe2 , prepared by a solid-state synthesis route, has been employed as an efficient anode with remarkable Li+ storage capacity. The as-prepared 2H-MoTe2 electrodes exhibit an initial specific capacity of 432 mAh g-1 and retain a high reversible specific capacity of 291 mAh g-1 after 260 cycles at 1.0 A g-1 . Further, a full-cell prototype is demonstrated by using 2H-MoTe2 anode with lithium cobalt oxide cathode, showing a high energy density of 454 Wh kg-1 (based on the MoTe2 mass) and capacity retention of 80% over 100 cycles. Synchrotron-based in situ X-ray absorption near-edge structures have revealed the unique lithium reaction pathway and storage mechanism, which is supported by density functional theory based calculations.

Synthesis and optical applications of low dimensional metal-halide perovskites.

Metal halide perovskites have received substantial attention in research communities due to their outstanding efficiency achievements in the field of photovoltaics, optoelectronics and electronics, exhibiting extraordinary optical, electrical and mechanical properties. The exceptional structural tunability enables perovskite material to possess low-dimensional form at the atomic level and extends their applications into optoelectronic and photonic fields. This review discusses the recent progress of synthetic routes and fundamental optoelectronic properties of low-dimensional metal halide perovskites. In addition, the focus is to highlight the potential applications of perovskites in various devices including solar cells, light-emitting diodes, lasers, waveguides and memory devices. Finally, outlooks and the challenges that face the development of the perovskite materials in the near future are also presented.

Lattice -Mismatch-Induced Ultrastable 1T-Phase MoS2-Pd/Au for Plasmon-Enhanced Hydrogen Evolution.

Metallic 1T-phase transition metal dichalcogenides (TMDs) are of considerable interest in enhancing catalytic applications due to their abundant active sites and good conductivity. However, the unstable nature of 1T-phase TMDs greatly impedes their practical applications. Herein, we developed a new approach for the synthesis of highly stable 1T-phase Au/Pd-MoS2 nanosheets (NSs) through a metal assembly induced ultrastable phase transition for achieving a very high electrocatalytic activity in the hydrogen evolution reaction. The phase transition was evoked by a novel mechanism of lattice-mismatch-induced strain based on density functional theory (DFT) calculations. Raman spectroscopy and transmission electron microscopy (TEM) were used to confirm the phase transition on experimental grounds. A novel heterostructured 1T MoS2-Au/Pd catalyst was designed and synthesized using this mechanism, and the catalyst exhibited a 0 mV onset potential in the hydrogen evolution reaction under light illumination. Therefore, this method can potentially be used to fabricate 1T-phase TMDs with remarkably enhanced activities for different applications.

High-Yield Electrochemical Production of Large-Sized and Thinly Layered NiPS3 Flakes for Overall Water Splitting.

Achieving large-sized and thinly layered 2D metal phosphorus trichalcogenides with high quality and yield has been an urgent quest due to extraordinary physical/chemical characteristics for multiple applications. Nevertheless, current preparation methodologies suffer from uncontrolled thicknesses, uneven morphologies and area distributions, long processing times, and inferior quality. Here, a sonication-free and fast (in minutes) electrochemical cathodic exfoliation approach is reported that can prepare large-sized (typically ≈150 µm2 ) and thinly layered (≈70% monolayer) NiPS3 flakes with high crystallinity and pure phase structure with a yield ≈80%. During the electrochemical exfoliation process, the tetra-n-butylammonium salt with a large ionic diameter is decomposed into gaseous species after the intercalation and efficiently expands the tightly stratified bulk NiPS3 crystals, as revealed by in situ and ex situ characterizations. Atomically thin NiPS3 flakes can be obtained by slight manual shaking rather than sonication, which largely preserves in-plane structural integrity with large size and minimum damage. The obtained high quality NiPS3 offers a new and ideal model for overall water splitting due to its inherent fully exposed S and P atoms that are often the active sites for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Consequently, the bifunctional NiPS3 exhibits outstanding performance for overall water splitting.

Ultra-Broadband Flexible Photodetector Based on Topological Crystalline Insulator SnTe with High Responsivity.

Topological crystalline insulators (TCIs) are predicted to be a promising candidate material for ultra-broadband photodetectors ranging from ultraviolet (UV) to terahertz (THz) due to its gapless surface state and narrow bulk bandgap. However, the low responsivity of TCIs-based photodetectors limits their further applications. In this regard, a high-performance photodetector based on SnTe, a recently developed TCI, working in a broadband wavelength range from deep UV to mid-IR with high responsivity is reported. By taking advantage of the strong light absorption and small bandgap of SnTe, photodetectors based on the as-grown SnTe crystalline nanoflakes as well as specific short channel length achieve a high responsivity (71.11 A W-1 at 254 nm, 49.03 A W-1 at 635 nm, 10.91 A W-1 at 1550 nm, and 4.17 A W-1 at 4650 nm) and an ultra-broad spectral response (254-4650 nm) simultaneously. Moreover, for the first time, a durable flexible SnTe photodetector fabricated directly on a polyethylene terephthalate film is demonstrated. These results prove the great potential of TCIs as a promising material for integrated and flexible optoelectronic devices.