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Highly confined and low-loss polaritons are known to propagate isotropically over graphene and hexagonal boron nitride in the plane, leaving limited degrees of freedom in manipulating light at the nanoscale. The emerging family of biaxial van der Waals materials, such as α-MoO 3 and V 2 O 5 , support exotic polariton propagation, as their auxiliary optical axis is in the plane. Here, exploiting this strong in-plane anisotropy, we report edge-tailored hyperbolic polaritons in patterned α-MoO 3 nanocavities via real-space nanoimaging. We find that the angle between the edge orientation and the crystallographic direction significantly affects the optical response, and can serve as a key tuning parameter in tailoring the polaritonic patterns. By shaping α-MoO 3 nanocavities with different geometries, we observe edge-oriented and steerable hyperbolic polaritons as well as forbidden zones where the polaritons detour. The lifetime and figure of merit of the hyperbolic polaritons can be regulated by the edge aspect ratio of nanocavity. The possibility to manipulate the propagation of polaritons is limited by the isotropy of 2D materials like graphene and hexagonal boron nitride. Here, the authors exploit the anisotropy of α-MoO 3 and study edge tailored hyperbolic polariton manipulation in α-MoO 3 nanocavities via real space nanoimaging.

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 range 1 – 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-V 2 O 5 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. The spectral range of long-lived and confined phonon polaritons in a polar van der Waals crystal is shown to be tunable by intercalation of Na atoms, expanding their potential for nanophotonic applications in the mid-infrared domain.

Chemically derived graphene oxide (GO) has recently moved on from simply being a graphene precursor to attracting interest for its own properties. This Review discusses how the presence of oxygenated groups and domains of sp 2 - and sp 3 -hybridized carbons makes GO tunable and promising for various physical and biological applications. Chemically derived graphene oxide (GO) is an atomically thin sheet of graphite that has traditionally served as a precursor for graphene, but is increasingly attracting chemists for its own characteristics. It is covalently decorated with oxygen-containing functional groups — either on the basal plane or at the edges — so that it contains a mixture of sp 2 - and sp 3 -hybridized carbon atoms. In particular, manipulation of the size, shape and relative fraction of the sp 2 -hybridized domains of GO by reduction chemistry provides opportunities for tailoring its optoelectronic properties. For example, as-synthesized GO is insulating but controlled deoxidation leads to an electrically and optically active material that is transparent and conducting. Furthermore, in contrast to pure graphene, GO is fluorescent over a broad range of wavelengths, owing to its heterogeneous electronic structure. In this Review, we highlight the recent advances in optical properties of chemically derived GO, as well as new physical and biological applications.

MicroRNA exhibits differential expression levels in cancer and can affect cellular transformation, carcinogenesis and metastasis. Although fluorescence techniques using dye molecule labels have been studied, label-free molecular-level quantification of miRNA is extremely challenging. We developed a surface plasmon resonance sensor based on two-dimensional nanomaterial of antimonene for the specific label-free detection of clinically relevant biomarkers such as miRNA-21 and miRNA-155. First-principles energetic calculations reveal that antimonene has substantially stronger interaction with ssDNA than the graphene that has been previously used in DNA molecule sensing, due to thanking for more delocalized 5 s /5 p orbitals in antimonene. The detection limit can reach 10 aM, which is 2.3–10,000 times higher than those of existing miRNA sensors. The combination of not-attempted-before exotic sensing material and SPR architecture represents an approach to unlocking the ultrasensitive detection of miRNA and DNA and provides a promising avenue for the early diagnosis, staging, and monitoring of cancer. Label-free molecular-level quantification of MicroRNA (miRNA) remains challenging. Here, the authors develop a new surface plasmon resonance sensor based on two-dimensional nanomaterial of antimonene for the specific label-free detection of clinically relevant biomarkers such as miRNA-21 and miRNA-155.

Phonon polaritons (PhPs) have attracted significant interest in the nano-optics communities because of their nanoscale confinement and long lifetimes. Although PhP modification by changing the local dielectric environment has been reported, controlled manipulation of PhPs by direct modification of the polaritonic material itself has remained elusive. Here, chemical switching of PhPs in α-MoO 3 is achieved by engineering the α-MoO 3 crystal through hydrogen intercalation. The intercalation process is non-volatile and recoverable, allowing reversible switching of PhPs while maintaining the long lifetimes. Precise control of the intercalation parameters enables analysis of the intermediate states, in which the needle-like hydrogenated nanostructures functioning as in-plane antennas effectively reflect and launch PhPs and form well-aligned cavities. We further achieve spatially controlled switching of PhPs in selective regions, leading to in-plane heterostructures with various geometries. The intercalation strategy introduced here opens a relatively non-destructive avenue connecting infrared nanophotonics, reconfigurable flat metasurfaces and van der Waals crystals. Phonon polaritons hold promises for nanophotonic applications but external control of phonon polaritons remains challenging. Here, the authors achieve reversible and non-volatile switching of phonon polariton by modifying crystal structure and lattice vibrations via hydrogenation.

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 forces 1 , 2 (vdW materials). These polaritons can be tuned by electric fields 3 , 4 or by material thickness 5 , leading to applications including nanolasers 6 , tunable infrared and terahertz detectors 7 , and molecular sensors 8 . Polaritons with anisotropic propagation along the surface of vdW materials have been predicted, caused by in-plane anisotropic structural and electronic properties 9 . In such materials, elliptic and hyperbolic in-plane polariton dispersion can be expected (for example, plasmon polaritons in black phosphorus 9 ), 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-MoO 3 , a natural vdW material. By infrared nano-imaging and nano-spectroscopy of semiconducting α-MoO 3 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 polaritons 3 – 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 temperature 10 . They are also a factor of about four larger than the best values so far reported for phonon polaritons in isotopically engineered boron nitride 11 and for graphene plasmon polaritons at low temperatures 12 . 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. Observation of the anisotropic propagation of polaritons along the surface of layered, semiconducting α-MoO 3 confirms the existence of this phenomenon in natural materials.

The challenge of science and technology is to design and make materials that will dominate the future of our society. In this context, black phosphorus has emerged as a new, intriguing two‐dimensional (2D) material, together with its monolayer, which is referred to as phosphorene. The exploration of this new 2D material demands various fabrication methods to achieve potential applications— this demand motivated this review. This article is aimed at supplementing the concrete understanding of existing phosphorene fabrication techniques, which forms the foundation for a variety of applications. Here, the major issue of the degradation encountered in realizing devices based on few‐layered black phosphorus and phosphorene is reviewed. The prospects of phosphorene in future research are also described by discussing its significance and explaining ways to advance state‐of‐art of phosphorene‐based devices. In addition, a detailed presentation on the demand for future studies to promote well‐systemized fabrication methods towards large‐area, high‐yield and perfectly protected phosphorene for the development of reliable devices in optoelectronic applications and other areas is offered. The degradation encountered in realizing few‐layered black phosphorus and phosphorene devices is reviewed. In particular, a detailed presentation of the demand for future studies to promote well‐systemized fabrication methods towards large‐area, high‐yield and perfectly protected phosphorene for the development of reliable devices in optoelectronic applications and other areas is offered.

Moiré superlattices (MSLs) are modulated structures produced from homogeneous or heterogeneous 2D layers stacked with a twist angle and/or lattice mismatch. Expanding the range of available materials, methods for fabricating MSL, and realization of unique emergent properties are key challenges. Here we report a facile bottom-up synthesis of homogeneous MSL based on a wide-gap 2D semiconductor, BiOCl, using a one-pot solvothermal approach with robust reproducibility. Unlike previous MSLs usually prepared by directly stacking two monolayers, our BiOCl MSLs are realized in a scalable, direct way through chemical growth of spiral-type nanosheets driven by screw-dislocations. We find emergent properties including large band gap reduction (∼0.6 eV), two-fold increase in carrier lifetime, and strongly enhanced photocatalytic activity. First-principles calculations reveal that such unusual properties can be ascribed to the locally enhanced inter-layer coupling associated with the Moiré potential modulation. Our results demonstrate the promise of MSL materials for chemical and physical functions. Expanding the range of available materials, methods for fabricating Moiré superlattices, and realization of new emergent properties are key challenges. Here the authors report a facile bottom-up synthesis of homogeneous Moiré superlattices based on a wide-gap 2D semiconductor, bismuth oxychloride.

In emerging optoelectronic applications, such as water photolysis, exciton fission and novel photovoltaics involving low-dimensional nanomaterials, hot-carrier relaxation and extraction mechanisms play an indispensable and intriguing role in their photo-electron conversion processes. Two-dimensional transition metal dichalcogenides have attracted much attention in above fields recently; however, insight into the relaxation mechanism of hot electron-hole pairs in the band nesting region denoted as C-excitons, remains elusive. Using MoS 2 monolayers as a model two-dimensional transition metal dichalcogenide system, here we report a slower hot-carrier cooling for C-excitons, in comparison with band-edge excitons. We deduce that this effect arises from the favourable band alignment and transient excited-state Coulomb environment, rather than solely on quantum confinement in two-dimension systems. We identify the screening-sensitive bandgap renormalization for MoS 2 monolayer/graphene heterostructures, and confirm the initial hot-carrier extraction for the C-exciton state with an unprecedented efficiency of 80%, accompanied by a twofold reduction in the exciton binding energy. Light-matter interaction in atomically thin transition metal dichalcogenides is dominated by excitonic effects and hot-carrier relaxation/extraction mechanisms. Here, the authors report that the C exciton in two-dimensional MoS 2 exhibits a slower hot-carrier cooling than band-edge excitons.

A variety of deposition methods for two-dimensional crystals have been demonstrated; however, their wafer-scale deposition remains a challenge. Here we introduce a technique for depositing and patterning of wafer-scale two-dimensional metal chalcogenide compounds by transforming the native interfacial metal oxide layer of low melting point metal precursors (group III and IV) in liquid form. In an oxygen-containing atmosphere, these metals establish an atomically thin oxide layer in a self-limiting reaction. The layer increases the wettability of the liquid metal placed on oxygen-terminated substrates, leaving the thin oxide layer behind. In the case of liquid gallium, the oxide skin attaches exclusively to a substrate and is then sulfurized via a relatively low temperature process. By controlling the surface chemistry of the substrate, we produce large area two-dimensional semiconducting GaS of unit cell thickness (∼1.5 nm). The presented deposition and patterning method offers great commercial potential for wafer-scale processes. One of the key challenges 2D materials still face is their uniform wafer-scale deposition. Here, the authors present a deposition method for post-transition metal dichalcogenides, based on transformation of an ultra-thin oxide layer on the surface of liquid elemental gallium onto an oxide-coated substrate.