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Two-dimensional (2D) transition metal dichalcogenides (TMDs) hold great potential for future low-energy optoelectronics owing to their unique electronic, optical, and mechanical properties. Chemical vapor deposition (CVD) is the technique widely used for the synthesis of large-area TMDs. However, due to high sensitivity to the growth environment, reliable synthesis of monolayer TMDs via CVD remains challenging. Here we develop a controllable CVD process for large-area synthesis of monolayer WS2 crystals, films, and in-plane graphene-WS2 heterostructures by cleaning the reaction tube with hydrochloric acid, sulfuric acid and aqua regia. The concise cleaning process can remove the residual contaminates attached to the CVD reaction tube and crucibles, reducing the nucleation density but enhancing the diffusion length of WS2 species. The photoluminescence (PL) mappings of a WS2 single crystal and film reveal that the extraordinary PL around the edges of a triangular single crystal is induced by ambient water intercalation at the WS2-sapphire interface. The extraordinary PL can be controlled by the choice of substrates with different wettabilities.

Perhaps the most significant progress to the field of infrared optics and nanophotonics has been made through the real space realisation of polaritons in two-dimensional materials that provide maximum light confinement functionalities. The recent breakthrough discovery of in-plane hyperbolicity in the natural van der Waals material has revealed a most exciting optical property which enable an in-plane anisotropic dispersion. Yet, the most intriguing feature of in-plane anisotropic dispersion is the manipulation of polaritons at the nano scale. This development has opened a new window of opportunity in order to develop unique nanophotonic devices with unprecedented controls. This chapter will cover these developments with focus on fundamental understandings and progress of real space visualisation of in-plane anisotropic polaritons in the near-field range. The last section will conclude with the future prospects of this rapidly emerging area.

Negative reflection occurs when light is reflected towards the same side of the normal to the boundary from which it is incident. This exotic optical phenomenon, which provides a new avenue towards light manipulation, is not only yet to be visualized in real space but remains largely unexplored both at the nanoscale and in natural media. Here, we directly visualize nanoscale-confined polaritons negatively reflecting on subwavelength mirrors fabricated in a low-loss van der Waals crystal. Our near-field nanoimaging results unveil an unconventional and broad tunability of both the polaritonic wavelength and direction of propagation upon negative reflection. Based on these findings, we introduce a novel device in nano-optics: a hyperbolic nanoresonator, in which hyperbolic polaritons with different momenta reflect back to a common point source, enhancing its intensity. These results pave the way to realize nanophotonics in low-loss natural media, providing a novel and efficient route to confine and control the flow of light at the nanoscale, key for future optical on-chip nanotechnologies.

Polaritons in polar biaxial crystals with extreme anisotropy offer a promising route to manipulate nanoscale light-matter interactions. The dynamical modulation of their dispersion is great significance for future integrated nano-optics but remains challenging. Here, we report a momentum-directed strategy, a coupling between the modes with extra momentum supported by the interface and in-plane hyperbolic polaritons, to tailor topological transitions of anisotropic polaritons in biaxial crystals. We experimentally demonstrate such tailored polaritons at the interface of heterostructures between graphene and {\alpha}-phase molybdenum trioxide ({\alpha}-MoO3). The interlayer coupling can be electrically modulated by changing the Fermi level in graphene, enabling a dynamic topological transition. More interestingly, we found that the topological transition occurs at a constant Fermi level when tuning the thickness of {\alpha}-MoO3. The momentum-directed strategy implemented by interface engineering offers new insights for optical topological transitions, which may shed new light for programmable polaritonics, energy transfer and neuromorphic photonics.

Weyl points are the degenerate points in three-dimensional momentum space with nontrivial topological phase, which are usually realized in classical system with structure and symmetry designs. Here we proposed a one-dimensional layer-stacked photonic crystal using anisotropic materials to realize ideal type-II Weyl points without structure designs. The topological transition from two Dirac points to four Weyl points can be clearly observed by tuning the twist angle between layers. Besides, on the interface between the photonic type-II Weyl material and air, gappless surface states have also been demonstrated in an incomplete bulk bandgap. By breaking parameter symmetry, these ideal type-II Weyl points at the same frequency would transform into the non-ideal ones, and exhibit topological surface states with single group velocity. Our work may provide a new idea for the realization of photonic Weyl points or other semimetal phases by utilizing naturally anisotropic materials., Comment: 9pages; 4 figures

Phonon polaritons (PhPs),light coupled to lattice vibrations,with in-plane hyperbolic dispersion exhibit ray-like propagation with large wavevectors and enhanced density of optical states along certain directions on a surface. As such, they have raised a surge of interest as they promise unprecedented possibilities for the manipulation of infrared light with planar circuitry and at the nanoscale. Here, we demonstrate, for the first time, the focusing of in-plane hyperbolic PhPs propagating along thin slabs of MoO3. To that end, we developed metallic nanoantennas of convex geometries for both the efficient launching and focusing of the polaritons. Remarkably, the foci obtained exhibit enhanced near-field confinement and absorption compared to foci produced by in-plane isotropic PhPs. More intriguingly, foci sizes as small as lamdap/5 =lamda0/50 were achieved (lamdap is the polariton wavelength and lamda0 the photon wavelength). Focusing of in-plane hyperbolic polaritons introduces a first and most basic building block developing planar polariton optics utilizing in-plane anisotropic van der Waals materials and metasurfaces.

Surface phonon polaritons (SPhPs) in polar dielectrics offer new opportunities for infrared nanophotonics due to sub-diffraction confinement with low optical losses. Though the polaritonic field confinement can be significantly improved by modifying the dielectric environment, it is challenging to break the fundamental limits in photon confinement and propagation behavior of SPhP modes. In particular, as SPhPs inherently propagate isotropically in these bulk polar dielectrics, how to collectively realize ultra-large field confinement, in-plane hyperbolicity and unidirectional propagation remains elusive. Here, we report an approach to solve the aforementioned issues of bulk polar dielectric's SPhPs at one go by constructing a heterostructural interface between biaxial van der Waals material (e.g., MoO3) and bulk polar dielectric (e.g., SiC, AlN, and GaN). Due to anisotropy-oriented mode couplings at the interface, 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 MoO3. More interestingly, this proof of concept allows steerable, angle-dependent and unidirectional polariton excitation by suspending MoO3 on patterned SiC air cavities. Our finding exemplifies a generalizable framework to manipulate the flow of nano-light and engineer unusual polaritonic responses in many other hybrid systems consisting of van der Waals materials and bulk polar dielectrics.

Atomically thin transition metal dichalcogenide crystals (TMDCs) have extraordinary optical properties that make them attractive for future optoelectronic applications. Integration of TMDCs into practical all-dielectric heterostructures hinges on the ability to passivate and protect them against necessary fabrication steps on large scales. Despite its limited scalability, encapsulation of TMDCs in hexagonal boron nitride (hBN) currently has no viable alternative for achieving high performance of the final device. Here, we show that the novel, ultrathin Ga$_2$O$_3$ glass is an ideal centimeter-scale coating material that enhances optical performance of the monolayers and protects them against further material deposition. In particular, Ga$_2$O$_3$ capping of commercial grade WS$_2$ monolayers outperforms hBN in both scalability and optical performance at room temperature. These properties make Ga$_2$O$_3$ highly suitable for large scale passivation and protection of monolayer TMDCs in functional heterostructures.

Twisted two-dimensional bi-layers offer exquisite control on the electronic bandstructure through the interlayer rotation and coupling, enabling magic-angle flat-band superconductivity and moir\'e excitons. Here, we demonstrate how analogous principles, combined with large anisotropy, enable extreme control and manipulation of the photonic dispersion of phonon polaritons (PhPs) in van der Waals (vdW) bi-layers. We experimentally observe tunable topological transitions from open (hyperbolic) to closed (elliptic) dispersion contours in twisted bi-layered {\alpha}-MoO3 at photonic magic angles, induced by polariton hybridization and robustly controlled by a topological quantity. At these transitions the bilayer dispersion flattens, exhibiting low-loss tunable polariton canalization and diffractionless propagation with resolution below {\lambda}0/40. Our findings extend twistronics and moir\'e physics to nanophotonics and polaritonics, with great potential for nano-imaging, nanoscale light propagation, energy transfer and quantum applications., Comment: Nature, in press

In this paper, we report two new kinds of absolute optical instruments that can make stigmatically images for geometric optics in two dimensional space. One is called the duplex Mikaelian lens, which is made by splicing two half Mikaelian lenses with different periods. The other is exponential conformal transformer of duplex Mikaelian lens with the ratio of different periods of its two half Mikaelian lenses a rational number, which we call duplex Maxwell's fish eye lens. Duplex Mikaelian lenses have continuous translation symmetry with arbitrary real number, while duplex Maxwell's fish eye lenses have continuous rotational symmetry from 0 to 2*Pi. Hence each duplex Maxwell's fish eye lens corresponds to a duplex Mikaelian lens. We further demonstrate the caustic effect of geometric optics in duplex Mikaelian lenses and duplex Maxwell's fish eye lenses. In addition, we investigate the Talbot effect of wave optics in the duplex Mikaelian lens based on numeric calculations. Our findings based on splicing and exponential conformal mapping enlarge the family of absolute optical instruments., Comment: 14 pages, 5 figures; This is an application of geometric optics when I was preparing the course of University Physics; Senlin Liu, Yuze Wu, Yi Yang, and Zichun Zhou are undergraduate students in Xiamen University Malaysia

We design a new absolute optical instrument by composing Luneburg lens and Lissajous lens, and analyze its imaging mechanism from the perspective of simple harmonic oscillations. The imaging positions are determined by the periods of motions in x and y directions. Besides, instruments composed with multi parts are also devised, which can form imaging or self-imaging as long as the motion periods of x and y directions are satisfied to similar conditions. Our work provides a new way to analyze the imaging of different lens by simply dissociating the equations of motions, and reveal the internal mechanism of some absolute optical instruments., Comment: 4 pages, 4 figures; This is an application of simple harmonic oscillations when I am preparing the course of University Physics; Huashuo Han, Pinchao He, Keqin Xia, and Jiaxiang Zhang are undergraduate students in Xiamen University Malaysia

Two-dimensional (2D) noble-metal dichalcogenides have emerged as a new platform for the realization of versatile flat optics with a considerable degree of miniaturization. However, light field manipulation at the atomic scale is widely considered unattainable since the vanishing thickness and intrinsic losses of 2D materials completely suppress both resonances and phase accumulation effects. Empowered by conventionally perceived adverse effects of intrinsic losses, we show that the structured PtSe2 films integrated with a uniform substrate can regulate nontrivial singular phase and realize atomic-thick meta-optics in the presence of topological darkness. We experimentally demonstrate a series of atomic-thick binary meta-optics that allows 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.

The biaxial van der Waals semiconductor $\alpha$-phase molybdenum trioxide ($\alpha$-MoO$_3$) has recently received significant attention due to its ability to support highly anisotropic phonon polaritons (PhPs) -infrared (IR) light coupled to lattice vibrations in polar materials-, offering an unprecedented platform for controlling the flow of energy at the nanoscale. However, to fully exploit the extraordinary IR response of this material, an accurate dielectric function is required. Here, we report the accurate IR dielectric function of $\alpha$-MoO$_3$ by modelling far-field, polarized IR reflectance spectra acquired on a single thick flake of this material. Unique to our work, the far-field model is refined by contrasting the experimental dispersion and damping of PhPs, revealed by polariton interferometry using scattering-type scanning near-field optical microscopy (s-SNOM) on thin flakes of $\alpha$-MoO$_3$, with analytical and transfer-matrix calculations, as well as full-wave simulations. Through these correlative efforts, exceptional quantitative agreement is attained to both far- and near-field properties for multiple flakes, thus providing strong verification of the accuracy of our model, while offering a novel approach to extracting dielectric functions of nanomaterials, usually too small or inhomogeneous for establishing accurate models only from standard far-field methods. In addition, by employing density functional theory (DFT), we provide insights into the various vibrational states dictating our dielectric function model and the intriguing optical properties of $\alpha$-MoO$_3$.

Current micro nanomechanical system are usually based on rigid crystalline semiconductors that normally have high quality factors but lack adaptive responses to variable frequencies, a capability ubiquitous for communications in the biological world, such as bat and whale calls. Here, we demonstrate a soft mechanical resonator based on a freestanding organic-inorganic hybrid plasmonic superlattice nanosheet, which can respond adaptively to either incident light intensity or wavelength. This is achieved because of strong plasmonic coupling in closely-packed nanocrystals which can efficiently concentrate and convert photons into heat. The heat causes the polymer matrix to expand, leading to a change in the nanomechanical properties of the plasmonic nanosheet. Notably, the adaptive frequency responses are also reversible and the responsive ranges are fine-tunable by adjusting the constituent nanocrystal building blocks. We believe that our plasmonic nanosheets may open a new route to design next-generation intelligent bio-mimicking opto-mechanical resonance systems.

Recently, a new emerging field about heavily-doped colloidal plasmonic nanocrystals (NCs) has attracted great attention due to their lower and expediently adjustable free carrier densities, lower and tunable LSPR band in the spectral range from NIR to MIR and higher optical nonlinearity. These new kinds of plasmonic materials will show huge potential and opportunities for nonlinear optical applications, such as ultrafast switching, nonlinear sensing and pulse laser generation. In this work, we demonstrate that high-quality mode-locking and Q-switching pulses at 1560 nm can both be generated by using controllable concentration of Cu3-xP NCs solution and fabricating evanescently interacted saturable absorbers. Furthermore, the plasmonic NCs material has good reproduction for fabricating SA devices and promising potential for large-scale industrial production. Our results may attract great attention for further investigations of heavily-doped plasmonic NCs as next generation, cheap and solution-processed element for fascinating applications in optoelectronic devices., Comment: 16 pages, 4 Figures

The inherent susceptibility of low-dimensional materials to thermal fluctuations has long been expected to poses a major challenge to achieving intrinsic long-range ferromagnetic order in two-dimensional materials. The recent explosion of interest in atomically thin materials and their assembly into van der Waals heterostructures has renewed interest in two-dimensional ferromagnetism, which is interesting from a fundamental scientific point of view and also offers a missing ingredient necessary for the realization of spintronic functionality in van der Waals heterostructures. Recently several atomically thin materials have been shown to be robust ferromagnets. Such ferromagnetism is thought to be enabled by magneto crystalline anisotropy which suppresses thermal fluctuations. In this article, we review recent progress in two-dimensional ferromagnetism in detail and predict new possible two-dimensional ferromagnetic materials. We also discuss the prospects for applications of atomically thin ferromagnets in novel dissipationless electronics, spintronics, and other conventional magnetic technologies. Particularly atomically thin ferromagnets are promising to realize time reversal symmetry breaking in two-dimensional topological systems, providing a platform for electronic devices based on the quantum anomalous Hall Effect showing dissipationless transport. Our proposed directions will assist the scientific community to explore novel two-dimensional ferromagnetic families which can spawn new technologies and further improve the fundamental understanding of this fascinating area., Comment: To be appear in Applied Physics Reviews

A variety of fabrication methods for van der Waals heterostructures have been demonstrated; however, their wafer-scale deposition remains a challenge. Here we report few-layer van der Waals PtS2/PtSe2 heterojunction photodiodes fabricated on a 2" SiO2/Si substrate that is only limited by the size of work chamber of the growth equipment, offering throughputs necessary for practical applications. Theoretical simulation results show that the bandgap of PtS2 is shrunk to half of its original size in the PtS2/PtSe2 heterostructures, while PtSe2 exhibits a limited response to the coupling. Both PtSe2 and PtS2 layers in the coupled system are still semiconductors. Dynamic photovoltaic switching in the heterojunctions is observed at zero-volt state under laser illuminations of 532 to 2200 nm wavelengths. The PtS2/PtSe2 photodiodes show excellent characteristics in terms of a high photoresponsivity of 361 mAW-1, an external quantum efficiency (EQE) of 84%, and a fast response speed (66 ms). The wafer-scale production of 2D photodiodes in this work accelerates the possibility of 2D materials for practical applications in the next-generation energy-efficient electronics.

Hybrid organic-inorganic halide perovskites are low-cost solution-processable solar cell materials with photovoltaic properties that rival those of crystalline silicon. The perovskite films are typically sandwiched between thin layers of hole and electron transport materials, which efficiently extract photogenerated charges. This affords high-energy conversion efficiencies but results in significant performance and fabrication challenges. Herein we present a simple charge transport layer-free perovskite solar cell (PSC), comprising only a perovskite layer with two interdigitated gold back-contacts. Charge extraction is achieved via self-assembled molecular monolayers (SAMs) and their associated dipole fields at the metal/perovskite interface. Photovoltages of approximately 600 mV generated by SAM-modified PSCs are equivalent to the built-in potential generated by individual dipole layers. Efficient charge extraction results in photocurrents of up to 12.1 mA/cm2 under simulated sunlight, despite a large electrode spacing., Comment: 18 pages, 5 figures

We experimentally demonstrate ultrathin flat lenses with a thickness of 7 {\AA}, which corresponds to the fundamental physical limit of the thickness of the material, is fabricated in a large area, monolayer, CVD-prepared tungsten chalcogenides single crystals using the low-cost flexible laser writing method. The lenses apply the ultra-high refractive index to introduce abrupt amplitude modulation of the incident light to achieve three-dimensional (3D) focusing diffraction-limited resolution (0.5{\lambda}) and a focusing efficiency as high as 31%. An analytical physical model based diffraction theory is derived to simulate the focusing process, which shows excellent agreement with the experimental results.

Black phosphorus is a very promising material for telecommunication due to its direct bandgap and strong resonant absorption in near-infrared wavelength range. However, ultrafast nonlinear photonic applications relying on the ultrafast photo-carrier dynamics as well as optical nonlinearity in black phosphorus remain unexplored. In this work, we investigate nonlinear optical properties of solution exfoliated BP and demonstrate the usage of BP as a new saturable absorber for high energy pulse generation in fiber laser. In order to avoid the oxidization and degradation of BP, we encapsulated BP by polymer matrix which is optically transparent in the spectrum range of interest to form a composite. Two fabrication approaches were demonstrated to produce BP-polymer composite films which were further incorporated into fiber laser cavity as nonlinear media. BP shows very fast carrier dynamics and BP-polymer composite has a modulation depth of 10.6%. A highly stable Q-switched pulse generation was achieved and the single pulse energy of ~194 nJ was demonstrated. The ease of handling of such black phosphorus-polymer composite thin films affords new opportunities for wider applications such as optical sensing, signal processing and light modulation., Comment: 18 pages, 4 figures

Graphene is a rising star in nonlinear optics due to its saturable absorption and giant Kerr nonlinearity, these properties are useful in digital optics based on optical nonlinear devices. However, practical applications require large optical nonlinearities and these are inherently limited by the interaction length of atomically thin graphene. Here, we demonstrate optical bistability in a Fabry Perot cavity containing monolayer and bilayer graphene which have been restructured to form nanobubbles. We find that graphene nanobubble can act as a new type of optical nonlinear media due to its vertical side wall as well as added curvature, which enable strong non linear dispersive effects leading to a large optically induced phase change. Unlike thermally induced bistability, the all optical switching between two transmission states happens within a time scale of tens of nanoseconds. Nanobubble based optical devices with intrinsic optical nonlinearity help to overcome the optical path length limitation of atomically thin two dimensional films and allow us to explore the promise of using such elements as the building block of digital all-optical circuitry., Comment: 17 pages, 4 figures

We manipulate optical Tamm states in graphene-based photonics to achieve and steer large magneto-optical effects. Here we report the presence of a giant Faraday rotation via a single graphene layer of atomic thickness while keeping a high transmission. The Faraday rotation is enhanced across the interface between two photonic crystals due to the presence of an interface mode, which presents a strong electromagnetic field confinement at the location of the graphene sheet. Our proposed scheme opens a promising avenue to realize high performance graphene magneto-optical devices that can be extended to other two-dimensional structures., Comment: 18 pages, 4 figures

Under strong laser illumination, few-layer graphene exhibits both a transmittance increase due to saturable absorption and a nonlinear phase shift. Here, we unambiguously distinguish these two nonlinear optical effects and identify both real and imaginary parts of the complex nonlinear refractive index of graphene. We show that graphene possesses a giant nonlinear refractive index n2=10-7cm2W-1, almost nine orders of magnitude larger than bulk dielectrics. We find that the nonlinear refractive index decreases with increasing excitation flux but slower than the absorption. This suggests that graphene may be a very promising nonlinear medium, paving the way for graphene-based nonlinear photonics., Comment: Optics Letters received 12/02/2011; accepted 03/12/2012; posted 03/21/2012,Doc. ID 159129

We demonstrate that the intrinsic properties of monolayer graphene allow it to act as a more effective saturable absorber for mode-locking fiber lasers compared to multilayer graphene. The absorption of monolayer graphene can be saturated at lower excitation intensity compared to multilayer graphene, graphene with wrinkle-like defects, and functionalized graphene. Monolayer graphene has a remarkable large modulation depth of 95.3%, whereas the modulation depth of multilayer graphene is greatly reduced due to nonsaturable absorption and scattering loss. Picoseconds ultrafast laser pulse (1.23 ps) can be generated using monolayer graphene as saturable absorber. Due to the ultrafast relaxation time, larger modulation depth and lower scattering loss of monolayer graphene, it performs better than multilayer graphene in terms of pulse shaping ability, pulse stability and output energy., Comment: 23 pages

Soliton operation and soliton wavelength tuning of erbium-doped fiber lasers mode locked with atomic layer graphene was experimentally investigated under various cavity dispersion conditions. It was shown that not only wide range soliton wavelength tuning but also soltion pulse width variation could be obtained in the fiber lasers. Our results show that the graphene mode locked erbium-doped fiber lasers provide a compact, user friendly and low cost wavelength tunable ultrahsort pulse source.