Enhanced interactions of interlayer excitons in free-standing heterobilayers.

Strong, long-range dipole-dipole interactions between interlayer excitons (IXs) can lead to new multiparticle correlation regimes1,2, which drive the system into distinct quantum and classical phases2-5, including dipolar liquids, crystals and superfluids. Both repulsive and attractive dipole-dipole interactions have been theoretically predicted between IXs in a semiconductor bilayer2,6-8, but only repulsive interactions have been reported experimentally so far3,9-16. This study investigated free-standing, twisted (51°, 53°, 45°) tungsten diselenide/tungsten disulfide (WSe2/WS2) heterobilayers, in which we observed a transition in the nature of dipolar interactions among IXs, from repulsive to attractive. This was caused by quantum-exchange-correlation effects, leading to the appearance of a robust interlayer biexciton phase (formed by two IXs), which has been theoretically predicted6-8 but never observed before in experiments. The reduced dielectric screening in a free-standing heterobilayer not only resulted in a much higher formation efficiency of IXs, but also led to strongly enhanced dipole-dipole interactions, which enabled us to observe the many-body correlations of pristine IXs at the two-dimensional quantum limit. In addition, we firstly observed several emission peaks from moiré-trapped IXs at room temperature in a well-aligned, free-standing WSe2/WS2 heterobilayer. Our findings open avenues for exploring new quantum phases with potential for applications in non-linear optics.

Twisted van der Waals Quantum Materials: Fundamentals, Tunability, and Applications.

Twisted van der Waals (vdW) quantum materials have emerged as a rapidly developing field of two-dimensional (2D) semiconductors. These materials establish a new central research area and provide a promising platform for studying quantum phenomena and investigating the engineering of novel optoelectronic properties such as single photon emission, nonlinear optical response, magnon physics, and topological superconductivity. These captivating electronic and optical properties result from, and can be tailored by, the interlayer coupling using moiré patterns formed by vertically stacking atomic layers with controlled angle misorientation or lattice mismatch. Their outstanding properties and the high degree of tunability position them as compelling building blocks for both compact quantum-enabled devices and classical optoelectronics. This paper offers a comprehensive review of recent advancements in the understanding and manipulation of twisted van der Waals structures and presents a survey of the state-of-the-art research on moiré superlattices, encompassing interdisciplinary interests. It delves into fundamental theories, synthesis and fabrication, and visualization techniques, and the wide range of novel physical phenomena exhibited by these structures, with a focus on their potential for practical device integration in applications ranging from quantum information to biosensors, and including classical optoelectronics such as modulators, light emitting diodes, lasers, and photodetectors. It highlights the unique ability of moiré superlattices to connect multiple disciplines, covering chemistry, electronics, optics, photonics, magnetism, topological and quantum physics. This comprehensive review provides a valuable resource for researchers interested in moiré superlattices, shedding light on their fundamental characteristics and their potential for transformative applications in various fields.

Negative Capacitance Field Effect Transistors based on Van der Waals 2D Materials.

Steep subthreshold swing (SS) is a decisive index for low energy consumption devices. However, the SS of conventional field effect transistors (FETs) has suffered from Boltzmann Tyranny, which limits the scaling of SS to sub-60 mV dec-1 at room temperature. Ferroelectric gate stack with negative capacitance (NC) is proved to reduce the SS effectively by the amplification of the gate voltage. With the application of 2D ferroelectric materials, the NC FETs can be further improved in performance and downscaled to a smaller dimension as well. This review introduces some related concepts for in-depth understanding of NC FETs, including the NC, internal gate voltage, SS, negative drain-induced barrier lowering, negative differential resistance, single-domain state, and multi-domain state. Meanwhile, this work summarizes the recent advances of the 2D NC FETs. Moreover, the electrical characteristics of some high-performance NC FETs are expressed as well. The factors which affect the performance of the 2D NC FETs are also presented in this paper. Finally, this work gives a brief summary and outlook for the 2D NC FETs.

12.6 dB squeezed light at 1550 nm from a bow-tie cavity for long-term high duty cycle operation.

Squeezed states are an interesting class of quantum states that have numerous applications. This work presents the design, characterization, and operation of a bow-tie optical parametric amplifier (OPA) for squeezed vacuum generation. We report the high duty cycle operation and long-term stability of the system that makes it suitable for post-selection based continuous-variable quantum information protocols, cluster-state quantum computing, quantum metrology, and potentially gravitational wave detectors. Over a 50 hour continuous operation, the measured squeezing levels were greater than 10 dB with a duty cycle of 96.6%. Alternatively, in a different mode of operation, the squeezer can also operate 10 dB below the quantum noise limit over a 12 hour period with no relocks, with an average squeezing of 11.9 dB. We also measured a maximum squeezing level of 12.6 dB at 1550 nm. This represents one of the best reported squeezing results at 1550 nm to date for a bow-tie cavity. We discuss the design aspects of the experiment that contribute to the overall stability, reliability, and longevity of the OPA, along with the automated locking schemes and different modes of operation.

Quasi-line Spectral Emissions from Highly Crystalline One-Dimensional Organic Nanowires.

Zero-phonon line (ZPL) emissions have key applications in single-photon emission sources, quantum information processing, and single-molecule spectroscopy. All recent attempts to realize ZPL emissions are based on the techniques of confining and doping molecules in matrixes or solutions in low-temperature Shpol'skii systems. The requirement of two-component systems reduces the light emission efficiency from the molecules and limits their applications in solid-state electronic applications and quantum computing devices. Here, we report the first experimental demonstration of the Shpol'skii effect in a one-component organic solid-state system at low temperature. We observe a ZPL emission with a width of ∼1 to 2 nm and a high value of the Debye-Waller factor (0.72) from our epitaxially grown highly crystalline and ordered 1D organic nanowire, which is attributed to a specific molecular configuration and a higher degree of molecular orientation as compared to that of the bulk thin film counterpart. Our results pave the way for organic 1D wires (with quasi-line spectra) for applications in lasing, nanosensors, and interconnects/functional units in next-generation miniaturized optoelectronics.

Multiwavelength Single Nanowire InGaAs/InP Quantum Well Light-Emitting Diodes.

We report multiwavelength single InGaAs/InP quantum well nanowire light-emitting diodes grown by metal organic chemical vapor deposition using selective area epitaxy technique and reveal the complex origins of their electroluminescence properties. We observe that the single InGaAs/InP quantum well embedded in the nanowire consists of three components with different chemical compositions, axial quantum well, ring quantum well, and radial quantum well, leading to the electroluminescence emission with multiple wavelengths. The electroluminescence measurements show a strong dependence on current injection levels as well as temperatures and these are explained by interpreting the equivalent circuits in a minimized area of the device. It is also found that the electroluminescence properties are closely related to the distinctive triangular morphology with an inclined facet of the quantum well nanowire. Our study provides important new insights for further design, growth, and fabrication of high-performance quantum well-based nanowire light sources for a wide range of future optoelectronic and photonic applications.

In-Plane Isotropic/Anisotropic 2D van der Waals Heterostructures for Future Devices.

Mono- to few-layers of 2D semiconducting materials have uniquely inherent optical, electronic, and magnetic properties that make them ideal for probing fundamental scientific phenomena up to the 2D quantum limit and exploring their emerging technological applications. This Review focuses on the fundamental optoelectronic studies and potential applications of in-plane isotropic/anisotropic 2D semiconducting heterostructures. Strong light-matter interaction, reduced dimensionality, and dielectric screening in mono- to few-layers of 2D semiconducting materials result in strong many-body interactions, leading to the formation of robust quasiparticles such as excitons, trions, and biexcitons. An in-plane isotropic nature leads to the quasi-2D particles, whereas, an anisotropic nature leads to quasi-1D particles. Hence, in-plane isotropic/anisotropic 2D heterostructures lead to the formation of quasi-1D/2D particle systems allowing for the manipulation of high binding energy quasi-1D particle populations for use in a wide variety of applications. This Review emphasizes an exciting 1D-2D particles dynamic in such heterostructures and their potential for high-performance photoemitters and exciton-polariton lasers. Moreover, their scopes are also broadened in thermoelectricity, piezoelectricity, photostriction, energy storage, hydrogen evolution reactions, and chemical sensor fields. The unique in-plane isotropic/anisotropic 2D heterostructures may open the possibility of engineering smart devices in the nanodomain with complex opto-electromechanical functions.

Highly Enhanced Many-Body Interactions in Anisotropic 2D Semiconductors.

Atomically thin two-dimensional (2D) semiconductors have presented a plethora of opportunities for future optoelectronic devices and photonics applications, made possible by the strong light matter interactions at the 2D quantum limit. Many body interactions between fundamental particles in 2D semiconductors are strongly enhanced compared with those in bulk semiconductors because of the reduced dimensionality and, thus, reduced dielectric screening. These enhanced many body interactions lead to the formation of robust quasi-particles, such as excitons, trions, and biexcitons, which are extremely important for the optoelectronics device applications of 2D semiconductors, such as light emitting diodes, lasers, and optical modulators, etc. Recently, the emerging anisotropic 2D semiconductors, such as black phosphorus (termed as phosphorene) and phosphorene-like 2D materials, such as ReSe2, 2D-perovskites, SnS, etc., show strong anisotropic optical and electrical properties, which are different from conventional isotropic 2D semiconductors, such as transition metal dichalcogenide (TMD) monolayers. This anisotropy leads to the formation of quasi-one-dimensional (quasi-1D) excitons and trions in a 2D system, which results in even stronger many body interactions in anisotropic 2D materials, arising from the further reduced dimensionality of the quasi-particles and thus reduced dielectric screening. Many body interactions have been heavily investigated in TMD monolayers in past years, but not in anisotropic 2D materials yet. The quasi-particles in anisotropic 2D materials have fractional dimensionality which makes them perfect candidates to serve as a platform to study fundamental particle interactions in fractional dimensional space. In this Account, we present our recent progress related to 2D phosphorene, a 2D system with quasi-1D excitons and trions. Phosphorene, because of its unique anisotropic properties, provides a unique 2D platform for investigating the dynamics of excitons, trions, and biexcitons in reduced dimensions and fundamental many body interactions. We begin by explaining the fundamental reasons for the highly enhanced interactions in the 2D systems influenced by dielectric screening, resulting in high binding energies of excitons and trions, which are supported by theoretical calculations and experimental observations. Phosphorene has shown much higher binding energies of excitons and trions than TMD monolayers, which allows robust quasi-particles in anisotropic materials at room temperature. We also discuss the role of extrinsic defects induced in phosphorene, resulting in localized excitonic emissions in the near-infrared range, making it suitable for optical telecommunication applications. Finally, we present our vision of the exciting device applications based on the highly enhanced many body interactions in phosphorene, including exciton-polariton devices, polariton lasers, single-photon emitters, and tunable light emitting diodes (LEDs).

Defect Engineering in Few-Layer Phosphorene.

Defect engineering in 2D phosphorene samples is becoming an important and powerful technique to alter their properties, enabling new optoelectronic applications, particularly at the infrared wavelength region. Defect engineering in a few-layer phosphorene sample via introduction of substrate trapping centers is realized. In a three-layer (3L) phosphorene sample, a strong photoluminescence (PL) emission peak from localized excitons at ≈1430 nm is observed, a much lower energy level than free excitonic emissions. An activation energy of ≈77 meV for the localized excitons is determined in temperature-dependent PL measurements. The relatively high activation energy supports the strong stability of the localized excitons even at elevated temperature. The quantum efficiency of localized exciton emission in 3L phosphorene is measured to be approximately three times higher than that of free excitons. These results could enable exciting applications in infrared optoelectronics.

Light-Matter Interactions in Phosphorene.

Since the beginning of 2014, phosphorene, a monolayer or few-layer of black phosphorus, has been rediscovered as a two-dimensional (2D) thin film, revealing a plethora of properties different from the bulk material studied so far. Similar to graphene and transition metal dichalcogenides (TMDs), phosphorene is also a layered material that can be exfoliated to yield individual layers. It is one of the few monoelemental 2D crystals and the only one, besides graphene, known to be stable in monolayer, few layer, and bulk form. Recently the intensified research in phosphorene is motivated not only by the study of its fundamental physical properties in the 2D regime, such as tunable bandgap and anisotropic behavior, but also by the high carrier mobility and good on/off ratio of phosphorene-based device prototypes, making it a potential alternative for next generation nanooptoelectronics and nanophotonics applications in the "post-graphene age" The electronic bandgap of phosphorene changes from 0.3 eV in the bulk to 2.1 eV in monolayer. Thus, phosphorene exhibits strong light-matter interactions in the visible and infrared (IR) frequencies. In this Account, we present the progress on understanding the various interactions between light and phosphorene, giving insight into the mechanism of these interactions and the respective applications. We begin by discussing the fundamental optical properties of phosphorene, using theoretical calculations to depict the layer-dependent electronic band structures and anisotropic optical properties. Many-body effects in phosphorene, including excitons and trions and their binding energies and dynamics are reviewed as observed in experiments. For phosphorene, the fast degradation in ambient condition, caused by photoinduced oxidation, is considered as a longstanding challenge. In contrast, oxidation can be used to engineer the band structure of phosphorene and, in parallel, its optical properties. Based on the strong light-matter interactions, we introduce a controllable method to directly oxidize phosphorene by laser techniques. With the oxidization induced by laser scanning, localized bandgap engineering can be achieved and microphotonics are demonstrated on the oxidized phosphorene. Finally, we will present a brief discussion on the realization of phosphorene-based building blocks of optoelectronic devices. Naturally, the strong light-matter interactions in phosphorene could enable efficient photoelectric conversion in optoelectronic devices. We will describe high performance photodetectors based on phosphorene, and the working mechanism of those devices will be introduced. The photovoltaic effect could also be exhibited in phosphorene. This indicates the pervasive potential of phosphorene in nanooptoelectronics.

Strongly enhanced photoluminescence in nanostructured monolayer MoS2 by chemical vapor deposition.

Two-dimensional (2D) layered molybdenum disulfide (MoS2) has become a very promising candidate semiconducting material for future optoelectronic devices, owing to its unique properties. However, monolayer MoS2 is still a weak photon emitter, compared with other direct band gap semiconductors, which requires extra techniques or complicated steps to enhance its photon emission efficiency. Here, we demonstrated that nanostructured monolayer MoS2, produced by one-step chemical vapor deposition (CVD) growth, shows highly enhanced PL emission. The effective enhancement factor could be up to ∼43. Our results open the door to manipulating the optical properties of future devices by using nanostructured 2D monolayers.

Exciton and Trion Dynamics in Bilayer MoS2.

The control of exciton and triondynamics in bilayer MoS2 is demonstrated, via the comodulations by both temperature and electric field. The calculations here show that the band structure of bilayer MoS2 changes from indirect at room temperature toward direct nature as temperature decreases, which enables the electrical tunability of the K-K direct PL transition in bilayer MoS2 at low temperature.

Tailor-Made Gold Nanomaterials for Applications in Soft Bioelectronics and Optoelectronics.

In modern nanoscience and nanotechnology, gold nanomaterials are indispensable building blocks that have demonstrated a plethora of applications in catalysis, biology, bioelectronics, and optoelectronics. Gold nanomaterials possess many appealing material properties, such as facile control over their size/shape and surface functionality, intrinsic chemical inertness yet with high biocompatibility, adjustable localized surface plasmon resonances, tunable conductivity, wide electrochemical window, etc. Such material attributes have been recently utilized for designing and fabricating soft bioelectronics and optoelectronics. This motivates to give a comprehensive overview of this burgeoning field. The discussion of representative tailor-made gold nanomaterials, including gold nanocrystals, ultrathin gold nanowires, vertically aligned gold nanowires, hard template-assisted gold nanowires/gold nanotubes, bimetallic/trimetallic gold nanowires, gold nanomeshes, and gold nanosheets, is begun. This is followed by the description of various fabrication methodologies for state-of-the-art applications such as strain sensors, pressure sensors, electrochemical sensors, electrophysiological devices, energy-storage devices, energy-harvesting devices, optoelectronics, and others. Finally, the remaining challenges and opportunities are discussed.

Enhancing 2D Photonics and Optoelectronics with Artificial Microstructures.

By modulating subwavelength structures and integrating functional materials, 2D artificial microstructures (2D AMs), including heterostructures, superlattices, metasurfaces and microcavities, offer a powerful platform for significant manipulation of light fields and functions. These structures hold great promise in high-performance and highly integrated optoelectronic devices. However, a comprehensive summary of 2D AMs remains elusive for photonics and optoelectronics. This review focuses on the latest breakthroughs in 2D AM devices, categorized into electronic devices, photonic devices, and optoelectronic devices. The control of electronic and optical properties through tuning twisted angles is discussed. Some typical strategies that enhance light-matter interactions are introduced, covering the integration of 2D materials with external photonic structures and intrinsic polaritonic resonances. Additionally, the influences of external stimuli, such as vertical electric fields, enhanced optical fields and plasmonic confinements, on optoelectronic properties is analysed. The integrations of these devices are also thoroughly addressed. Challenges and future perspectives are summarized to stimulate research and development of 2D AMs for future photonics and optoelectronics.

Enhanced interactions of excitonic complexes in free-standing WS2.

Excitonic complexes, bound states of electrons and holes, provide a promising platform in monolayer transition-metal dichalcogenide (TMDC) semiconductors for investigating diverse many-body interaction phenomena. The surrounding dielectric environment has been found to strongly influence the excitonic properties of the TMDC monolayers. While the impact of different dielectric surroundings on two-dimensional semiconductor materials and their strong correlations have been well studied, the effects on exciton formation and its properties resulting from a further reduction in dielectric screening remain elusive. In this study, we examined free-standing tungsten disulfide (WS2) monolayers, where the efficient generation of higher-order correlated excitonic complexes is readily observed. This phenomenon arises from the effective mutual interactions among excitons and internal carriers, attributed to the modulated exciton dynamics generated by the further reduced dielectric screening effect in the freestanding structure. The formation efficiency of excitonic complexes is enhanced and the multiple biexciton species (five particles such as charged biexcitons and acceptor/donor-bound biexcitons) are successfully induced under low excitation intensity and moderate temperature conditions. Our findings offer valuable insights into the influence of the dielectric environment on exciton interactions and enable a productive avenue for exploring fundamental many-body interactions, providing new possibilities for dielectric engineering of atomic thin semiconductors.

Enhanced Room Temperature Ferromagnetism in Highly Strained 2D Semiconductor Cr2Ge2Te6.

Emergent magnetism in van der Waals materials offers exciting opportunities in fabricating atomically thin spintronic devices. One pertinent obstacle has been the low transition temperatures (Tc) inherent to these materials, precluding room temperature applications. Here, we show that large structural gradients found in highly strained nanoscale wrinkles in Cr2Ge2Te6 (CGT) lead to significant increases of Tc. Magnetic force microscopy was utilized in characterizing multiple strained CGT nanostructures leading to experimental evidence of elevated Tc, depending on the strain percentage estimated from finite element analysis. Our findings are further supported by ab initio and DFT studies of the strained material, which indicates that strain directly augments the ferromagnetic coupling between Cr atoms in CGT, influenced by superexchange interaction; this provides strong insight into the mechanism of the enhanced magnetism and Tc.

Variant Plateau's law in atomically thin transition metal dichalcogenide dome networks.

Since its fundamental inception from soap bubbles, Plateau's law has sparked extensive research in equilibrated states. However, most studies primarily relied on liquids, foams or cellular structures, whereas its applicability has yet to be explored in nano-scale solid films. Here, we observed a variant Plateau's law in networks of atomically thin domes made of solid two-dimensional (2D) transition metal dichalcogenides (TMDs). Discrete layer-dependent van der Waals (vdWs) interaction energies were experimentally and theoretically obtained for domes protruding in different TMD layers. Significant surface tension differences from layer-dependent vdWs interaction energies manifest in a variant of this fundamental law. The equivalent surface tension ranges from 2.4 to 3.6 N/m, around two orders of magnitude greater than conventional liquid films, enabling domes to sustain high gas pressure and exist in a fundamentally variant nature for several years. Our findings pave the way towards exploring variant discretised states with applications in opto-electro-mechanical devices.

Nano-engineering and nano-manufacturing in 2D materials: marvels of nanotechnology.

Two-dimensional materials have attracted significant interest and investigation since the marvellous discovery of graphene. Due to their unique physical, mechanical and optical properties, van der Waals (vdW) materials possess extraordinary potential for application in future optoelectronics devices. Nano-engineering and nano-manufacturing in the atomically thin regime has further opened multifarious avenues to explore novel physical properties. Among them, moiré heterostructures, strain engineering and substrate manipulation have created numerous exotic and topological phenomena such as unconventional superconductivity, orbital magnetism, flexible nanoelectronics and highly efficient photovoltaics. This review comprehensively summarizes the three most influential techniques of nano-engineering in 2D materials. The latest development in the marvels of moiré structures in vdW materials is discussed; in addition, topological structures in layered materials and substrate engineering on the nanoscale are thoroughly scrutinized to highlight their significance in micro- and nano-devices. Finally, we conclude with remarks on challenges and possible future directions in the rapidly expanding field of nanotechnology and nanomaterial.

Extraordinary Phonon Displacement and Giant Resonance Raman Enhancement in WSe2/WS2 Moiré Heterostructures.

Twisted van der Waals heterostructures are known to induce surprisingly diverse and intriguing phenomena, such as correlated electronic phase and unconventional optical properties. This can be realized by controlled rotation of adjacent atomic planes, which provides an uncommon way to manipulate inelastic light-matter interactions. Here, we discover an extraordinary blue shift of 5-6 wavenumbers for high-frequency phonon modes in WS2/WSe2 twisted heterobilayers, captured meticulously using Raman spectroscopy. Phonon spectra displace rapidly over a subtle change in interlayer twist angle owing to heterostrain and atomic reconstruction from the Moiré pattern. First-order linear coefficients of the phonon modes in twisted heterostructures are further found to increase largely compared to their monolayer counterpart and vary immensely with the twist angle. Exceptional and extravagant enhancement of up to 50-fold is observed in the Raman vibrational intensity at a specific twist angle; this is largely influenced by the resonance process derived from a simple critical twist angle model. In addition, we depict how the resonance can be modulated by changing the thermal conditions and also the stacking angle. Therefore, our work further highlights the twist-driven phonon dynamics in pristine two-dimensional heterostructures, adding vital insight into Moiré physics and promoting comprehensive understanding of structural and optical properties in Moiré superlattices.

Extraordinary Nonlinear Optical Interaction from Strained Nanostructures in van der Waals CuInP2S6.

Local strain engineering and structural modification of 2D materials furnish benevolent control over their optoelectronic properties and provide an exciting approach to tune light-matter interaction in layered materials. Application of strain at the nanoscale is typically obtained through permanently deformed nanostructures such as nanowrinkles, which yield large band gap modulation, photoluminescence enhancement, and surface potential. Ultrathin transition metal dichalcogenides (TMDs) have been greatly analyzed for such purposes. Herein, we extend strain-induced nanoengineering to an emerging 2D material, CuInP2S6 (CIPS), and visualize extraordinary control over nonlinear light-matter interaction. Wrinkle nanostructures exhibit ∼160-fold enhancement in second harmonic generation (SHG) compared to unstrained regions, which is additionally influenced by a change in the dielectric environment. The SHG enhancement was significantly modulated by the percentage of applied strain which was numerically estimated. Furthermore, polarization-dependent SHG revealed quenching and enhancement in the parallel and perpendicular directions, respectively, due to the direction of the compressive vector. Our work provides an important advancement in controlling optoelectronic properties beyond TMDs for imminent applications in flexible electronics.