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.

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.

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.

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.

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.

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.

Interactions between Fermi polarons in monolayer WS2.

Interactions between quasiparticles are of fundamental importance and ultimately determine the macroscopic properties of quantum matter. A famous example is the phenomenon of superconductivity, which arises from attractive electron-electron interactions that are mediated by phonons or even other more exotic fluctuations in the material. Here we introduce mobile exciton impurities into a two-dimensional electron gas and investigate the interactions between the resulting Fermi polaron quasiparticles. We employ multi-dimensional coherent spectroscopy on monolayer WS2, which provides an ideal platform for determining the nature of polaron-polaron interactions due to the underlying trion fine structure and the valley specific optical selection rules. At low electron doping densities, we find that the dominant interactions are between polaron states that are dressed by the same Fermi sea. In the absence of bound polaron pairs (bipolarons), we show using a minimal microscopic model that these interactions originate from a phase-space filling effect, where excitons compete for the same electrons. We furthermore reveal the existence of a bipolaron bound state with remarkably large binding energy, involving excitons in different valleys cooperatively bound to the same electron. Our work lays the foundation for probing and understanding strong electron correlation effects in two-dimensional layered structures such as moiré superlattices.

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.

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.

Engineering the Dynamics and Transport of Excitons, Trions, and Biexcitons in Monolayer WS2.

The study of transport and diffusion dynamics of quasi-particles such as excitons, trions, and biexcitons in two-dimensional (2D) semiconductors has opened avenues for their application in high-speed excitonic and optoelectronic devices. However, long-range transport and fast diffusion of these quasi-particles have not been reported for 2D systems such as transition metal dichalcogenides (TMDCs). The reported diffusion coefficients from TMDCs are low, limiting their use in high-speed excitonic devices and other optoelectronic applications. Here, we report the highest exciton diffusion coefficient value in monolayer WS2 achieved via engineering the radiative lifetime and diffusion lengths using static back-gate voltage and substrate engineering. Electrostatic doping is observed to modulate the radiative lifetime and in turn the diffusion coefficient of excitons by ∼three times at room temperature. By combining electrostatic doping and substrate engineering, we push the diffusion coefficient to an extremely high value of 86.5 cm2/s, which has not been reported before in TMDCs and is even higher than the values in some 1D systems. At low temperatures, we further report the control of dynamic and spatial diffusion of excitons, trions, and biexcitons from WS2. The electrostatic control of dynamics and transport of these quasi-particles in monolayers establishes monolayer TMDCs as ideal candidates for high-speed excitonic circuits, optoelectronic, and photonic device applications.

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.

Varied Magnetic Phases in a van der Waals Easy-Plane Antiferromagnet Revealed by Nitrogen-Vacancy Center Microscopy.

Interest in van der Waals materials often stems from a desire to miniaturize existing technologies by exploiting their intrinsic layered structures to create near-atomically thin components that do not suffer from surface defects. One appealing property is an easily switchable yet robust magnetic order, which is only sparsely demonstrated in the case of in-plane anisotropy. In this work, we use widefield nitrogen-vacancy (NV) center magnetic imaging to measure the properties of individual flakes of CuCrP2S6, a multiferroic van der Waals magnet known to exhibit weak easy-plane anisotropy in the bulk. We chart the crossover between the in-plane ferromagnetism in thin flakes down to the trilayer and the bulk behavior dominated by a low-field spin-flop transition. Further, by exploiting the directional dependence of NV center magnetometry, we are able to observe an instance of a predominantly out-of-plane ferromagetic phase near zero field, in contrast with our expectation and previous experiments on the bulk material. We attribute this to the presence of surface anisotropies caused by the sample preparation process or exposure to the ambient environment, which is expected to have more general implications for a broader class of weakly anisotropic van der Waals magnets.

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.

Recent Developments in van der Waals Antiferromagnetic 2D Materials: Synthesis, Characterization, and Device Implementation.

Magnetism in two dimensions is one of the most intriguing and alluring phenomena in condensed matter physics. Atomically thin 2D materials have emerged as a promising platform for exploring magnetic properties, leading to the development of essential technologies such as supercomputing and data storage. Arising from spin and charge dynamics in elementary particles, magnetism has also unraveled promising advances in spintronic devices and spin-dependent optoelectronics and photonics. Recently, antiferromagnetism in 2D materials has received extensive attention, leading to significant advances in their understanding and emerging applications; such materials have zero net magnetic moment yet are internally magnetic. Several theoretical and experimental approaches have been proposed to probe, characterize, and modulate the magnetic states efficiently in such systems. This Review presents the latest developments and current status for tuning the magnetic properties in distinct 2D van der Waals antiferromagnets. Various state-of-the-art optical techniques deployed to investigate magnetic textures and dynamics are discussed. Furthermore, device concepts based on antiferromagnetic spintronics are scrutinized. We conclude with remarks on related challenges and technological outlook in this rapidly expanding field.

Two-dimensional multiferroics.

Due to unprecedented application prospects such as high-density and low-power multistate storage, spintronics and nanoelectronics, two-dimensional (2D) multiferroics, coupled with at least two ferroic orders, have gotten a lot of interest in recent years. Multiple functions can be achieved in 2D multiferroics via coupling phenomena such as magnetoelectricity, piezoelectricity, and magnetoelasticity, which offers technical support for the creation of multifunctional devices. The research progress of 2D ferromagnetic-ferroelectric multiferroic materials, ferroelectric-ferroelastic multiferroic materials, and ferromagnetic-ferroelastic materials in recent years is reviewed in this paper. The categorization of 2D multiferroics is explored in terms of the multiple sources of ferroelectricity. The top-down approaches and the bottom-up methods used to fabricate 2D multiferroics materials are introduced. Finally, the authors outline potential research prospects and application scenarios for 2D multiferroic materials.

Tunable unidirectional nonlinear emission from transition-metal-dichalcogenide metasurfaces.

Nonlinear light sources are central to a myriad of applications, driving a quest for their miniaturisation down to the nanoscale. In this quest, nonlinear metasurfaces hold a great promise, as they enhance nonlinear effects through their resonant photonic environment and high refractive index, such as in high-index dielectric metasurfaces. However, despite the sub-diffractive operation of dielectric metasurfaces at the fundamental wave, this condition is not fulfilled for the nonlinearly generated harmonic waves, thereby all nonlinear metasurfaces to date emit multiple diffractive beams. Here, we demonstrate the enhanced single-beam second- and third-harmonic generation in a metasurface of crystalline transition-metal-dichalcogenide material, offering the highest refractive index. We show that the interplay between the resonances of the metasurface allows for tuning of the unidirectional second-harmonic radiation in forward or backward direction, not possible in any bulk nonlinear crystal. Our results open new opportunities for metasurface-based nonlinear light-sources, including nonlinear mirrors and entangled-photon generation.

A High-Efficiency Wavelength-Tunable Monolayer LED with Hybrid Continuous-Pulsed Injection.

High-efficiency and wavelength-tunable light-emitting diode (LED) devices will play an important role in future advanced optoelectronic systems. Traditional semiconductor LED devices typically have a fixed emission wavelength that is determined by the energy of the emission states. Here, a novel high-efficiency and wavelength-tunable monolayer WS2 LED device, which operates in the hybrid mode of continuous-pulsed injection, is developed. This hybrid injection enables highly enhanced emission efficiency (>20 times) and effective size of emission area (>5 times) at room temperature. The emission wavelength of the WS2 monolayer LED device can be tuned over more than 40 nm by driving AC voltages, from exciton emission to trion emission, and further to defect emission. The quantum efficiency of defect electroluminescence (EL) emission is measured to be more than 24.5 times larger than that from free exciton and trion EL emission. The separate carrier injection in the LED also demonstrates advantages in allowing defect species to be visualized and distinguished in real space. Those defects are assigned to be negatively charged defects. The results open a new route to develop high-performance and wavelength-tunable LED devices for future advanced optoelectronic applications.

Giant Photoluminescence Enhancement and Resonant Charge Transfer in Atomically Thin Two-Dimensional Cr2Ge2Te6/WS2 Heterostructures.

Hybridization of two-dimensional (2D) magnetic semiconductors with transition-metal dichalcogenides (TMDC) monolayers can significantly engineer the light-matter interactions and provide a promising platform for enhanced excitonic systems with artificially tailored band alignments. Here, we report the fabrication of heterostructures with monolayer WS2 on 2D Cr2Ge2Te6 (CGT), which displayed giant photoluminescence enhancement at specific CGT layer numbers. The highly enhanced quantum yield obtained can be explained by novel photoexcited carrier dynamics, facilitated by alternate relaxation channels, resulting in resonance charge transfer at the heterointerface. 2D CGT revealed a strongly layer-dependent work function (up to ∼750 meV), which greatly modulates the band positioning in the heterostructure. These heterostructures conceived both type I and type II band alignments, which are verified by Kelvin probe force microscopy and PL measurements. In addition to layer modulation, we uncover temperature and power dependence of the resonance charge transfer in the multilayer heterostructure. Our findings provide further insights into the ultrafast charge dynamics occurring at the atomic interfaces. The results may pave the way for novel optoelectronics based on van der Waals heterostructures.

π-phase modulated monolayer supercritical lens.

The emerging monolayer transition metal dichalcogenides have provided an unprecedented material platform for miniaturized opto-electronic devices with integrated functionalities. Although excitonic light-matter interactions associated with their direct bandgaps have received tremendous research efforts, wavefront engineering is less appreciated due to the suppressed phase accumulation effects resulting from the vanishingly small thicknesses. By introducing loss-assisted singular phase behaviour near the critical coupling point, we demonstrate that integration of monolayer MoS2 on a planar ZnO/Si substrate, approaching the physical thickness limit of the material, enables a π phase jump. Moreover, highly dispersive extinctions of MoS2 further empowers broadband phase regulation and enables binary phase-modulated supercritical lenses manifesting constant sub-diffraction-limited focal spots of 0.7 Airy units (AU) from the blue to yellow wavelength range. Our demonstrations downscaling optical elements to atomic thicknesses open new routes for ultra-compact opto-electronic systems harnessing two-dimensional semiconductor platforms with integrated functionalities.