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.
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.
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.
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.
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 â¼160-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.
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.
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.
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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.
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 â¼750 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.
