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Second harmonic generation is a non-linear optical phenomenon in which coherent radiation with frequency ω interacts with a non-centrosymmetric material and produces coherent radiation at frequency 2ω. Owing to the exciting physical phenomena that take place during the non-linear optical excitation at the nanoscale, there is currently extensive research in the non-linear optical responses of nanomaterials, particularly in low-dimensional materials. Here, we review recent advancements in the polarization-resolved second harmonic generation propertied from atomically thin two-dimensional (2D) crystals and present a unified theoretical framework to account for their nonlinear optical response. Two major classes of 2D materials are particularly investigated, namely metal chalcogenides and perovskites. The first attempts to tune and control the second harmonic generation properties of such materials via the application of specific nanophotonic schemes are additionally demonstrated and discussed. Besides presenting recent advances in the field, this work also delineates existing limitations and highlights emerging possibilities and future prospects in this field.

Ultrathin solid slabs often have properties different from those of the bulk phase. This effect can be observed both in traditional three-dimensional materials and in van der Waals (vdW) solids in the few monolayer limit. In the present work, the band gap variation of the CdTe slabs, induced by their thickness, was studied by the density functional theory (DFT) method for the sphalerite (zinc-blende) phase and for the recently proposed inverted phase. The sphalerite phase has the Te–Cd–Te–Cd atomic plane sequence, while in the inverted phase Cd atoms are sandwiched by Te planes forming vdW blocks with the sequence Te–Cd–Cd–Te. Based on these building blocks, a bulk vdW CdTe crystal was built, whose thermodynamical stability was verified by DFT calculations. Band structures and partial densities of states for sphalerite and inverted phases were calculated. It was demonstrated for both phases that using slabs with a thickness of one to several monolayers for sphalerite phase (vdW blocks for inverted phase), structures with band gaps varying in a wide range can be obtained. The presented results allow us to argue that ultrathin CdTe can be a promising electronic material. [ABSTRACT FROM AUTHOR]

Large‐area epitaxy of layered materials is one of the cornerstones for a successful exploitation of van der Waals (vdW) materials in the semiconductor industry. The formation of 60° twin stacking faults and 60° grain boundaries is of major concern for the defect‐free epitaxial growth. Although strategies to overcome the occurrence of these defects are being considered, more fundamental understanding on the origin of these defects is highly essential. This work focuses on understanding the formation of 60° twins in (quasi‐)vdW epitaxy of 2D chalcogenides. Molecular beam epitaxy (MBE) experiments reveal the striking difference in 60° twin occurrence between WSe2 and Bi2Se3 in both quasi‐vdW heteroepitaxy and vdW homoepitaxy. Density functional theory (DFT) calculations link this difference to the interlayer vdW coupling strength at the unit cell level. The stronger interlayer vdW coupling in Bi2Se3 unit cells compared to WSe2 unit cells is explained to result in a reduced twin occurrence. Hence, such compounds show significantly more promise for defect‐free epitaxial integration. This interesting aspect of (quasi‐)vdW epitaxy reveals that the strength of interlayer vdW coupling is key for workable 2D materials and opens perspectives for other strongly coupled vdW materials. [ABSTRACT FROM AUTHOR]

The optical properties of WSe2-layered crystals doped with 0.5% niobium (Nb) grown by the chemical vapor transport method were characterized by piezoreflectance (PzR), photoconductivity (PC) spectroscopy, frequency-dependent photocurrent, and time-resolved photoresponse. With the incorporation of 0.5% Nb, the WSe2 crystal showed slight blue shifts in the near band edge excitonic transitions and exhibited strongly enhanced photoresponsivity. Frequency-dependent photocurrent and time-resolved photoresponse were measured to explore the kinetic decay processes of carriers. Our results show the potential application of layered crystals for photodetection devices based on Nb-doped WSe2-layered crystals. [ABSTRACT FROM AUTHOR]

Understanding the mechanisms and kinetics of defect annihilations, particularly at the atomic scale, is important for the preparation of high-quality crystals for realizing the full potential of 2D transition metal dichalcogenides (TMDCs) in electronics and quantum photonics. Herein, by performing in situ annealing experiments in an atomic resolution scanning transmission electron microscope, it is found that stacking faults and rotational disorders in multilayered 2D crystals can be healed by grain boundary (GB) sliding, which works like a "wiper blade" to correct all metastable phases into thermodynamically stable phases along its trace. The driving force for GB sliding is the gain in interlayer binding energy as the more stable phase grows at the expanse of the metastable ones. Density functional theory calculations show that the correction of 2D stacking faults is triggered by the ejection of Mo atoms in mirror twin boundaries, followed by the collective migrations of 1D GB. The study highlights the role of the often-neglected interlayer interactions for defect repair in 2D materials and shows that exploiting these interactions has significant potential for obtaining large-scale defect-free 2D films., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Emulation of brain-like signal processing with thin-film devices can lay the foundation for building artificially intelligent learning circuitry in future. Encompassing higher functionalities into single artificial neural elements will allow the development of robust neuromorphic circuitry emulating biological adaptation mechanisms with drastically lesser neural elements, mitigating strict process challenges and high circuit density requirements necessary to match the computational complexity of the human brain. Here, 2D transition metal di-chalcogenide (MoS 2 ) neuristors are designed to mimic intracellular ion endocytosis-exocytosis dynamics/neurotransmitter-release in chemical synapses using three approaches: (i) electronic-mode: a defect modulation approach where the traps at the semiconductor-dielectric interface are perturbed; (ii) ionotronic-mode: where electronic responses are modulated via ionic gating; and (iii) photoactive-mode: harnessing persistent photoconductivity or trap-assisted slow recombination mechanisms. Exploiting a novel multigated architecture incorporating electrical and optical biases, this incarnation not only addresses different charge-trapping probabilities to finely modulate the synaptic weights, but also amalgamates neuromodulation schemes to achieve "plasticity of plasticity-metaplasticity" via dynamic control of Hebbian spike-time dependent plasticity and homeostatic regulation. Coexistence of such multiple forms of synaptic plasticity increases the efficacy of memory storage and processing capacity of artificial neuristors, enabling design of highly efficient novel neural architectures., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Molybdenum disulfide (MoS 2 ) and bismuth telluride (Bi 2 Te 3 ) are the two most common types of structures adopted by 2D chalcogenides. In view of their unique physical properties and structure, 2D chalcogenides have potential applications in various fields. However, the excellent properties of these 2D crystals depend critically on their crystal structures, where defects, cracks, holes, or even greater damage can be inevitably introduced during the preparation and transferring processes. Such defects adversely impact the performance of devices made from 2D chalcogenides and, hence, it is important to develop ways to intuitively and precisely repair these 2D crystals on the atomic scale, so as to realize high-reliability devices from these structures. Here, an in situ study of the repair of the nanopores in MoS 2 and Bi 2 Te 3 is carried out under electron beam irradiation by transmission electron microscopy. The experimental conditions allow visualization of the structural dynamics of MoS 2 and Bi 2 Te 3 crystals with unprecedented resolution. Real-time observation of the healing of defects at atomic resolution can potentially help to reproducibly fabricate and simultaneously image single-crystalline free-standing 2D chalcogenides. Thus, these findings demonstrate the viability of using an electron beam as an effective tool to precisely engineer materials to suit desired applications in the future., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Engineered atomic dislocations have been used to create a novel, Sb 2 Te 3 nanoplate-like architecture that exhibits a unique antisymmetric chirality. High-resolution transmission electron microscopy (HRTEM) coupled with atomic force microscopy and X-ray photoelectron spectroscopy reveals the architectures to be extremely well ordered with little residual strain. Surface modification of these topologically complex macrostructures (≈3 µm) has been achieved by direct growth of metallic Ag nanoparticles onto the edge sites of the Sb 2 Te 3 . Again, HRTEM shows this nanoparticle decoration to be atomically sharp at the boundaries and regularly spaced along the selvedge of the nanostructure. Transport experiments of densified films of these assemblies exhibit marked increases in carrier density after nanoengineering, yielding 3.5 × 10 4 S m -1 in electrical conductivity. An increased Seebeck coefficient by 20% in parallel with electrical conductivity is also observed. This gives a thermoelectric power factor of 371 µW m -1 K -2 , which is the highest value for a flexible, freestanding film to date. These results suggest an entirely new direction in the search for wearable power harvesters based on topologically complex, low-dimensional nanoassemblies., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)