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1. Exfoliation and Analysis of Large-area, Air-Sensitive Two-Dimensional Materials

   https://doi.org/10.3791/58693  

   Thompson, J. P.; Doha, M. H.; Murphy, P.; Hu, J.; Churchill, H. O. (January 2019, Journal of visualized experiments)

   We describe methods for producing and analyzing large, thin flakes of air-sensitive two-dimensional materials. Thin flakes of layered or van der Waals crystals are produced using mechanical exfoliation, in which layers are peeled off a bulk crystal using adhesive tape. This method produces high-quality flakes, but they are often small and can be hard to find, particularly for materials with relatively high cleavage energies such as black phosphorus. By heating the substrate and the tape, two-dimensional material adhesion to the substrate is promoted, and the flake yield can be increased by up to a factor of ten. After exfoliation, it is necessary to image or otherwise analyze these flakes but some two-dimensional materials are sensitive to oxygen or water and will degrade when exposed air. We have designed and tested a hermetic transfer cell to temporarily maintain the inert environment of a glovebox so that air-sensitive flakes can be imaged and analyzed with minimal degradation. The compact design of the transfer cell is such that optical analysis of sensitive materials can be performed outside of a glovebox without specialized equipment or modifications to existing equipment. 

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2. High mobility in a van der Waals layered antiferromagnetic metal

   https://doi.org/10.1126/sciadv.aay6407  

   Lei, Shiming; Lin, Jingjing; Jia, Yanyu; Gray, Mason; Topp, Andreas; Farahi, Gelareh; Klemenz, Sebastian; Gao, Tong; Rodolakis, Fanny; McChesney, Jessica L.; et al (February 2020, Science Advances)

   Van der Waals (vdW) materials with magnetic order have been heavily pursued for fundamental physics as well as for device design. Despite the rapid advances, so far, they are mainly insulating or semiconducting, and none of them has a high electronic mobility—a property that is rare in layered vdW materials in general. The realization of a high-mobility vdW material that also exhibits magnetic order would open the possibility for novel magnetic twistronic or spintronic devices. Here, we report very high carrier mobility in the layered vdW antiferromagnet GdTe 3 . The electron mobility is beyond 60,000 cm 2 V −1 s −1 , which is the highest among all known layered magnetic materials, to the best of our knowledge. Among all known vdW materials, the mobility of bulk GdTe 3 is comparable to that of black phosphorus. By mechanical exfoliation, we further demonstrate that GdTe 3 can be exfoliated to ultrathin flakes of three monolayers. 

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3. Natural layered mercury antimony sulfosalt livingstonite with anisotropic optical properties

   https://doi.org/10.1364/OE.458576  

   Tripathi, Ravi P.; Gao, Jie; Yang, Xiaodong (January 2022, Optics Express)

   Naturally occurring layered mineral livingstonite is identified as a new type of van der Waals (vdW) heterostructure based 2D material, consisting of two commensurately modulated alternating layers of HgSb 2 S 4 and Sb 2 S 4 . The heterostructures of livingstonite crystal are prepared as thin flakes via mechanical exfoliation method. The prepared livingstonite crystals are further investigated in the context of vibrational, linear, and nonlinear optical properties, including anisotropic Raman scattering, wavelength-dependent linear dichroism (LD) transition effect, birefringence, and anisotropic third-harmonic generation (THG). Owing to the monoclinic crystal structure, livingstonite crystals exhibit strong anisotropic vibrational and optical responses. In contrast to conventional vdW heterostructures, the anomalous LD transition effect and the evolution of butterfly-shaped THG emission pattern in livingstonite crystals are demonstrated. Furthermore, the third-order nonlinear susceptibility is estimated for livingstonite crystal using the thickness-dependent THG emission response. Overall, the discussed outcomes establish livingstonite as a new type of naturally grown vdW heterostructure based 2D material and offer insights in tailoring linear and nonlinear light-matter interactions in such vdW heterostructures, which may find further relevance in polarized optical applications and on-chip integrated photonic circuits. 

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4. Exfoliation of boron carbide into ultrathin nanosheets

   https://doi.org/10.1039/D0NR07971E  

   Guo, Yuqi; Gupta, Adway; Gilliam, Matthew S.; Debnath, Abhishek; Yousaf, Ahmed; Saha, Sanchari; Levin, Mark D.; Green, Alexander A.; Singh, Arunima K.; Wang, Qing Hua (January 2021, Nanoscale)

   Liquid phase exfoliation (LPE) is a method that can be used to produce bulk quantities of two-dimensional (2D) nanosheets from layered van der Waals (vdW) materials. In recent years, LPE has been applied to several non-vdW materials with anisotropic bonding to produce nanosheets and platelets, but it has not been demonstrated for materials with strong isotropic bonding. In this paper, we demonstrate the exfoliation of boron carbide (B 4 C), the third hardest known material, into ultrathin nanosheets. B 4 C has a structure consisting of strongly bonded boron icosahedra and carbon chains, but does not have anisotropic cleavage energies to suggest that it can be readily cleaved into nanosheets. B 4 C has been widely studied for its very high melting point, high mechanical strength, and chemical stability, as well as its zero- and one-dimensional nanostructured forms. Herein, ultrathin nanosheets are successfully prepared by sonication of B 4 C powder in organic solvents and are characterized by microscopy and spectroscopy. Density functional theory (DFT) simulations reveal that B 4 C can be cleaved along several different crystallographic planes with similar energetic favourability, facilititated by an unexpected mechanism of breaking boron icosahedra and forming new boron-rich cage structures at the surface. Atomic force microscopy (AFM) shows that the nanosheets produced by LPE are as thin as 5 nm, with an average thickness of 31.4 nm and average area of 16 000 nm 2 . Raman spectroscopy shows that many of the nanosheets exhibit additional carbon-rich peaks that change with laser irradiation, which are attributed to atomic rearrangements and amorphization at the nanosheet surfaces, consistent with the diverse cleavage planes. High-resolution transmission electron microscopy (HRTEM) demonstrates that many different cleavage planes exist among the exfoliated nanosheets, in agreement with DFT simulations. This work elucidates the exfoliation mechanism of 2D B 4 C and suggests that LPE can be applied to generate nanosheets from a variety of non-layered and non-vdW materials. 

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5. 2D layered SiP as anisotropic nonlinear optical material

   https://doi.org/10.1038/s41598-021-85938-4  

   Sar, Huseyin; Gao, Jie; Yang, Xiaodong (December 2021, Scientific Reports)

   null (Ed.)

   Abstract Two-dimensional (2D) material of silicon phosphide (SiP) has recently been shown as a promising optical material with large band gap, fast photoresponse and strong anisotropy. However, the nonlinear optical properties of 2D SiP have not been investigated yet. Here, the thickness-dependent in-plane anisotropic third-harmonic generation (THG) from the mechanically exfoliated 2D layered SiP flakes is reported. The crystal orientation of the SiP flake is determined by the angle-resolved polarized Raman spectroscopy. The angular dependence of the THG emission with respect to the incident linear polarization is found to be strongly anisotropic with the two-fold polarization dependence pattern. Furthermore, the effect of the SiP flake thickness on the THG power is analyzed. 

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