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1. Top-Down Processing Towards Ångström-Thin Two-Dimensional (2D) Elemental Metals

   https://doi.org/10.1115/MSEC2020-8495  

   Rubayat-E Tanjil, Md ; Agbakansi, Stanley ; Suero, Keegan Phayden ; Douglas, Ossie ; Jeong, Yunjo ; Yin, Zhewen ; Panaccione, Wyatt ; Wang, Michael Cai ( January 2021 , Top-Down Processing Towards Ångström-Thin Two-Dimensional (2D) Elemental Metals)

   Two-dimensional (2D) materials have recently garnered significant interest due to their novel and emergent properties. A plethora of 2D materials have been discovered and intensively studied, such as graphene, hexagonal boron nitride, transitionmetal dichalcogenides (TMDCs), and other metallic compound MXenes (nitrides, phosphides, and hydroxides), as well as elemental 2D materials (borophene, germanene, phosphorene, silicene, etc.). Considering the widespread interest in conventional van der Waals 2D materials, two-dimensional metallic nanosheets (2DMNS), a recent addition to the 2D materials family, have exhibited diverse potential spanning optics, electronics, magnetics, catalysis, etc. However, the close-packed, non-layered structure and non-directional, isotropic bonding of metallic materials make it difficult to access metals in their 2D forms, unlike 2D van der Waals materials, which have intrinsically layered structure (strong in-plane bonding in addition to the weak interlayer interaction). Until now, conventional top-down and bottom-up synthesis schemes of these 2DMNS have encountered various limitations such as precursor availability, substrate incompatibility, difficulty of control over thickness and stoichiometry, limited thermal budget, etc. To overcome these manufacturing limitations of 2DMNS, here we report a facile, rapid, large-scale, and cost-effective fabrication technique of nanometer-scale copper (Cu) 2DMNS via iterative rolling, folding, and calendering (RFC) that is readily generalizable to other conventional elemental metallic materials. Overall, we successfully show a scalable fabrication technique of 2DMNS.

    

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2. Top-Down Processing Towards Ångström-Thin Two-Dimensional (2D) Elemental Metals

   Rubayat-E Tanjil, Md ; Agbakansi, Stanley ; Suero, Keegan ; Douglas, Ossie ; Jeong, Yunjo ; Yin, Zhewen ; Panaccione, Wyatt ; Cai Wang, Michael ( September 2020 , ASME 2020 15th International Manufacturing Science and Engineering Conference)

   null (Ed.)

   Two-dimensional (2D) materials have recently garnered significant interest due to their novel and emergent properties. A plethora of 2D materials have been discovered and intensively studied, such as graphene, hexagonal boron nitride, transition-metal dichalcogenides TMDCs), and other metallic compound MXenes (nitrides, phosphides, and hydroxides), as well as elemental 2D materials (borophene, germanene, phosphorene, silicene, etc.). Considering the widespread interest in conventional van der Waals 2D materials, two-dimensional metallic nanosheets (2DMNS), a recent addition to the 2D materials family, have exhibited diverse potential spanning optics, electronics, magnetics, catalysis, etc. However, the close-packed, non-layered structure and non-directional, isotropic bonding of metallic materials make it difficult to access metals in their 2D forms, unlike 2D van der Waals materials, which have intrinsically layered structure (strong in-plane bonding in addition to the weak interlayer interaction). Until now, conventional top-down and bottom-up synthesis schemes of these 2DMNS have encountered various limitations such as precursor availability, substrate incompatibility, difficulty of control over thickness and stoichiometry, limited thermal budget, etc. To overcome these manufacturing limitations of 2DMNS, here we report a facile, rapid, large-scale, and cost-effective fabrication technique of nanometer-scale copper (Cu) 2DMNS via iterative rolling, folding, and calendering (RFC) that is readily generalizable to other conventional elemental metallic materials. Overall, we successfully show a scalable fabrication technique of 2DMNS. 

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3. The influence of crystal thickness and interlayer interactions on the properties of heavy ion irradiated MoS 2

   https://doi.org/10.1088/2053-1583/ab817b  

   Isherwood, Liam H. ; Hennighausen, Zachariah ; Son, Seok-Kyun ; Spencer, Ben F. ; Wady, Paul T. ; Shubeita, Samir M. ; Kar, Swastik ; Casiraghi, Cinzia ; Baidak, Aliaksandr ( May 2020 , 2D Materials)

   Ion irradiation is a versatile tool to introduce controlled defects into two-dimensional (2D) MoS₂on account of its unique spatial resolution and plethora of ion types and energies available. In order to fully realise the potential of this technique, a holistic understanding of ion-induced defect production in 2D MoS₂crystals of different thicknesses is mandatory. X-ray photoelectron spectroscopy, electron diffraction and Raman spectroscopy show that thinner MoS₂crystals are more susceptible to radiation damage caused by 225 keV Xe⁺ions. However, the rate of defect production in quadrilayer and bulk crystals is not significantly different under our experimental conditions. The rate at which S atoms are sputtered as a function of radiation exposure is considerably higher for monolayer MoS₂, compared to bulk crystals, leading to MoO₃formation. P-doping of MoS₂is observed and attributed to the acceptor states introduced by vacancies and charge transfer interactions with adsorbed species. Moreover, the out-of-plane vibrational properties of irradiated MoS₂crystals are shown to be strongly thickness-dependent: in mono- and bilayer MoS₂, the confinement of phonons by defects results in a blueshift of the$A_{1g}$mode. Whereas, a redshift is observed in bulk crystals due to attenuation of the effective restoring forces acting on S atoms caused by vacancies in adjacent MoS₂layers. Consequently, the$A_{1g}$frequency of tri- and quadrilayer crystals is statistically invariant on account oft competition between phonon confinement effects and interlayer interactions. The$A_{1g}$linewidth is observed to decrease in bi- and trilayer crystals after low dose irradiation and is attributed to layer decoupling. This work shows that there is a complex interplay between defect production, crystal thickness and interlayer interactions in MoS₂. Our results demonstrate that ion irradiation is an effective tool to modulate the electronic, vibrational and structural properties of MoS₂, which may prove beneficial for practical applications.

    

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4. Anisotropic Properties of Quasi‐1D In 4 Se 3 : Mechanical Exfoliation, Electronic Transport, and Polarization‐Dependent Photoresponse

   https://doi.org/10.1002/adfm.202106459  

   Vorobeva, Nataliia S. ; Lipatov, Alexey ; Torres, Angel ; Dai, Jun ; Abourahma, Jehad ; Le, Duy ; Dhingra, Archit ; Gilbert, Simeon J. ; Galiy, Pavlo V. ; Nenchuk, Taras M. ; et al ( September 2021 , Advanced Functional Materials)

   Theoretical and experimental investigations of various exfoliated samples taken from layered In₄Se₃crystals are performed. In spite of the ionic character of interlayer interactions in In₄Se₃and hence much higher calculated cleavage energies compared to graphite, it is possible to produce few‐nanometer‐thick flakes of In₄Se₃by mechanical exfoliation of its bulk crystals. The In₄Se₃flakes exfoliated on Si/SiO₂have anisotropic electronic properties and exhibit field‐effect electron mobilities of about 50 cm² V⁻¹ s⁻¹at room temperature, which are comparable with other popular transition metal chalcogenide (TMC) electronic materials, such as MoS₂and TiS₃. In₄Se₃devices exhibit a visible range photoresponse on a timescale of less than 30 ms. The photoresponse depends on the polarization of the excitation light consistent with symmetry‐dependent band structure calculations for the most expectedaccleavage plane. These results demonstrate that mechanical exfoliation of layered ionic In₄Se₃crystals is possible, while the fast anisotropic photoresponse makes In₄Se₃a competitive electronic material, in the TMC family, for emerging optoelectronic device applications.

    

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5. Determining the twist angle of stacked MoS 2 layers using machine learning‐assisted low‐frequency interlayer Raman fingerprints

   https://doi.org/10.1002/jrs.6577  

   Tang, Jing ; Wang, Zifan ; Tan, Qishuo ; Cao, Jun ; Ling, Xi ( July 2023 , Journal of Raman Spectroscopy)

   The investigation of twisted stacked few‐layer MoS₂has revealed novel electronic, optical, and vibrational properties over an extended period. For the successful integration of twisted stacked few‐layer MoS₂into a wide range of applications, it is crucial to employ a noninvasive, versatile technique for characterizing the layered architecture of these complex structures. In this work, we introduce a machine learning‐assisted low‐frequency Raman spectroscopy method to characterize the twist angle of few‐layer stacked MoS₂samples. A feedforward neural network (FNN) is utilized to analyze the low‐frequency breathing mode as a function of the twist angle. Moreover, using finite difference method (FDM) and density functional theory (DFT) calculations, we show that the low‐frequency Raman spectra of MoS₂are mainly influenced by the effect of the nearest and second nearest layers. A new improved linear chain model (TA‐LCM) with taking the twist angle into the consideration is developed to understand the interlayer breathing modes of stacked few‐layer MoS₂. This approach can be extended to other 2D materials systems and provides an intelligent way to investigate naturally stacked and twisted interlayer interactions.

    

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