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Free, publicly-accessible full text available April 12, 2024
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Abstract The phase transitions of two-dimensional (2D) materials are key to the operation of many devices with applications including energy storage and low power electronics. Nanoscale confinement in the form of reduced thickness can modulate the phase transitions of 2D materials both in their thermodynamics and kinetics. Here, using in situ Raman spectroscopy we demonstrate that reducing the thickness of MoS 2 below five layers slows the kinetics of the phase transition from 2H- to 1T′-MoS 2 induced by the electrochemical intercalation of lithium. We observe that the growth rate of 1T′ domains is suppressed in thin MoS 2 supported by SiO 2 , and attribute this growth suppression to increased interfacial effects as the thickness is reduced below 5 nm. The suppressed kinetics can be reversed by placing MoS 2 on a 2D hexagonal boron nitride ( h BN) support, which readily facilitates the release of strain induced by the phase transition. Additionally, we show that the irreversible conversion of intercalated 1T′-MoS 2 into Li 2 S and Mo is also thickness-dependent and the stability of 1T′-MoS 2 is significantly increased below five layers, requiring a much higher applied electrochemical potential to break down 1T′-MoS 2 into Li 2 S and Mo nanoclusters.more » « less
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null (Ed.)Two-dimensional (2D) transition metal dichalcogenide (TMD) layers have gained increasing attention for a variety of emerging electrical, thermal, and optical applications. Recently developed metallic 2D TMD layers have been projected to exhibit unique attributes unattainable in their semiconducting counterparts; e.g. , much higher electrical and thermal conductivities coupled with mechanical flexibility. In this work, we explored 2D platinum ditelluride (2D PtTe 2 ) layers – a relatively new class of metallic 2D TMDs – by studying their previously unexplored electro-thermal properties for unconventional window applications. We prepared wafer-scale 2D PtTe 2 layer-coated optically transparent and mechanically flexible willow glasses via a thermally-assisted tellurization of Pt films at a low temperature of 400 °C. The 2D PtTe 2 layer-coated windows exhibited a thickness-dependent optical transparency and electrical conductivity of >10 6 S m −1 – higher than most of the previously explored 2D TMDs. Upon the application of electrical bias, these windows displayed a significant increase in temperature driven by Joule heating as confirmed by the infrared (IR) imaging characterization. Such superior electro-thermal conversion efficiencies inherent to 2D PtTe 2 layers were utilized to demonstrate various applications, including thermochromic displays and electrically-driven defogging windows accompanying mechanical flexibility. Comparisons of these performances confirm the superiority of the wafer-scale 2D PtTe 2 layers over other nanomaterials explored for such applications.more » « less
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Modern electronics have been geared toward exploring novel electronic materials that can encompass a broad set of unusual functionalities absent in conventional platforms. In this regard, two-dimensional (2D) transition metal dichalcogenide (TMD) semiconductors are highly promising, owing to their large mechanical resilience coupled with superior transport properties and van der Waals (vdW) attraction-enabled relaxed assembly. Moreover, 2D TMD heterolayers based on chemically distinct constituent layers exhibit even more intriguing properties beyond their mono-component counterparts, which can materialize only when they are manufactured on a technologically practical wafer-scale. This mini-review provides a comprehensive overview of recent progress in exploring wafer-scale 2D TMD heterolayers of various kinds. It extensively surveys a variety of manufacturing strategies and discusses their scientific working principles, resulting 2D TMD heterolayers, their material properties, and device applications. Moreover, it offers extended discussion on remaining challenges and future outlooks toward further improving the material quality of 2D TMD heterolayers in both material and manufacturing aspects.more » « less
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Intercalation of alkali metals is widely studied to introduce a structural phase transition from 2H to 1T′ in 2D group VI transition metal dichalcogenides (TMDCs). This highly efficient phase transition method has enabled an access to a library of phases with novel physical and chemical properties attractive for functional devices and electrochemical catalysis. However, despite numerous studies that have predicted that charge doping mainly contributes to the structural phase transition in the intercalation process, a mechanistic understanding of the phase transition at the atomic level has not been fully revealed. Furthermore, the coupled effects of strain and other intrinsic or extrinsic factors on the intercalation‐induced phase transition have not been quantitatively determined. Herein, the progress of the intercalation‐induced phase transition is briefly overviewed and the knowledge gaps in the current understanding of phase transition and intercalation in 2D TMDCs are highlighted. To fully gain the microscopic picture of the intercalation‐induced phase transition, in situ multimodal probes to monitor the real‐time structure−property relationship during intercalation are suggested. The proposed research directions further direct material scientists to efficiently engineer phase transition pathways in 2D materials to explore novel functional phases.