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        Multifunctional Two-Dimensional PtSe<sub>2</sub>-Layer Kirigami Conductors with 2000% Stretchability and Metallic-to-Semiconducting Tunability

        Okogbue, Emmanuel,Han, Sang Sub,Ko, Tae-Jun,Chung, Hee-Suk,Ma, Jinwoo,Shawkat, Mashiyat Sumaiya,Kim, Jung Han,Kim, Jong Hun,Ji, Eunji,Oh, Kyu Hwan,Zhai, Lei,Lee, Gwan-Hyoung,Jung, Yeonwoong American Chemical Society 2019 NANO LETTERS Vol.19 No.11

        <P>Two-dimensional transition-metal dichalcogenide (2D TMD) layers are highly attractive for emerging stretchable and foldable electronics owing to their extremely small thickness coupled with extraordinary electrical and optical properties. Although intrinsically large strain limits are projected in them (i.e., several times greater than silicon), integrating 2D TMDs in their pristine forms does not realize superior mechanical tolerance greatly demanded in high-end stretchable and foldable devices of unconventional form factors. In this article, we report a versatile and rational strategy to convert 2D TMDs of limited mechanical tolerance to tailored 3D structures with extremely large mechanical stretchability accompanying well-preserved electrical integrity and modulated transport properties. We employed a concept of strain engineering inspired by an ancient paper-cutting art, known as kirigami patterning, and developed 2D TMD-based kirigami electrical conductors. Specifically, we directly integrated 2D platinum diselenide (2D PtSe<SUB>2</SUB>) layers of controlled carrier transport characteristics on mechanically flexible polyimide (PI) substrates by taking advantage of their low synthesis temperature. The metallic 2D PtSe<SUB>2</SUB>/PI kirigami patterns of optimized dimensions exhibit an extremely large stretchability of ∼2000% without compromising their intrinsic electrical conductance. They also present strain-tunable and reversible photoresponsiveness when interfaced with semiconducting carbon nanotubes (CNTs), benefiting from the formation of 2D PtSe<SUB>2</SUB>/CNT Schottky junctions. Moreover, kirigami field-effect transistors (FETs) employing semiconducting 2D PtSe<SUB>2</SUB> layers exhibit tunable gate responses coupled with mechanical stretching upon electrolyte gating. The exclusive role of the kirigami pattern parameters in the resulting mechanoelectrical responses was also verified by a finite-element modeling (FEM) simulation. These multifunctional 2D materials in unconventional yet tailored 3D forms are believed to offer vast opportunities for emerging electronics and optoelectronics.</P> [FIG OMISSION]</BR>

      • Centimeter-Scale Periodically Corrugated Few-Layer 2D MoS<sub>2</sub> with Tensile Stretch-Driven Tunable Multifunctionalities

        Okogbue, Emmanuel,Kim, Jung Han,Ko, Tae-Jun,Chung, Hee-Suk,Krishnaprasad, Adithi,Flores, Jean Calderon,Nehate, Shraddha,Kaium, Md Golam,Park, Jong Bae,Lee, Sei-Jin,Sundaram, Kalpathy B.,Zhai, Lei,Roy, American Chemical Society 2018 ACS APPLIED MATERIALS & INTERFACES Vol.10 No.36

        <P>Two-dimensional (2D) transition metal dichalcogenide (TMD) layers exhibit superior optical, electrical, and structural properties unattainable in any traditional materials. Many of these properties are known to be controllable via external mechanical inputs, benefiting from their extremely small thickness coupled with large in-plane strain limits. However, realization of such mechanically driven tunability often demands highly complicated engineering of 2D TMD layer structures, which is difficult to achieve on a large wafer scale in a controlled manner. Herein, we explore centimeter-scale periodically corrugated 2D TMDs, particularly 2D molybdenum disulfide (MoS<SUB>2</SUB>), and report their mechanically tunable multifunctionalities. We developed a water-assisted process to homogeneously integrate few layers of 2D MoS<SUB>2</SUB> on three-dimensionally corrugated elastomeric substrates on a large area (>2 cm<SUP>2</SUP>). The evolution of electrical, optical, and structural properties in these three-dimensionally corrugated 2D MoS<SUB>2</SUB> layers was systematically studied under controlled tensile stretch. We identified that they present excellent electrical conductivity and photoresponsiveness as well as systematically tunable surface wettability and optical absorbance even under significant mechanical deformation. These novel three-dimensionally structured 2D materials are believed to offer exciting opportunities for large-scale, mechanically deformable devices of various form factors and unprecedented multifunctionalities.</P> [FIG OMISSION]</BR>

      • Horizontal-to-Vertical Transition of 2D Layer Orientation in Low-Temperature Chemical Vapor Deposition-Grown PtSe<sub>2</sub> and Its Influences on Electrical Properties and Device Applications

        Han, Sang Sub,Kim, Jong Hun,Noh, Chanwoo,Kim, Jung Han,Ji, Eunji,Kwon, Junyoung,Yu, Seung Min,Ko, Tae-Jun,Okogbue, Emmanuel,Oh, Kyu Hwan,Chung, Hee-Suk,Jung, YounJoon,Lee, Gwan-Hyoung,Jung, Yeonwoong American Chemical Society 2019 ACS APPLIED MATERIALS & INTERFACES Vol.11 No.14

        <P>Two-dimensional (2D) transition-metal dichalcogenides (2D TMDs) in the form of MX<SUB>2</SUB> (M: transition metal, X: chalcogen) exhibit intrinsically anisotropic layered crystallinity wherein their material properties are determined by constituting M and X elements. 2D platinum diselenide (2D PtSe<SUB>2</SUB>) is a relatively unexplored class of 2D TMDs with noble-metal Pt as M, offering distinct advantages over conventional 2D TMDs such as higher carrier mobility and lower growth temperatures. Despite the projected promise, much of its fundamental structural and electrical properties and their interrelation have not been clarified, and so its full technological potential remains mostly unexplored. In this work, we investigate the structural evolution of large-area chemical vapor deposition (CVD)-grown 2D PtSe<SUB>2</SUB> layers of tailored morphology and clarify its influence on resulting electrical properties. Specifically, we unveil the coupled transition of structural-electrical properties in 2D PtSe<SUB>2</SUB> layers grown at a low temperature (i.e., 400 °C). The layer orientation of 2D PtSe<SUB>2</SUB> grown by the CVD selenization of seed Pt films exhibits horizontal-to-vertical transition with increasing Pt thickness. While vertically aligned 2D PtSe<SUB>2</SUB> layers present metallic transports, field-effect-transistor gate responses were observed with thin horizontally aligned 2D PtSe<SUB>2</SUB> layers prepared with Pt of small thickness. Density functional theory calculation identifies the electronic structures of 2D PtSe<SUB>2</SUB> layers undergoing the transition of horizontal-to-vertical layer orientation, further confirming the presence of this uniquely coupled structural-electrical transition. The advantage of low-temperature growth was further demonstrated by directly growing 2D PtSe<SUB>2</SUB> layers of controlled orientation on polyimide polymeric substrates and fabricating their Kirigami structures, further strengthening the application potential of this material. Discussions on the growth mechanism behind the horizontal-to-vertical 2D layer transition are also presented.</P> [FIG OMISSION]</BR>

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