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      A photofunctional bottom-up bis(dipyrrinato)zinc(II) complex nanosheet

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          Abstract

          Two-dimensional polymeric nanosheets have recently gained much attention, particularly top-down nanosheets such as graphene and metal chalcogenides originating from bulk-layered mother materials. Although molecule-based bottom-up nanosheets manufactured directly from molecular components can exhibit greater structural diversity than top-down nanosheets, the bottom-up nanosheets reported thus far lack useful functionalities. Here we show the design and synthesis of a bottom-up nanosheet featuring a photoactive bis(dipyrrinato)zinc(II) complex motif. A liquid/liquid interfacial synthesis between a three-way dipyrrin ligand and zinc(II) ions results in a multi-layer nanosheet, whereas an air/liquid interfacial reaction produces a single-layer or few-layer nanosheet with domain sizes of >10 μm on one side. The bis(dipyrrinato)zinc(II) metal complex nanosheet is easy to deposit on various substrates using the Langmuir–Schäfer process. The nanosheet deposited on a transparent SnO 2 electrode functions as a photoanode in a photoelectric conversion system, and is thus the first photofunctional bottom-up nanosheet.

          Abstract

          The creation of functional 2D bottom-up nanosheets woven from molecular components remains a large challenge. Here, a bottom-up nanosheet featuring a photofunctional bis(dipyrrinato)zinc(II) complex motif is synthesized using interfacial syntheses, enabling a photoelectric conversion system.

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          Most cited references32

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          Electric Field Effect in Atomically Thin Carbon Films

          We report a naturally-occurring two-dimensional material (graphene that can be viewed as a gigantic flat fullerene molecule, describe its electronic properties and demonstrate all-metallic field-effect transistor, which uniquely exhibits ballistic transport at submicron distances even at room temperature.
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            Emerging photoluminescence in monolayer MoS2.

            Novel physical phenomena can emerge in low-dimensional nanomaterials. Bulk MoS(2), a prototypical metal dichalcogenide, is an indirect bandgap semiconductor with negligible photoluminescence. When the MoS(2) crystal is thinned to monolayer, however, a strong photoluminescence emerges, indicating an indirect to direct bandgap transition in this d-electron system. This observation shows that quantum confinement in layered d-electron materials like MoS(2) provides new opportunities for engineering the electronic structure of matter at the nanoscale.
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              Half-Metallic Graphene Nanoribbons

              Electrical current can be completely spin polarized in a class of materials known as half-metals, as a result of the coexistence of metallic nature for electrons with one spin orientation and insulating for electrons with the other. Such asymmetric electronic states for the different spins have been predicted for some ferromagnetic metals - for example, the Heusler compounds- and were first observed in a manganese perovskite. In view of the potential for use of this property in realizing spin-based electronics, substantial efforts have been made to search for half-metallic materials. However, organic materials have hardly been investigated in this context even though carbon-based nanostructures hold significant promise for future electronic device. Here we predict half-metallicity in nanometre-scale graphene ribbons by using first-principles calculations. We show that this phenomenon is realizable if in-plane homogeneous electric fields are applied across the zigzag-shaped edges of the graphene nanoribbons, and that their magnetic property can be controlled by the external electric fields. The results are not only of scientific interests in the interplay between electric fields and electronic spin degree of freedom in solids but may also open a new path to explore spintronics at nanometre scale, based on graphene.
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                Author and article information

                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Pub. Group
                2041-1723
                02 April 2015
                : 6
                : 6713
                Affiliations
                [1 ]Department of Chemistry, Graduate School of Science, The University of Tokyo , 7-3-1, Hongo, Bunkyo-ku, Tokyo 113-0033, Japan
                [2 ]Institute of Molecular Functional Materials, Department of Chemistry and Partner State Key Laboratory of Environmental and Biological Analysis, Hong Kong Baptist University , Waterloo Road, Hong Kong, China
                [3 ]Division of Chemical Engineering, Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University , 1-3, Machikaneyama, Toyonaka, Osaka 560-8531, Japan
                [4 ]Department of Chemistry, Graduate School of Science, Osaka University , 1-1, Machikaneyama, Toyonaka, Osaka 560-0043, Japan
                [5 ]HKBU Institute of Research and Continuing Education, Shenzhen Virtual University Park , Shenzhen 518057, China
                Author notes
                Article
                ncomms7713
                10.1038/ncomms7713
                4396372
                25831973
                2dd54ee3-115f-4858-a720-ab50e3fba6a6
                Copyright © 2015, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved.

                This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/

                History
                : 22 August 2014
                : 18 February 2015
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