Advanced Materials

Modulation of Third-Order Nonlinear Optical Properties by Backbone Modification of Polymeric Pillared-Layer Heterometallic Clusters

Authors

  • Chi Zhang,

    Corresponding author
    1. Research Center for Advanced Molecular Materials School of Chemistry and Chemical Engineering Scientific Research Academy Jiangsu University Zhenjiang 212013 (P.R. China)
    2. Institute of Molecular Engineering and Advanced Materials School of Chemical Engineering Nanjing University of Science and Technology Nanjing 210094 (P.R. China)
    • Research Center for Advanced Molecular Materials School of Chemistry and Chemical Engineering Scientific Research Academy Jiangsu University Zhenjiang 212013 (P.R. China).
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  • Yuan Cao,

    1. Institute of Molecular Engineering and Advanced Materials School of Chemical Engineering Nanjing University of Science and Technology Nanjing 210094 (P.R. China)
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  • Jinfang Zhang,

    1. Research Center for Advanced Molecular Materials School of Chemistry and Chemical Engineering Scientific Research Academy Jiangsu University Zhenjiang 212013 (P.R. China)
    2. Institute of Molecular Engineering and Advanced Materials School of Chemical Engineering Nanjing University of Science and Technology Nanjing 210094 (P.R. China)
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  • Suci Meng,

    1. Institute of Theoretical and Computational Chemistry School of Chemistry and Chemical Engineering Nanjing University Nanjing 210093 (P.R. China)
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  • Tsuyoshi Matsumoto,

    1. Research Center for Materials Science Department of Chemistry, Graduate School of Science Nagoya University Nagoya 464-8602 (Japan)
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  • Yinglin Song,

    1. National Special Laboratory of Nonlinear Optics and Information Processing Department of Applied Physics Harbin Institute of Technology Harbin 150001 (P.R. China)
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  • Jing Ma,

    1. Institute of Theoretical and Computational Chemistry School of Chemistry and Chemical Engineering Nanjing University Nanjing 210093 (P.R. China)
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  • Zhaoxu Chen,

    1. Institute of Theoretical and Computational Chemistry School of Chemistry and Chemical Engineering Nanjing University Nanjing 210093 (P.R. China)
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  • Kazuyuki Tatsumi,

    1. Research Center for Materials Science Department of Chemistry, Graduate School of Science Nagoya University Nagoya 464-8602 (Japan)
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  • Mark G. Humphrey

    Corresponding author
    1. Department of Chemistry Australian National University Canberra, ACT 0200 (Australia)
    • Department of Chemistry Australian National University Canberra, ACT 0200 (Australia).
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  • This research was financially supported by the National Natural Science Foundation of China (No. 50472048), the Program for New Century Excellent Talents in University (NCET-05-0499), the Foundation of UJS, NUST, and HIT. M.G.H. is an Australian Research Council (ARC) Australian Professorial Fellow. Supporting information for this article is available online from Wiley InterScience or from the author.

Abstract

Three polymeric heterothiometallic clusters with 3D pillar-layer-alternating honeycomblike frameworks are synthesized by a one-pot self-assembly reaction. Z-scan experiments demonstrate that the nonlinear optical (NLO) behavior of these clusters can be modulated by modifying the conjugated chain of the connecting backbone ligands (see figure). Time-dependent density functional theory calculations support and rationalize the observed NLO modulation.

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