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Isomerism in Complexes
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Polymorphism and Thermally Induced Structural Transformation in Semiconducting Cd(II) Coordination Polymers.

Ryohei Akiyoshi1, Honoka Motokawa1, Asuka Nishibe1

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Three semiconducting coordination polymer polymorphs were studied. Thermal treatment induced a structural transformation in KGF-79, creating a polar structure with second harmonic generation activity and photoconductivity.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Crystallography

Background:

  • Semiconducting coordination polymers offer tunable electronic and optical properties.
  • Polymorphism in [Cd(2-SNPh)2]n, a cadmium(II)-thiolate coordination polymer, influences structural and functional characteristics.
  • Understanding structure-property relationships is crucial for developing advanced materials.

Purpose of the Study:

  • To investigate the structural diversity and properties of three polymorphs of a cadmium(II)-thiolate coordination polymer, [Cd(2-SNPh)2]n.
  • To elucidate the mechanism of thermally induced structural transformation and its impact on material properties.
  • To explore the photoconductive behavior and charge transport mechanisms in these materials.

Main Methods:

  • Single-crystal X-ray structural analysis to determine the atomic arrangement of KGF-51 and KGF-71.
  • Microcrystal electron diffraction analysis to characterize the 1D triple-strand structure of KGF-79.
  • Time-resolved microwave conductivity measurements to assess photoconductivity.
  • First-principles calculations to understand charge transport mechanisms.

Main Results:

  • KGF-51 exhibits a 1D single-strand ladder chain structure.
  • KGF-71 displays a 1D double-strand chain structure stabilized by S···S interactions.
  • Thermal treatment of KGF-51 and KGF-71 yields KGF-79, a 1D triple-strand chain structure with enhanced S···S interactions.
  • KGF-79 shows a transition from nonpolar to polar structure, resulting in second harmonic generation (SHG) activity.
  • All three polymorphs demonstrate photoconductivity attributed to charge transport along (-Cd-S-)n chains via hopping.

Conclusions:

  • The study reveals three distinct polymorphs of a cadmium(II)-thiolate coordination polymer with varying dimensionality and structural motifs.
  • Thermally induced, irreversible transformation leads to a polar structure (KGF-79) with emergent SHG properties.
  • The inorganic (-Cd-S-)n chains are key pathways for charge transport, enabling photoconductivity in all polymorphs through a hopping mechanism.