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Solid-State Spin Equilibrium of Ni(cyclam)2 Complex: Magnetostructural Correlations in Two Polymorphs.

Yoji Horii1, Yuki Kanegae1, Kiyonori Takahashi2

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Two nickel(II) complexes with cyclam ligands were studied. One polymorph exhibited a gradual spin transition, unlike the other, highlighting anisotropic interactions in octahedral nickel(II) complexes.

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Area of Science:

  • Coordination Chemistry
  • Materials Science
  • Magnetochemistry

Background:

  • Spin crossover (SCO) complexes, particularly iron(II)-based, are extensively studied for their potential applications.
  • Understanding the factors influencing spin transitions in other transition metal complexes is crucial for designing new materials.

Purpose of the Study:

  • To synthesize and characterize two crystal polymorphs of Ni(cyclam)I2.
  • To investigate the magnetic properties and spin transition behavior of these polymorphs.
  • To elucidate the nature of interactions governing spin equilibrium in octahedral nickel(II) complexes.

Main Methods:

  • Synthesis of two Ni(cyclam)I2 crystal polymorphs: trans-[Ni(cyclam)I2] (1a) and catena-[Ni(cyclam)(μ-I)]I (1b).
  • Temperature-dependent X-ray structural analysis.
  • Magnetic measurements (temperature-dependent).
  • Analysis using the spin-equilibrium model.

Main Results:

  • Polymorph 1a (molecular-crystal) displayed a gradual spin transition.
  • Polymorph 1b (zigzag-chain) did not show an obvious spin transition.
  • The entropy difference for spin transition in 1a was smaller than typical iron(II) SCO complexes.
  • Evidence for highly anisotropic interactions (z-elongation, x,y-shortening) in the coordination octahedron of Ni(II) was observed.

Conclusions:

  • The spin transition behavior is highly dependent on the crystal polymorph.
  • The spin transition in Ni(II) complexes is characterized by anisotropic coordination geometry changes.
  • The observed phenomenon provides insights into the design principles for novel spin-switching materials.