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Area of Science:

  • Solid-state chemistry
  • Coordination chemistry
  • Magnetochemistry

Background:

  • Investigates the heterospin complex [Cu(hfac)2L(Me/Et)], formed from copper(II) hexafluoroacetylacetonate [Cu(hfac)2] and a nitronyl nitroxide radical (L(Me/Et)).
  • Focuses on temperature-induced transformations in solid-state materials.

Purpose of the Study:

  • To elucidate the complex cascade of solid-state processes initiated by temperature variations in the [Cu(hfac)2L(Me/Et)] complex.
  • To characterize the structural and magnetic changes associated with cooling and heating cycles.

Main Methods:

  • Synthesis of the heterospin complex [Cu(hfac)2L(Me/Et)].
  • Variable-temperature magnetic susceptibility measurements (μeff(T)) to monitor spin transitions and structural changes.
  • Analysis of temperature-dependent depolymerization, pair formation, and spin crossover phenomena.

Main Results:

  • Cooling below 260 K induced depolymerization and formation of a pair heterospin complex: [Cu(hfac)2L(Me/Et)2][[Cu(hfac)2]3L(Me/Et)2].
  • Further cooling below 144 K resulted in a spin transition, decreasing the effective magnetic moment from 2.52 to 2.24 μB.
  • Heating reversed the process, with an increase in magnetic moment followed by polymer chain reformation, exhibiting two distinct hysteresis loops (high T: 283 K/260 K, low T: 161 K/144 K).

Conclusions:

  • The heterospin complex undergoes a cascade of reversible solid-state transformations driven by temperature.
  • Observed spin transitions and hysteresis loops are characteristic of cooperative structural changes in the solid state.
  • Model complexes confirm spin transitions in related polynuclear structures.