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Area of Science:

  • Materials Science
  • Supramolecular Chemistry
  • Crystallography

Background:

  • Integrating electronic switching with molecular machinery is crucial for developing stimuli-responsive materials.
  • Spin crossover (SCO) materials offer tunable electronic properties based on external stimuli.
  • Molecular motion within crystal lattices can lead to macroscopic material responses.

Purpose of the Study:

  • To demonstrate a synergistic coupling of spin crossover (SCO) and molecular motion.
  • To construct a hydrogen-bonded supramolecular architecture exhibiting cooperative electronic and molecular structural changes.
  • To explore the potential for creating multifunctional dynamic crystals with unique responses.

Main Methods:

  • Synthesized a supramolecular architecture using spin-active [Fe(3-bpp)2]2+ complexes and flexible bpa molecules.
  • Investigated temperature-induced spin conversion and its mechanical association with bpa conformational changes.
  • Analyzed the resulting phase transition, lattice deformation, thermosalient effect, and pyroelectric response.

Main Results:

  • Achieved a synergistic coupling between temperature-induced spin conversion and large-amplitude molecular motion (pedal-like conformational change of bpa).
  • Observed a diffusionless martensitic phase transition with anisotropic lattice deformation, leading to a thermosalient effect (crystal jumping).
  • Demonstrated that bpa conformational changes induce counteranion displacement, modulating lattice polarization and resulting in a pyroelectric response.

Conclusions:

  • Established a rational design strategy for bridging electronic switching and molecular mechanics in dynamic crystals.
  • Showcased a material exhibiting cooperative electronic and molecular structural evolution, leading to macroscopic mechanical motion and electrical output.
  • Paved the way for sophisticated multifunctional dynamic crystals by linking SCO and molecular mechanics.