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First Step Towards a Devil's Staircase in Spin-Crossover Materials.

Elzbieta Trzop1, Daopeng Zhang2,3, Lucia Piñeiro-Lopez2

  • 1Institut de Physique de Rennes, Université de Rennes 1, UMR UR1-CNRS 6251, 35000, Rennes, France.

Angewandte Chemie (International Ed. in English)
|May 20, 2016
PubMed
Summary
This summary is machine-generated.

This study reveals a unique spin-crossover phenomenon in a bimetallic coordination polymer, featuring multi-step transitions between high-spin (HS) and low-spin (LS) states. The material exhibits complex ordering of these spin states, forming periodic and aperiodic spin-state concentration waves.

Keywords:
Devil's staircaseaperiodicitycoordination polymersphase transitionsspin-crossover

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Area of Science:

  • Materials Science
  • Crystallography
  • Chemistry

Background:

  • Spin-crossover (SCO) materials exhibit transitions between high-spin (HS) and low-spin (LS) states, often triggered by external stimuli like temperature.
  • Coordination polymers offer tunable structures and properties, making them promising for advanced material applications.

Purpose of the Study:

  • To investigate the spin-crossover behavior of a novel bimetallic 2D coordination polymer, {Fe[(Hg(SCN)3 )2 ](4,4 ahydro-bipy)2 }n.
  • To characterize the multi-step spin-state transitions and the resulting ordering of HS and LS states.

Main Methods:

  • Synthesis and characterization of the bimetallic 2D coordination polymer.
  • Temperature-dependent measurements to study the spin-crossover phenomenon.
  • 4D superspace crystallography for structural refinement of spin-modulated phases.

Main Results:

  • The compound exhibits a staircase-like thermal spin-crossover with multiple steps in the HS molar fraction (γHS).
  • Two distinct ordering phenomena were observed: a periodic spin-state concentration wave (SSCW) at γHS ≈0.5 and an aperiodic SSCW at γHS ≈0.34.
  • The aperiodic SSCW shows a HS-LS sequence incommensurate with the molecular lattice.

Conclusions:

  • The observed multi-step spin-crossover and formation of spatially modulated phases are discussed in the context of "Devil's staircase" transitions.
  • This work highlights a unique manifestation of molecular HS/LS bistability leading to complex ordered structures.