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Spin–Spin Coupling: One-Bond Coupling01:17

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Coupling interactions are strongest between NMR-active nuclei bonded to each other, where spin information can be transmitted directly through the pair of bonding electrons. While nuclei polarize their electrons to the opposite spins, the bonding electron pair has opposite spins. Configurations with antiparallel nuclear spins are expected to be lower in energy. When coupling makes antiparallel states more favorable, J is considered to have a positive value. The one-bond coupling constant, 1J,...
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Two NMR-active nuclei bonded to a central atom can be involved in geminal or two-bond coupling. Geminal coupling is commonly seen between diastereotopic protons in chiral molecules and unsymmetrical alkenes, among others.
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Spin-Crossover Anticooperativity Induced by Weak Intermolecular Interactions.

Valentin V Novikov1, Ivan V Ananyev1, Alexander A Pavlov1

  • 1†Nesmeyanov Institute of Organoelement Compounds RAS Vavilova, 28, Moscow 119991, Russia.

The Journal of Physical Chemistry Letters
|August 16, 2015
PubMed
Summary
This summary is machine-generated.

Weak intermolecular interactions, like π···Cl, can disrupt cooperative spin-crossover (SCO) molecular switches. Analyzing crystal packing is crucial for designing effective SCO materials, challenging the broad applicability of "chemical pressure" concepts.

Keywords:
clathrochelatescobalt(II)cooperativitymacrocyclic compoundsmolecular switchesspin crossover

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Area of Science:

  • Materials Science
  • Supramolecular Chemistry
  • Solid-State Chemistry

Background:

  • Rational design of spin-crossover (SCO) molecular switches typically focuses on molecular building blocks.
  • Crystal packing and weak intermolecular interactions are often overlooked in SCO material design.
  • The
  • chemical pressure
  • concept is widely applied to explain SCO behavior.

Purpose of the Study:

  • To investigate the role of weak intermolecular interactions in the spin-crossover (SCO) behavior of cobalt(II) clathrochelates.
  • To determine if crystal packing influences SCO cooperativity, especially in molecules with constant volume.
  • To challenge the universality of the
  • chemical pressure
  • concept in SCO design.

Main Methods:

  • Synthesis and characterization of cobalt(II) clathrochelates.
  • Single-crystal X-ray diffraction to analyze crystal packing and intermolecular interactions.
  • Variable-temperature magnetic susceptibility measurements to study SCO behavior in solid state and solution.

Main Results:

  • Identified weak (1.2 kcal/mol) π···Cl intermolecular interactions in cobalt(II) clathrochelates.
  • Observed pronounced anticooperativity of SCO in the solid state, attributed to these weak interactions.
  • SCO behavior in the solid state was more gradual compared to solution, despite no change in molecular volume.

Conclusions:

  • Weak intermolecular interactions significantly impact SCO cooperativity, leading to anticooperativity.
  • Crystal packing analysis, including weak interactions, is essential for rational SCO molecular switch design.
  • The scope of the
  • chemical pressure
  • concept in SCO is limited, underscoring the importance of detailed intermolecular interaction studies.