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NMR-active nuclei have energy levels called 'spin states' that are associated with the orientations of their nuclear magnetic moments. In the absence of a magnetic field, the nuclear magnetic moments are randomly oriented, and the spin states are degenerate. When an external magnetic field is applied, the spin states have only 2 + 1 orientations available to them. A proton with = ½ has two available orientations. Similarly, for a quadrupolar nucleus with a nuclear spin value of one, the...
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The spin state of an NMR-active nucleus can have a slight effect on its immediate electronic environment. This effect propagates through the intervening bonds and affects the electronic environments of NMR-active nuclei up to three bonds away; occasionally, even farther. This phenomenon is called spin–spin coupling or J-coupling. Coupling interactions are mutual and result in small changes in the absorption frequencies of both nuclei involved. While nuclei of the same element are involved...
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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 systems where the difference in chemical shifts of the coupled nuclei is greater than ten times J are called first-order spin systems. These nuclei are weakly coupled, and their chemical shifts and coupling constant can generally be estimated from the well-separated signals in the spectrum.
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Vicinal or three-bond coupling is commonly observed between protons attached to adjacent carbons. Here, nuclear spin information is primarily transferred via electron spin interactions between adjacent C‑H bond orbitals. This generally favors the antiparallel arrangement of spins, so 3J values are usually positive.
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Long-range spin dependent delocalization promoted by the pseudo Jahn-Teller effect.

Benjamin W Stein1, Diane A Dickie1, Sachin Nedungadi2

  • 1Department of Chemistry and Chemical Biology, The University of New Mexico, MSC03 2060, 1 University of New Mexico, Albuquerque, New Mexico 87131-0001, USA.

The Journal of Chemical Physics
|November 30, 2019
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Summary

This study demonstrates ferromagnetic coupling of localized verdazyl radical spins, similar to previous findings with nitronylnitroxide radicals. This magnetic exchange originates from a second-order vibronic effect in a specific ruthenium complex.

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Area of Science:

  • Coordination Chemistry
  • Magnetochemistry
  • Materials Science

Background:

  • Previous work established strong spin-dependent delocalization (double exchange) in nitronylnitroxide-cobalt-catecholate complexes.
  • Ferromagnetic alignment of nitronylnitroxide spins was observed in mixed-valent SQ-Co(iii)-Cat triads.

Purpose of the Study:

  • To investigate ferromagnetic coupling of localized verdazyl (Vdz) radical spins.
  • To elucidate the mechanism of magnetic exchange in a new class of molecular complexes.

Main Methods:

  • Synthesis and characterization of [Vdz-diox-Ru(py)2-diox-Vdz]0 complexes.
  • Magnetic susceptibility measurements to probe spin interactions.
  • Theoretical analysis to understand the origin of magnetic exchange.

Main Results:

  • Ferromagnetic coupling of localized verdazyl radical spins was successfully achieved.
  • The [diox-Ru-diox]0 triad was found to be diamagnetic due to strong antiferromagnetic SQ-Ru(iii) exchange.
  • The observed magnetic exchange arises from a second-order vibronic effect (pseudo Jahn-Teller effect).

Conclusions:

  • Ferromagnetic coupling can be extended to verdazyl radical systems.
  • Vibronic effects play a crucial role in mediating magnetic interactions in these molecular systems.
  • The findings contribute to the design of novel magnetic materials with tailored spin properties.