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When atoms or molecules absorb light at the proper frequency, their electrons are excited to higher-energy orbitals. For many main group atoms and molecules, the absorbed photons are in the ultraviolet range of the electromagnetic spectrum, which cannot be detected by the human eye. For coordination compounds, the energy difference between the d orbitals often allows photons in the visible range to be absorbed and emitted, which is seen as colors by the human...
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Chain-growth or addition polymerization is successive addition reactions of monomers with a polymer chain. In radical chain-growth polymerization, the reaction proceeds via a free-radical intermediate. The free radical is formed from radical initiators, which spontaneously generate free radicals by homolytic fission. Organic peroxides (such as dibenzoyl peroxide, as shown in Figure 1) or azo compounds are popular radical initiators. A low concentration ratio of radical initiator to monomer is...
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Radicals adjacent to electron-donating groups are called nucleophilic radicals. These radicals readily react with electrophilic alkenes. The SOMO–LUMO interactions are the driving force for the reaction, where the high-energy SOMO of the electron-rich, nucleophilic radicals interacts with the low-energy LUMO of the electron-deficient, electrophilic alkenes. Such SOMO–LUMO interactions are the basis of reactive radical traps, affecting the selectivity in radical reactions. For...
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The radical chain-growth polymerization mechanism consists of three steps: initiation, propagation, and termination of polymerization. The polymerization initiates when a free radical generated from the radical initiator adds to the unsaturated bond in the monomer. The unpaired electron of the free radical and one π electron in the unsaturated bond creates a σ bond between the free radical and the monomer. As a result, the other π electron in the unsaturated bond converts this species into...
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Coordination compounds and complexes exhibit different colors, geometries, and magnetic behavior, depending on the metal atom/ion and ligands from which they are composed. In an attempt to explain the bonding and structure of coordination complexes, Linus Pauling proposed the valence bond theory, or VBT, using the concepts of hybridization and the overlapping of the atomic orbitals. According to VBT, the central metal atom or ion (Lewis acid) hybridizes to provide empty orbitals of suitable...
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Polímeros de coordinación basados en radicales como una plataforma para la magnetoluminiscencia

Shun Kimura1,2, Ryota Matsuoka1,3, Shojiro Kimura4

  • 1Institute for Molecular Science, 5-1 Higashiyama, Myodaiji, Okazaki, Aichi 444-8787, Japan.

Journal of the American Chemical Society
|April 7, 2021
PubMed
Resumen

Los investigadores desarrollaron un nuevo método para la magnetoluminiscencia radical utilizando polímeros de coordinación. Estos materiales muestran cambios significativos en la luminiscencia bajo campos magnéticos, a diferencia de los radicales dispersos.

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Área de la Ciencia:

  • Ciencias de los materiales
  • Química orgánica
  • Física del estado sólido

Sus antecedentes:

  • Los radicales orgánicos poseen propiedades electrónicas y magnéticas únicas relacionadas con el espín.
  • Las propiedades de luminiscencia que surgen de las interacciones de espín en los radicales orgánicos rara vez se informan.
  • La magnetoluminiscencia, el efecto de los campos magnéticos sobre la luminiscencia, se ha observado principalmente en los radicales dispersos en las matrices de acogida.

Objetivo del estudio:

  • Informar sobre un nuevo método para lograr la magnetoluminiscencia radical en polímeros de coordinación basados en radicales (PC).
  • Investigar las propiedades de luminiscencia de los radicales orgánicos específicos (bisPyTM y trisPyM) y sus Zn(II) CPs.
  • Explorar la influencia de los campos magnéticos externos en la luminiscencia de estos PC basados en radicales.

Principales métodos:

  • Síntesis y caracterización de polímeros de coordinación basados en radicales (PC) mediante el uso de radicales bis ((3,5-dicloro-4-piridil) ((2,4,6-triclorofenil) metilo (bisPyTM) y tris ((3,5-dicloro-4-piridil) metilo (trisPyM).
  • Investigación de las propiedades de luminiscencia en estado sólido a bajas temperaturas (4,2 K).
  • Análisis de las estructuras cristalinas, las propiedades magnéticas y la magnetoluminiscencia dependiente de la temperatura y el tiempo.

Principales resultados:

  • Las emisiones en estado sólido de los radicales bisPyTM y trisPyM no se vieron afectadas significativamente por los campos magnéticos externos a 4,2 K.
  • La luminiscencia de los PC basados en radicales fue modulada en gran medida por campos magnéticos externos.
  • Los estudios sugieren que la reducción de las interacciones radical-radical dentro de los PC es crucial para lograr la magnetoluminiscencia.

Conclusiones:

  • Los polímeros de coordinación basados en radicales ofrecen una nueva plataforma para observar la magnetoluminiscencia radical.
  • La modulación de la luminiscencia por los campos magnéticos en CPs es significativamente mayor que en los radicales dispersos.
  • Minimizar las interacciones radical-radical es una estrategia clave para desarrollar materiales con propiedades de magnetoluminiscencia sintonizables.