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Una nueva clase de sistemas de valencia mixta con centros redox orgánicos degenerados en órbita. Ejemplos basados en
Peter H Dinolfo1, Veaceslav Coropceanu, Jean-Luc Brédas
1Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.
Journal of the American Chemical Society
|September 28, 2006
Resumen
Este estudio explora las propiedades de valencia mixta centrada en ligandos (LCMV) en nuevos complejos de prisma supramoleculares. Los investigadores encontraron interacciones electrónicas únicas y redistribución de carga dentro de estos inusuales compuestos de valencia mixta (MV).
Área de la Ciencia:
- Química supramolecular de las moléculas.
- La electroquímica es electroquímica.
- Ciencia de los materiales Ciencia de los materiales.
Sus antecedentes:
- Los compuestos de valencia mixta (MV) exhiben propiedades electrónicas y ópticas interesantes.
- Los complejos supramoleculares ofrecen arquitecturas sintonizables para el estudio de los fenómenos de transferencia de electrones.
Objetivo del estudio:
- Investigar las propiedades de valencia mixta centrada en ligandos (LCMV) de dos nuevos complejos supramoleculares de prisma triangular.
- Caracterizar la estructura electrónica y la distribución de la carga en estos inusuales sistemas MV.
Principales métodos:
- Voltametría cíclica para estudiar el comportamiento redox de los ligandos puentes.
- La electroabsorción (espectroscopia de Stark) para sondear las transiciones electrónicas.
- Cálculos de la Teoría Funcional de Densidad (DFT) para el análisis de la estructura electrónica.
Principales resultados:
- Los ligandos de tri-(4-piridil)-1,3,5-triazina (tPyTz) accesibles por redox se someten a reducciones secuenciales de un electrón.
- Los prismas reducidos individuales exhiben intensas bandas de transferencia de intervalos (IT) de infrarrojo cercano (NIR), lo que indica un fuerte acoplamiento electrónico.
- Las mediciones de electroabsorción revelan pequeños cambios de momento dipolo y vectores de momento dipolo de transición no colineal.
- Los cálculos de DFT apoyan un mecanismo de interacción electrónica a través del espacio y el levantamiento de degeneración orbital en formas de MV.
Conclusiones:
- Los prismas supramoleculares estudiados representan una clase inusual de compuestos MV donde los ligandos tPyTz actúan como centros redox.
- La excitación óptica de TI conduce a una redistribución de carga no simétrica debido a la degeneración orbital levantada.
- Estos hallazgos proporcionan información sobre el comportamiento electrónico de los sistemas MV supramoleculares complejos.
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