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Moléculas donantes-puentes-aceptantes de electrones con los radicales de nitróxido de nitronila: influencia de un

Erin T Chernick¹, Qixi Mi, Richard F Kelley

¹Department of Chemistry, Northwestern University, Evanston, Illinois 60208-3113, USA.

Journal of the American Chemical Society

|March 30, 2006

Resumen

La adición de radicales estables a los sistemas de donante-puente-aceptor controla la carga y la dinámica de giro. Un radical de nitróxido de nitronilo ralentizó la recombinación de carga en un trirrádico, a diferencia de los birrádicos, e indujo la polarización de espín.

Área de la Ciencia:

La fotoquímica y la fotofísica.
Química de espín La química de espín.
La electrónica molecular es la electrónica molecular.

Sus antecedentes:

Los sistemas de donante-puente-aceptor (D-B-A) son cruciales para el control de la carga y la transferencia de espín.
Los radicales estables ofrecen un medio para modular estas dinámicas dentro de las arquitecturas DBA.

Objetivo del estudio:

Investigar el efecto de la adición de un radical de nitróxido de nitronilo (NN*) estable a un sistema D-B-A en la dinámica de transferencia de carga y de giro.
Comprender cómo el radical NN* influye en los estados trirádicos fotogenerados y sus vías de recombinación.

Principales métodos:

Síntesis de un sistema D-B-A con un puente fenilo funcionalizado con p-metoxyanilina (MeOAn), 4-(N-piperidinyl) naftaleno-1,8-dicarboximida (6ANI), un nitróxido de nitronilo (NN *) y naftaleno-1,8:4,5-bis (dicarboximida) (NI).
Espectroscopia óptica de resolución temporal para monitorear la transferencia de carga y la recombinación.
Espectroscopia de resonancia paramagnética de electrones (EPR) para sondear la dinámica del espín y la polarización.

Principales resultados:

El radical NN* ralentizó significativamente la recombinación de carga en el estado trirrádico fotogenerado en comparación con los birrádicos análogos.
La interacción de intercambio de espín-espín entre el catión radical MeOAn y el anión radical NI no se vio afectada por NN*.
NN* aceleró el cruce intersistémico de pares de radicales e indujo una polarización de espín significativa en el producto de recombinación de carga, atribuido al acoplamiento antiferromagnético con un estado triple.

Conclusiones:

La adición de radicales estables como NN* proporciona una estrategia efectiva para controlar las tasas de recombinación de carga en los sistemas D-B-A.
La polarización de espín observada en NN* en el estado producto destaca una trayectoria única de la dinámica de espín impulsada por el acoplamiento con estados triplet.
Este estudio demuestra el potencial de la incorporación de radicales estables para la manipulación avanzada de espín en sistemas moleculares.

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