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Transferencia de electrones fotoinducida en un complejo de transferencia de carga formado entre el corannuleno y

Mihoko Yamada¹, Kei Ohkubo, Mitsuhiko Shionoya

¹Department of Material and Life Science, Graduate School of Engineering, Osaka University, ALCA, Japan Science and Technology (JST) , Suita, Osaka 565-0871, Japan.

Journal of the American Chemical Society

|August 29, 2014

Resumen

Un complejo de transferencia de carga formado entre el corannuleno y el Li(+) @C60 exhibe estados separados por carga triplet de larga duración. Estos estados, cruciales para la comprensión de la dinámica de transferencia de electrones, decaen lentamente debido a procesos de espín prohibido.

Área de la Ciencia:

Química supramolecular de las moléculas.
La fotoquímica es la fotoquímica.
Ciencia de los materiales Ciencia de los materiales.

Sus antecedentes:

El coranuleno y el Li(+) @C60 forman complejos de transferencia de carga a través de interacciones π-π.
Comprender la dinámica del estado excitado y la transferencia de electrones es clave en la ciencia de los materiales.

Objetivo del estudio:

Investigar la formación y las propiedades de un complejo de transferencia de carga entre el corannuleno y el Li(+)@C60.
Para caracterizar los estados separados de carga singlet y triplet generados tras la excitación.
Para determinar los factores que influyen en la vida útil del estado triple de carga separada.

Principales métodos:

Formación del complejo de transferencia de carga en el benzonitrilo.
Excitación láser de femtosegundos y nanosegundos.
Espectroscopia de resonancia paramagnética de electrones (EPR) a 4 K. Espectroscopia de resonancia paramagnética de electrones (EPR) a 4 K. Espectroscopia de resonancia paramagnética de electrones (EPR) a 4 K. Espectroscopia de resonancia paramagnética de electrones (EPR) a 4 K. Espectroscopia de resonancia paramagnética de electrones (EPR) a 4 K. Espectroscopia de resonancia paramagnética de electrones (EPR) a 4 K. Espectroscopia de resonancia paramagnética de electrones (EPR) a 4 K.
Mediciones de velocidad constante dependientes de la temperatura.

Principales resultados:

Se formó un complejo estable de transferencia de carga con una constante de unión de 1,9 × 10 M-1.
Se observó una vida útil del estado separado por carga única de 1,4 ns.
Triplet estado de carga separada generado con una vida útil de 240 μs.
Distancia de espín del electrón de 10 Å determinada para el estado triple.
Energía de reorganización (λ = 1.04 eV) y acoplamiento electrónico (V = 0.0080 cm−1) cuantificado.

Conclusiones:

El complejo de corannulene/Li(+) @C60 exhibe una separación de carga eficiente.
La larga vida útil del estado triple de carga separada se atribuye a la transferencia de electrones inversa de espín prohibido y el acoplamiento electrónico pequeño.
Este estudio proporciona información sobre los estados de carga separada de larga duración relevantes para la electrónica molecular y la conversión de energía.

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