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Altos rendimientos cuánticos de complejos de erbio binolado perfluorado y su luminiscencia polarizada circularmente
1Department of Chemistry, University of Connecticut, Storrs, Connecticut 06269, United States.
Journal of the American Chemical Society
|February 27, 2024
Resumen
Los investigadores desarrollaron nuevos complejos de erbio utilizando ligandos fluorados, logrando rendimientos cuánticos récord y brillo de luminiscencia polarizada circular (CPL) para su uso potencial en tecnologías de comunicación cuántica.
Área de la Ciencia:
- Ciencias de los materiales
- Química inorgánica
- La fotofísica
Sus antecedentes:
- Los complejos de erbio se investigan para aplicaciones luminiscentes.
- El logro de altos rendimientos cuánticos y la luminiscencia polarizada circular (CPL) es crucial para las tecnologías ópticas avanzadas.
- Las vías de desintegración no radiativas, como las vibraciones Csp2-H, a menudo limitan la eficiencia de la luminiscencia en los emisores moleculares.
Objetivo del estudio:
- Para sintetizar y caracterizar nuevos complejos de erbio tipo Shibasaki.
- Para mejorar el rendimiento cuántico y el brillo CPL mediante el uso de un ligando de Binol perfluorado (F12Binol).
- Explorar el impacto de los diferentes metales alcalinos en la esfera de coordinación secundaria en la estructura y las propiedades complejas.
Principales métodos:
- Síntesis de complejos de erbio tipo Shibasaki con el ligando F12Binol.
- Análisis espectroscópico que incluya RMN (19F, 7Li) y espectroscopia quiróptica.
- El rendimiento cuántico de la fotoluminiscencia y las mediciones de brillo CPL.
Principales resultados:
- Se han logrado rendimientos cuánticos récord (hasta el 11%) y brillo CPL (hasta 317 M-1 cm-1) para complejos moleculares de erbio.
- Demostró un aumento de 19 veces en el rendimiento cuántico y un aumento de 6 veces en el brillo CPL en comparación con los análogos no fluorados.
- Se observaron diferencias estructurales inesperadas basadas en el metal alcalino (K, Na, Li) en la esfera de coordinación secundaria.
- Se identificó que la fluoración total del ligando evita el apagado no radiativo de las vibraciones Csp2-H.
Conclusiones:
- Los complejos de erbio perfluorado tipo Shibasaki exhiben propiedades de luminiscencia sin precedentes.
- La fluoración de ligandos es una estrategia clave para superar el decaimiento no radiativo y mejorar la eficiencia de la luminiscencia.
- Estos hallazgos proporcionan principios de diseño para el desarrollo de emisores moleculares prácticos para la comunicación cuántica y otras aplicaciones ópticas avanzadas.
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