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Transferencia de electrones acoplados al cobre en nanocristales de sulfuro de cobre coloidales probados por

Kimberly H Hartstein¹, Carl K Brozek¹, Stijn O M Hinterding¹

¹Department of Chemistry , University of Washington , Seattle , Washington 98195-1700 , United States.

Journal of the American Chemical Society

|February 21, 2018

Resumen

Los nanocristales de sulfuro de cobre exhiben resonancias plasmónicas de superficie localizadas sintonizables (LSPR) a través de un dopaje controlado. Los estudios espectroelectroquímicos revelan que las vacantes catiónicas son clave para estabilizar los portadores de carga, lo que permite la conmutación reversible de LSPR para aplicaciones plasmónicas avanzadas.

Área de la Ciencia:

Ciencias de los materiales
Nanotecnología
Química Física

Sus antecedentes:

Los nanocristales de sulfuro de cobre soportan agujeros deslocalizados, lo que permite resonancias plasmónicas de superficie localizadas (LSPR) para aplicaciones infrarrojas.
El control de la forma, la composición y los portadores de carga del nanocristal es crucial para afinar las propiedades plasmónicas.
Comprender las transformaciones químicas de los semiconductores intrínsecos a los dopados es vital para el avance tecnológico.

Objetivo del estudio:

Para sondear cuantitativamente las energías de nivel de Fermi (E_F) en nanocristales de sulfuro de cobre durante las reacciones redox.
Para aclarar los procesos químicos microscópicos que rigen la conmutación LSPR.
Proporcionar conocimientos termodinámicos fundamentales sobre la generación de plasmones en nanoestructuras de semiconductores.

Principales métodos:

Aplicación de la potencialometría espectroelectroquímica como una sonda in situ.
Investigación de las reacciones redox para controlar la presencia y la posición de la banda LSPR.
Análisis de la estructura cristalina y los mecanismos de estabilización del portador de carga.

Principales resultados:

Se han demostrado bandas de LSPR espectroscópicamente indistinguibles en nanocristales de sulfuro de cobre con y sin vacíos catiónicos.
Se ha identificado que las vacantes catiónicas son más eficaces que los aniones superficiales para estabilizar el exceso de portadores libres.
Se observó la apariencia reversible de la banda LSPR, el desplazamiento E_F y los cambios en la estructura cristalina durante la oxidación y reducción.

Conclusiones:

El cambio de LSPR en los nanocristales de sulfuro de cobre es reversible y está relacionado con la formación de vacíos catiónicos y los desplazamientos a nivel de Fermi.
Las vacantes de cationes juegan un papel fundamental en la estabilización de los portadores libres y permiten la sintonización plasmónica.
El estudio proporciona datos termodinámicos cuantitativos para el diseño de sistemas de generación de plasmones reversibles.

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