Gooding Ann K, Gómez Daniel E, Mulvaney Paul
School of Chemistry & Bio21 Institute, University of Melbourne, 3010, Victoria, Australia.
ACS Nano. 2008 Apr;2(4):669-76. doi: 10.1021/nn7003469.
The photoluminescence (PL) of 2D monolayers of CdSe/CdS/ZnS semiconductor nanocrystals (NCs) deposited on gold substrates and incorporated into electrochemical cells has been studied. By combining simultaneous cyclic voltammetry and confocal microscopy it is demonstrated that when a positive potential is applied to the film in an acetonitrile electrolyte, the PL is irreversibly quenched. This is irrespective of whether the samples are under an inert atmosphere or exposed to air or water vapor. When a negative potential is applied under nitrogen, quenching is also observed; however, it is reversible. Conversely when a negative potential is applied to the NC films in aerated acetonitrile, the PL intensity increases. The enhancement of the PL is stable for at least 180 s while the potential is held at -1.0 V (vs Ag quasi-reference electrode). When the potential is removed the PL intensity returns to the starting value. These results clearly indicate that photobrightening and charge carrier injection are coupled processes. On the basis of these data, we propose a simple kinetic model that explains the origins of photobrightening.
对沉积在金基底上并集成到电化学电池中的二维CdSe/CdS/ZnS半导体纳米晶体(NCs)单层的光致发光(PL)进行了研究。通过结合同步循环伏安法和共聚焦显微镜表明,当在乙腈电解质中对薄膜施加正电位时,PL会不可逆地猝灭。这与样品是处于惰性气氛中还是暴露于空气或水蒸气无关。当在氮气下施加负电位时,也会观察到猝灭;然而,这是可逆的。相反,当在充气乙腈中对NC薄膜施加负电位时,PL强度会增加。当电位保持在 -1.0 V(相对于Ag准参比电极)时,PL的增强至少持续180秒且保持稳定。当去除电位时,PL强度恢复到起始值。这些结果清楚地表明光增强和电荷载流子注入是耦合过程。基于这些数据,我们提出了一个简单的动力学模型来解释光增强的起源。