A Anusha, Yadav Anjali, Vishnoi Pratap, Sharma Dharmendar Kumar
Department of Chemistry, Maulana Azad National Institute of Technology, Bhopal-462003, India.
New Chemistry Unit, International Centre for Materials Science, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur P.O., Bangalore-560064, India.
Nanoscale. 2025 Feb 27;17(9):5150-5160. doi: 10.1039/d4nr04879b.
Mixing different metal ions at the B site of ABX perovskites offers a promising approach for addressing challenges related to toxicity, stability and performance in optoelectronic applications. One such example is CsPbSnBr which addresses the toxicity issue posed by lead while allowing us to tune optoelectronic properties such as the band gap. In this work, nearly monodisperse CsPbSnBr quantum dots (QDs) were synthesized with variable Pb/Sn compositions, CsPbBr, CsPbSnBr and CsPbSnBr. The photoluminescence quantum yield (PLQY) of CsPbSnBr first increases for = 0.1 and then decreases for = 0.3 with respect to = 0. Such an effect of Sn incorporation on the PLQY was investigated using photoblinking studies which revealed three levels of blinking statistics namely ON, GRAY and OFF. These results along with the excited state lifetime measurements enabled us to understand charge carrier dynamics in the CsPbSnBr QDs. Based on our findings, we propose that the photogenerated hot electrons of Sn enhance the PLQY by filling the trap states centered on Pb, which otherwise promote non-radiative relaxations in the Sn-free CsPbBr. However, at higher Sn concentrations, non-radiative recombination becomes more pronounced, reducing the PLQY.
在ABX钙钛矿的B位混合不同的金属离子,为解决光电子应用中与毒性、稳定性和性能相关的挑战提供了一种很有前景的方法。一个这样的例子是CsPbSnBr,它解决了铅带来的毒性问题,同时使我们能够调节诸如带隙等光电子特性。在这项工作中,合成了具有可变Pb/Sn组成(CsPbBr、CsPbSnBr和CsPbSnBr)的近单分散CsPbSnBr量子点(QDs)。相对于x = 0,CsPbSnBr的光致发光量子产率(PLQY)在x = 0.1时首先增加,然后在x = 0.3时降低。利用光闪烁研究对Sn掺入对PLQY的这种影响进行了研究,该研究揭示了三种闪烁统计水平,即开(ON)、灰(GRAY)和关(OFF)。这些结果以及激发态寿命测量使我们能够了解CsPbSnBr量子点中的电荷载流子动力学。基于我们的发现,我们提出,Sn的光生热电子通过填充以Pb为中心的陷阱态来提高PLQY,否则这些陷阱态会促进无Sn的CsPbBr中的非辐射弛豫。然而,在较高的Sn浓度下,非辐射复合变得更加明显,从而降低了PLQY。