Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 5, 3584 CC Utrecht, The Netherlands.
Soft Condensed Matter, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 5, 3584 CC Utrecht, The Netherlands.
Sci Rep. 2017 Apr 12;7:45906. doi: 10.1038/srep45906.
Nanocrystalline cesium lead halide perovskites (CsPbX, X = Cl, Br, and I) form an exciting new class of semiconductor materials showing quantum confinement. The emission color can be tuned over the full visible spectral region making them promising for light‒emitting applications. Further control over the optical and magnetic properties of quantum dots (QDs) can be achieved through doping of transition metal (TM) ions such as Mn or Co. Here we demonstrate how, following QD synthesis in the presence of a Mn‒precursor, dropwise addition of silicon tetrachloride (SiCl) to the QDs in toluene results in the formation of Mn‒doped CsPbCl QDs showing bright orange Mn emission around 600 nm. Evidence for successful doping is provided by excitation spectra of the Mn emission, with all features of the CsPbCl QD absorption spectrum and a decrease of the 410 nm excitonic emission life time with increasing Mn‒concentration, giving evidence for enhanced exciton to Mn energy transfer. As a doping mechanism we propose a combination of surface etching and reconstruction and diffusion doping. The presently reported approach provides a promising avenue for doping TM ions into perovskites QDs enabling a wider control over optical and magnetic properties for this new class of QDs.
纳米晶铯铅卤钙钛矿（CsPbX，X=Cl、Br 和 I）形成了一类令人兴奋的新半导体材料，表现出量子限制效应。通过掺杂过渡金属（TM）离子，如 Mn 或 Co，可以实现对量子点（QD）的光学和磁性能的进一步控制。在本研究中，我们展示了如何在 QD 合成过程中加入 Mn 前体，然后逐滴加入四氯化硅（SiCl）到甲苯中的 QD 中，从而形成 Mn 掺杂的 CsPbCl QD，在 600nm 左右表现出明亮的橙色 Mn 发射。通过 Mn 发射的激发光谱提供了成功掺杂的证据，其中包括 CsPbCl QD 吸收光谱的所有特征，以及随着 Mn 浓度的增加，410nm 激子发射寿命的降低，这表明增强了激子到 Mn 的能量转移。我们提出了一种表面蚀刻和重构以及扩散掺杂的组合作为掺杂机制。目前报道的方法为 TM 离子掺杂钙钛矿 QD 提供了一条有前途的途径，为这一新类 QD 的光学和磁性能提供了更广泛的控制。
