Cai Tong, Yang Hanjun, Hills-Kimball Katie, Song Jeong-Pil, Zhu Hua, Hofman Elan, Zheng Weiwei, Rubenstein Brenda M, Chen Ou
Department of Chemistry , Brown University , Providence , Rhode Island 02912 , United States.
Department of Chemistry , Syracuse University , Syracuse , New York 13244 , United States.
J Phys Chem Lett. 2018 Dec 20;9(24):7079-7084. doi: 10.1021/acs.jpclett.8b03412. Epub 2018 Dec 7.
Doped lead halide perovskite nanocrystals (NCs) have garnered significant attention due to their superior optoelectronic properties. Here, we report a synthesis of Cd-doped CsPbCl NCs by decoupling Pb- and Cl-precursors in a hot injection method. The resulting Cd-doped perovskite NCs manifest a dual-wavelength emission profile with the first reported example of Cd-dopant emission. By controlling Cd-dopant concentration, the emission profile can be tuned with a dopant emission quantum yield of up to 8%. A new secondary emission (∼610 nm) is induced by an energy transfer process from photoexcited hosts to Cd-dopants and a subsequent electronic transition from the excited state (E) to the ground state (A) of [CdCl] units. This electronic transition matches well with a first-principles density functional theory calculation. Further, the optical behavior of Cd-doped CsPbCl NCs can be altered through postsynthetic anion-exchange reactions. Our studies present a new model system for doping chemistry studies in semiconductors for various optoelectronic applications.
掺杂的卤化铅钙钛矿纳米晶体(NCs)因其优异的光电性能而备受关注。在此,我们报告了一种通过热注入法将铅和氯前驱体解耦来合成镉掺杂的CsPbCl NCs的方法。所得的镉掺杂钙钛矿NCs表现出双波长发射谱,其中首次报道了镉掺杂剂发射的例子。通过控制镉掺杂剂浓度,发射谱可以被调节,掺杂剂发射量子产率高达8%。一种新的二次发射(约610纳米)是由光激发主体到镉掺杂剂的能量转移过程以及随后[CdCl]单元从激发态(E)到基态(A)的电子跃迁所诱导的。这种电子跃迁与第一性原理密度泛函理论计算结果吻合良好。此外,镉掺杂的CsPbCl NCs的光学行为可以通过合成后的阴离子交换反应来改变。我们的研究为各种光电应用的半导体掺杂化学研究提供了一个新的模型系统。