Atomic-scale imaging of ytterbium ions in lead halide perovskites

Sci Adv. 2023 Sep;9(35):eadi7931. doi: 10.1126/sciadv.adi7931. Epub 2023 Sep 1.

Abstract

Lanthanide-doped lead halide perovskites have demonstrated great potential for photoelectric applications. However, there is a long-standing controversy about the existence of lanthanide ions, e.g., whether the doping of Ln3+ is successful or not; the substituting sites of Ln3+ in lead halide perovskites are unclear. We directly identify the doped Yb3+ in CsPbCl3 perovskites by using the state-of-the-art transmission electron microscopy and three-dimensional atom probe tomography at atomic scale. Different from the previous assumptions and/or results, we evidence that Yb3+ simultaneously replace Pb2+ and occupy the lattice interstitial sites. Furthermore, we directly observe the cluster phenomenon of CsPbCl3 single crystal at near atomic scale. Density functional theory modeling further confirms and explains the mechanisms of our findings. Our findings thus provide an atomic-level understanding of the doping mechanism in perovskites and will stimulate a further thinking of the doping effect on the performance of perovskites.