Ricciarelli Damiano, Mosconi Edoardo, Merabet Boualem, Bizzarri Olivia, De Angelis Filippo
Department of Chemistry, Biology and Biotechnology, University of Perugia, Via Elce di Sotto 8, 06123 Perugia, Italy.
Istituto CNR di Scienze e Tecnologie Chimiche "Giulio Natta" (CNR-SCITEC), Via Elce di Sotto 8, 06123 Perugia, Italy.
J Phys Chem Lett. 2020 Jul 16;11(14):5482-5489. doi: 10.1021/acs.jpclett.0c01567. Epub 2020 Jun 26.
Metal halide perovskites exhibit impressive optoelectronic properties with applications in solar cells and light-emitting diodes. Co-doping the high-band gap CsPbCl perovskite with Bi and Mn enhances both material stability and luminescence, providing emission on a wide spectral range. To discuss the role of Bi and Mn dopants in tuning the CsPbCl perovskite energy levels and their involvement in carrier trapping, we report state-of-the-art hybrid density functional theory calculations, including spin-orbit coupling. We show that co-doping the perovskite with Bi and Mn delivers essentially the sum of the electronic properties of the single dopants, with no significant interaction or the preferential mutual location of them. Furthermore, we identify the structural features and energetics of transitions of electrons trapped at Bi and holes trapped at Mn dopant ions, respectively, and discuss their possible role in determining the optical properties of the co-doped perovskite.
金属卤化物钙钛矿展现出令人印象深刻的光电特性，在太阳能电池和发光二极管中有着应用。用铋（Bi）和锰（Mn）对高带隙CsPbCl钙钛矿进行共掺杂，可增强材料稳定性和发光性能，实现宽光谱范围的发射。为了探讨Bi和Mn掺杂剂在调节CsPbCl钙钛矿能级中的作用及其在载流子俘获中的参与情况，我们报告了包括自旋轨道耦合在内的最新混合密度泛函理论计算结果。我们表明，用Bi和Mn对钙钛矿进行共掺杂基本上给出了单一掺杂剂电子性质的总和，它们之间没有显著相互作用或优先的相互位置。此外，我们分别确定了捕获在Bi处的电子和捕获在Mn掺杂离子处的空穴的跃迁结构特征和能量，并讨论了它们在确定共掺杂钙钛矿光学性质方面可能发挥的作用。
