School of Materials Science and Engineering, Chonnam National University, 77, Yongbong-ro, Buk-Gu, Gwangju, 61186, Republic of Korea.
Nat Commun. 2018 Nov 8;9(1):4691. doi: 10.1038/s41467-018-07097-x.
Zero-dimensional (0D) inorganic perovskites have recently emerged as an interesting class of material owing to their intrinsic Pb emission, polaron formation, and large exciton binding energy. They have a unique quantum-confined structure, originating from the complete isolation of octahedra exhibiting single-molecule behavior. Herein, we probe the optical behavior of single-molecule-like isolated octahedra in 0D Cesium lead halide (CsPbX, X = Cl, Br/Cl, Br) nanocrystals through isovalent manganese doping at lead sites. The incorporation of manganese induced phase stabilization of 0D CsPbX over CsPbX by lowering the symmetry of PbX via enhanced octahedral distortion. This approach enables the synthesis of CsPbX free CsPbX nanocrystals. A high photoluminescence quantum yield for manganese emission was obtained in colloidal (29%) and solid (21%, powder) forms. These performances can be attributed to structure-induced confinement effects, which enhance the energy transfer from localized host exciton states to Mn dopant within the isolated octahedra.
零维（0D）无机钙钛矿由于其本征的 Pb 发射、极化子形成和大激子结合能而成为一类有趣的材料。它们具有独特的量子限制结构，源于完全隔离的八面体表现出单分子行为。在此，我们通过在铅位掺杂等价锰来探测 0D 铯铅卤化物（CsPbX，X = Cl、Br/Cl、Br）纳米晶体中单分子样孤立八面体的光学行为。锰的掺入通过增强八面体变形降低了 PbX 的对称性，从而稳定了 0D CsPbX 的相，使其不依赖于 CsPbX。该方法能够合成无 CsPbX 的 CsPbX 纳米晶体。在胶体（29%）和固态（21%，粉末）形式中获得了锰发射的高光致发光量子产率。这些性能可归因于结构诱导的限制效应，该效应增强了从局部主体激子态到孤立八面体中 Mn 掺杂剂的能量转移。
