Zhou Hongzhi, Feng Qingjie, Sun Cheng, Li Yahui, Tao Weijian, Tang Wei, Li Linjun, Shi Enzheng, Nan Guangjun, Zhu Haiming
Department of Chemistry, State Key Laboratory of Extreme Photonics and Instrumentation, Zhejiang Key Laboratory of Excited State Energy Conversion and Storage, Zhejiang University, Hangzhou, China.
Department of Physics, Zhejiang Normal University, Jinhua, Zhejiang, China.
Nat Commun. 2024 Oct 2;15(1):8541. doi: 10.1038/s41467-024-52952-9.
2D perovskites hold immense promise in optoelectronics due to their strongly bound electron-hole pairs (i.e., excitons). While exciton polaron from interplay between exciton and lattice has been established in 2D lead-based perovskites, the exciton nature and behavior in the emerging 2D tin-based perovskites remains unclear. By combining spin-resolved ultrafast spectroscopy and sophisticated theoretical calculations, we reveal 2D tin-based perovskites as genuine excitonic semiconductors with weak polaronic screening effect and persistent Coulomb interaction, thanks to weak exciton-phonon coupling. We determine an excited state exciton binding energy of ~0.18 eV in n = 2 tin iodide perovskites, nearly twice of that in lead counterpart, despite of same large value of ~0.2 eV from steady state measurement. This finding emphasizes the pivotal role of excited state polaronic effect in these materials. The robust excitons in 2D tin-based perovskites exhibit excitation power-insensitive, high-efficiency and color-purity emission, rendering them superior for light-emitting applications.
二维钙钛矿因其强束缚的电子-空穴对(即激子)在光电子学领域具有巨大潜力。虽然二维铅基钙钛矿中已证实激子与晶格相互作用产生的激子极化子,但新兴的二维锡基钙钛矿中的激子性质和行为仍不清楚。通过结合自旋分辨超快光谱和精密理论计算,我们揭示二维锡基钙钛矿是具有弱极化子屏蔽效应和持久库仑相互作用的真正激子半导体,这得益于其弱激子-声子耦合。我们确定在n = 2的碘化锡钙钛矿中,激发态激子结合能约为0.18 eV,尽管稳态测量得到的值同样约为0.2 eV,但几乎是铅基对应物的两倍。这一发现强调了激发态极化子效应在这些材料中的关键作用。二维锡基钙钛矿中稳健的激子表现出对激发功率不敏感、高效和色纯度高的发射特性,使其在发光应用方面具有优势。