Smith Matthew D, Jaffe Adam, Dohner Emma R, Lindenberg Aaron M, Karunadasa Hemamala I
Department of Chemistry , Stanford University , Stanford , California 94305 , USA . Email:
Department of Materials Science and Engineering , Stanford University , Stanford , California 94305 , USA.
Chem Sci. 2017 Jun 1;8(6):4497-4504. doi: 10.1039/c7sc01590a. Epub 2017 Apr 24.
Through structural and optical studies of a series of two-dimensional hybrid perovskites, we show that broadband emission upon near-ultraviolet excitation is common to (001) lead-bromide perovskites. Importantly, we find that the relative intensity of the broad emission correlates with increasing out-of-plane distortion of the Pb-(μ-Br)-Pb angle in the inorganic sheets. Temperature- and power-dependent photoluminescence data obtained on a representative (001) perovskite support an intrinsic origin to the broad emission from the bulk material, where photogenerated carriers cause excited-state lattice distortions mediated through electron-lattice coupling. In contrast, most inorganic phosphors contain extrinsic emissive dopants or emissive surface sites. The design rules established here could allow us to systematically optimize white-light emission from layered hybrid perovskites by fine-tuning the bulk crystal structure.
通过对一系列二维混合钙钛矿的结构和光学研究,我们表明近紫外激发下的宽带发射是(001)溴化铅钙钛矿所共有的。重要的是,我们发现宽带发射的相对强度与无机片中Pb-(μ-Br)-Pb角的面外畸变增加相关。在代表性的(001)钙钛矿上获得的温度和功率依赖的光致发光数据支持了来自块状材料的宽带发射的内在起源,其中光生载流子通过电子-晶格耦合引起激发态晶格畸变。相比之下,大多数无机磷光体含有外在的发射掺杂剂或发射表面位点。这里建立的设计规则可以使我们通过微调块状晶体结构来系统地优化层状混合钙钛矿的白光发射。