Department of Chemistry and ‡Department of Physics, Indian Institute of Science Education and Research (IISER) , Pune, India , 411008.
Nano Lett. 2016 Aug 10;16(8):4838-48. doi: 10.1021/acs.nanolett.6b01168. Epub 2016 Jul 12.
Colloidal CsPbBr3 perovskite nanocrystals (NCs) have emerged as an excellent light emitting material in last one year. Using time domain and time-resolved THz spectroscopy and density functional theory based calculations, we establish 3-fold free carrier recombination mechanism, namely, nonradiative Auger, bimolecular electron-hole recombination, and inefficient trap-assisted recombination in 11 nm sized colloidal CsPbBr3 NCs. Our results confirm a negligible influence of surface defects in trapping charge carriers, which in turn results into desirable intrinsic transport properties, from the perspective of device applications, such as remarkably high carrier mobility (∼4500 cm(2) V(-1) s(-1)), large diffusion length (>9.2 μm), and high luminescence quantum yield (80%). Despite being solution processed and possessing a large surface to volume ratio, this combination of high carrier mobility and diffusion length, along with nearly ideal photoluminescence quantum yield, is unique compared to any other colloidal quantum dot system.
胶体 CsPbBr3 钙钛矿纳米晶体(NCs)在过去一年中作为一种出色的发光材料而出现。通过时域和时间分辨太赫兹光谱以及基于密度泛函理论的计算,我们在 11nm 大小的胶体 CsPbBr3 NCs 中建立了 3 重自由载流子复合机制,即非辐射性的俄歇复合、双分子电子-空穴复合以及低效的陷阱辅助复合。从器件应用的角度来看,我们的结果证实了表面缺陷在俘获载流子方面的影响可以忽略不计,这反过来又导致了理想的本征输运性质,例如显著的高载流子迁移率(~4500cm2V-1s-1)、大扩散长度(>9.2μm)和高光致发光量子产率(80%)。尽管是溶液处理的并且具有大的表面积与体积比,但与任何其他胶体量子点系统相比,这种高载流子迁移率和扩散长度的组合以及近乎理想的光致发光量子产率是独特的。