论文标题
自组装的铅卤化物钙钛矿纳米晶体超级晶格的时间演变:对光致发光和能量传递的影响
Temporal Evolution of Self-Assembled Lead Halide Perovskite Nanocrystal Superlattices: Effects on Photoluminescence and Energy Transfer
论文作者
论文摘要
据报道,在自组装铅卤化物钙钛矿纳米晶体中的激子/电子耦合和合作相互作用会引起集体的低能发射峰,并加速动力学。在这里,我们报告说,由于自组装超晶格中的纳米晶反应性,可能会出现类似的光谱特征。这是通过在室温和低温微透明光谱的情况下使用CSPBBR3纳米晶超晶格的。结果表明,将这种结构保持在真空下,超晶格的逐渐收缩以及随后的纳米晶体结合发生了几天。结果,由于纳米晶之间的能量转移,在4 K处观察到狭窄的低能量发射峰,同时缩短了光致发光寿命。当暴露于空气时,自组装的CSPBBR3纳米晶体在超晶格的顶部会形成散装的cspbbr3颗粒。在4 K时,这些颗粒会产生狭窄的低能发射峰的分布,其寿命短,激发依赖性,振荡衰减,类似于超荧光的特征。总体而言,CSPBBR3纳米晶体的反应性极大地改变了它们的组件的发射,在研究集体光电特性时,不应忽略它们,或与超荧光效应混淆。
Excitonic/electronic coupling and cooperative interactions in self-assembled lead halide perovskite nanocrystals were reported to give rise to a collective low energy emission peak with accelerated dynamics. Here we report that similar spectroscopic features could appear as a result of the nanocrystal reactivity within the self-assembled superlattices. This is demonstrated by using CsPbBr3 nanocrystal superlattices under room temperature and cryogenic micro-photoluminescence spectroscopy. It is shown that keeping such structures under vacuum, a gradual contraction of the superlattices and subsequent coalescence of the nanocrystals occurs over several days. As a result, a narrow, low energy emission peak is observed at 4 K with a concomitant shortening of the photoluminescence lifetime due to the energy transfer between nanocrystals. When exposed to air, self-assembled CsPbBr3 nanocrystals develop bulk-like CsPbBr3 particles on top of the superlattices. At 4 K, these particles produce a distribution of narrow, low energy emission peaks with short lifetimes and excitation fluence-dependent, oscillatory decays, resembling the features of superfluorescence. Overall, the reactivity of CsPbBr3 nanocrystals dramatically alters the emission of their assemblies, which should not be overlooked when studying collective optoelectronic properties nor confused with superfluorescence effects.