Mondal Navendu, De Apurba, Das Somnath, Paul Sumanta, Samanta Anunay
School of Chemistry, University of Hyderabad, Hyderabad 500046, India. E-mail:
Nanoscale. 2019 May 28;11(20):9796-9818. doi: 10.1039/c9nr01745c. Epub 2019 May 9.
Perovskite nanocrystals (NCs), especially those based on cesium lead halides, have emerged in recent years as highly promising materials for efficient solar cells and photonic applications. The key to realization of full potential of these materials lies however in the molecular level understanding of the processes triggered by light. Herein we highlight the knowledge gained from photophysical investigations on these NCs of various sizes and compositions employing primarily the femtosecond pump-probe technique. We show how spectral and temporal characterization of the photo-induced transients provide insight into the mechanism and dynamics of relaxation of hot and thermalized charge carriers through their recombination and trapping. We discuss how the multiple excitons including the charged ones (trions), generated using high pump fluence or photon energy, recombine through the Auger-assisted process. We discussed the harvesting of hot carriers prior to their cooling and band-edge carriers from these perovskite NCs to wide band-gap metal oxides, metal chalcogenide NCs and molecular acceptors. How perovskites can influence the charge carrier dynamics in composites of organic and inorganic semiconductors is also discussed.
钙钛矿纳米晶体(NCs),尤其是基于铯铅卤化物的那些,近年来已成为用于高效太阳能电池和光子应用的极具前景的材料。然而,要实现这些材料的全部潜力,关键在于从分子层面理解光引发的过程。在此,我们重点介绍主要采用飞秒泵浦 - 探测技术对各种尺寸和组成的这些纳米晶体进行光物理研究所获得的知识。我们展示了光致瞬态的光谱和时间表征如何通过热载流子和热化电荷载流子的复合与俘获来深入了解其弛豫机制和动力学。我们讨论了使用高泵浦通量或光子能量产生的包括带电激子(三重态激子)在内的多个激子如何通过俄歇辅助过程复合。我们还讨论了在热载流子冷却之前以及从这些钙钛矿纳米晶体中获取带边载流子到宽带隙金属氧化物、金属硫族化物纳米晶体和分子受体的情况。此外,还讨论了钙钛矿如何影响有机和无机半导体复合材料中的电荷载流子动力学。