Titus Timi, Vishnu E Krishnan, Garai Arghyadeep, Dutta Sumit Kumar, Sandeep Kuttysankaran, Shelke Ankita, Ajithkumar Thalasseril G, Shaji Anil, Pradhan Narayan, Thomas K George
School of Chemistry, Indian Institute of Science Education and Research Thiruvananthapuram (IISER TVM), Vithura, Thiruvananthapuram, 695551, India.
Centre for Advanced Materials Research with International Engagement (CAMRIE), Indian Institute of Science Education and Research Thiruvananthapuram (IISER TVM), Vithura, Thiruvananthapuram, 695551, India.
Nano Lett. 2024 Aug 28;24(34):10434-10442. doi: 10.1021/acs.nanolett.4c01186. Epub 2024 Aug 14.
The metal halide perovskite nanocrystals exhibit a remarkable tolerance to midgap defect states, resulting in high photoluminescence quantum yields. However, the potential of these nanocrystals for applications in display devices is hindered by the suppression of biexcitonic emission due to various Auger recombination processes. By adopting single-particle photoluminescence spectroscopy, herein, we establish that the biexcitonic quantum efficiency increases with the increase in the number of facets on cesium lead bromide perovskite nanocrystals, progressing from cube to rhombic dodecahedron to rhombicuboctahedron nanostructures. The observed enhancement is attributed mainly to an increase in their surface polarity as the number of facets increases, which reduces the Coulomb interaction of charge carriers, thereby suppressing Auger recombination. Moreover, Auger recombination rate constants obtained from the time-gated photon correlation studies exhibited a discernible decrease as the number of facets increased. These findings underscore the significance of facet engineering in fine-tuning biexciton emission in metal halide perovskite nanocrystals.
金属卤化物钙钛矿纳米晶体对带隙中缺陷态表现出显著的耐受性,从而产生高光致发光量子产率。然而,由于各种俄歇复合过程导致双激子发射受到抑制,这些纳米晶体在显示设备中的应用潜力受到阻碍。在此,通过采用单粒子光致发光光谱,我们确定双激子量子效率随着溴化铯铅钙钛矿纳米晶体晶面数量的增加而增加,从立方体结构发展到菱形十二面体结构再到截角八面体纳米结构。观察到的增强主要归因于随着晶面数量增加其表面极性增加,这减少了电荷载流子的库仑相互作用,从而抑制了俄歇复合。此外,从时间分辨光子相关研究中获得的俄歇复合速率常数随着晶面数量的增加而明显降低。这些发现强调了晶面工程在微调金属卤化物钙钛矿纳米晶体中双激子发射方面的重要性。