Physics Department, National University of Singapore, 2 Science Drive 3, Singapore, 117542, Singapore.
Centre for Advanced 2D Materials and Graphene Research Centre, National University of Singapore, 6 Science Drive 2, Singapore, 117546, Singapore.
Adv Mater. 2018 May;30(18):e1704055. doi: 10.1002/adma.201704055. Epub 2018 Mar 25.
2D organic-inorganic hybrid perovskites (OIHPs) represent a unique class of materials with a natural quantum-well structure and quasi-2D electronic properties. Here, a versatile direct solution-based synthesis of mono- and few-layer OIHP nanosheets and a systematic study of their electronic structure as a function of the number of monolayers by photoluminescence and absorption spectroscopy are reported. The monolayers of various OIHPs are found to exhibit high electronic quality as evidenced by high quantum yield and negligible Stokes shift. It is shown that the ground exciton peak blueshifts by ≈40 meV when the layer thickness reduces from bulk to monolayer. It is also shown that the exciton binding energy remains effectively unchanged for (C H (CH ) NH ) PbI with the number of layers. Similar trends are observed for (C H NH ) PbI in contrast to the previous report. Further, the photoluminescence lifetime is found to decrease with the number of monolayers, indicating the dominant role of surface trap states in nonradiative recombination of the electron-hole pairs.
2D 有机-无机杂化钙钛矿(OIHPs)是一类具有天然量子阱结构和准二维电子特性的独特材料。在此,我们报道了一种通用的直接溶液法合成单原子层和少层 OIHP 纳米片的方法,并通过光致发光和吸收光谱系统研究了其电子结构随层数的变化。结果表明,各种 OIHP 的单层表现出较高的电子质量,这表现为高量子产率和可忽略的斯托克斯位移。研究表明,当层厚从体相减少到单层时,基激子峰蓝移约 40 meV。此外,对于(C H (CH ) NH )PbI,实验发现激子结合能随层数的变化基本保持不变。这与之前的报道相反,对于(C H NH )PbI 也观察到了类似的趋势。进一步地,研究发现光致发光寿命随层数的减少而减小,表明表面陷阱态在电子-空穴对的非辐射复合中起主导作用。