Photophysics and Optoelectronics, Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 4, 9747AG Groningen, The Netherlands.
Department of Materials Science and Engineering, Institute of Materials for Electronics and Energy Technology, Friedrich-Alexander-Universität Erlangen-Nürnberg, Energy Campus Nürnberg, 90429 Nürnberg, Germany.
J Chem Phys. 2019 Dec 7;151(21):214702. doi: 10.1063/1.5128885.
Metal halide perovskite shelled quantum dot solids have recently emerged as an interesting class of solution-processable materials that possess the desirable electronic properties of both quantum dots and perovskites. Recent reports have shown that lead sulfide quantum dots (PbS QDs) with perovskite ligand-shells can be successfully utilized in (opto)electronic devices such as solar cells, photoconductors, and field-effect transistors (FETs), a development attributed to the compatibility of lattice parameters between PbS and certain metal halide perovskites that results in the growth of the perovskite shell on the PbS QDs. Of several possible perovskite combinations used with PbS QDs, bismuth-based variants have been shown to have the lowest lattice mismatch and to display excellent performance in photoconductors. However, they also display photoluminescence (PL), which is highly sensitive to surface defects. In this work, we present an investigation of the transport and optical properties of two types of bismuth-based perovskite (MABiI and MABiI) shelled PbS QDs. Our photophysical study using temperature-dependent PL spectroscopy between 5 and 290 K indicates that the PL efficiency of the reference oleic acid (OA) capped samples is much higher than that of the Bi-shelled ones, which suffer from traps, most likely formed at their surfaces during the phase-transfer ligand exchange process. Nevertheless, the results from electrical measurements on FETs show the successful removal of the native-OA ligands, displaying electron dominated transport with modest mobilities of around 10 cm [V s] - comparable to the reported values for epitaxial Pb-based shelled samples. These findings advance our understanding of perovskite shelled QD-solids and point to the utility of these Bi-based variants as contenders for photovoltaic and other optoelectronic applications.
金属卤化物钙钛矿壳量子点固溶体最近成为一类有趣的溶液处理材料,具有量子点和钙钛矿的理想电子特性。最近的报道表明,具有钙钛矿配体壳的硫化铅量子点(PbS QDs)可以成功地用于(光电)器件,如太阳能电池、光电导体和场效应晶体管(FET),这一发展归因于 PbS 和某些金属卤化物钙钛矿之间晶格参数的兼容性,导致钙钛矿壳在 PbS QDs 上生长。在与 PbS QDs 一起使用的几种可能的钙钛矿组合中,基于铋的变体被证明具有最低的晶格失配,并在光电导体中显示出优异的性能。然而,它们也显示出光致发光(PL),这对表面缺陷非常敏感。在这项工作中,我们研究了两种类型的铋基钙钛矿(MABiI 和 MABiI)壳 PbS QDs 的输运和光学性质。我们使用 5 到 290 K 之间的温度依赖 PL 光谱进行的光物理研究表明,参考油酸(OA)封端样品的 PL 效率远高于 Bi 壳样品,Bi 壳样品受陷阱影响,这些陷阱很可能是在其表面在相转移配体交换过程中形成的。尽管如此,FET 上的电学测量结果表明成功去除了天然-OA 配体,显示出以电子为主导的输运,迁移率约为 10 cm [V s] - 与报道的外延 Pb 基壳样品的值相当。这些发现推进了我们对钙钛矿壳量子点固溶体的理解,并指出这些基于 Bi 的变体作为光伏和其他光电应用的竞争者的实用性。