Johnston Andrew, Walters Grant, Saidaminov Makhsud I, Huang Ziru, Bertens Koen, Jalarvo Niina, Sargent Edward H
Department of Electrical and Computer Engineering, University of Toronto, Toronto, Ontario M5S 1A4, Canada.
Department of Chemistry and Electrical & Computer Engineering, Centre for Advanced Materials and Related Technologies (CAMTEC), University of Victoria, Victoria V8P 5C2, Canada.
ACS Nano. 2020 Nov 24;14(11):15107-15118. doi: 10.1021/acsnano.0c05179. Epub 2020 Oct 26.
Engineering the composition of perovskite active layers has been critical in increasing the efficiency of perovskite solar cells (PSCs) to more than 25% in the latest reports. Partial substitutions of the monovalent cation and the halogen have been adopted in the highest-performing devices, but the precise role of bromine incorporation remains incompletely explained. Here we use quasi-elastic neutron scattering (QENS) to study, as a function of the degree of bromine incorporation, the dynamics of organic cations in triple-cation lead mixed-halide perovskites. We find that the inclusion of bromine suppresses low-energy rotations of formamidinium (FA), and we find that inhibiting FA rotation correlates with a longer-lived carrier lifetime. When the fraction of bromine approaches 0.15 on the halogen site-a composition used extensively in the PSC literature-the fraction of actively rotating FA molecules is minimized: indeed, the fraction of rotating FA is suppressed by more than 25% compared to the bromine-free perovskite.
在最近的报道中,设计钙钛矿活性层的组成对于将钙钛矿太阳能电池(PSC)的效率提高到25%以上至关重要。在性能最佳的器件中采用了单价阳离子和卤素的部分替代,但溴掺入的确切作用仍未得到充分解释。在这里,我们使用准弹性中子散射(QENS)来研究三价阳离子铅混合卤化物钙钛矿中有机阳离子的动力学,作为溴掺入程度的函数。我们发现,溴的加入抑制了甲脒(FA)的低能旋转,并且我们发现抑制FA旋转与更长的载流子寿命相关。当卤素位点上溴的比例接近0.15时(这是PSC文献中广泛使用的一种组成),活跃旋转的FA分子的比例最小化:实际上,与无溴钙钛矿相比,旋转FA的比例被抑制了25%以上。