Stewart Robert J, Grieco Christopher, Larsen Alec V, Maier Joshua J, Asbury John B
Department of Chemistry, The Pennsylvania State University , University Park, Pennsylvania 16802, United States.
Materials Characterization Lab, The Pennsylvania State University , University Park, Pennsylvania 16802, United States.
J Phys Chem Lett. 2016 Apr 7;7(7):1148-53. doi: 10.1021/acs.jpclett.6b00366. Epub 2016 Mar 14.
The electronic properties of organo-halide perovskite absorbers described in the literature have been closely associated with their morphologies and processing conditions. However, the underlying origins of this dependence remain unclear. A combination of inorganic synthesis, surface chemistry, and time-resolved photoluminescence spectroscopy was used to show that charge recombination centers in organo-halide perovskites are almost exclusively localized on the surfaces of the crystals rather than in the bulk. Passivation of these surface defects causes average charge carrier lifetimes in nanocrystalline thin films to approach the bulk limit reported for single-crystal organo-halide perovskites. These findings indicate that the charge carrier lifetimes of perovskites are correlated with their thin-film processing conditions and morphologies through the influence these have on the surface chemistry of the nanocrystals. Therefore, surface passivation may provide a means to decouple the electronic properties of organo-halide perovskites from their thin-film processing conditions and corresponding morphologies.
文献中描述的有机卤化物钙钛矿吸收剂的电子特性与其形态和加工条件密切相关。然而,这种依赖性的潜在根源仍不清楚。通过无机合成、表面化学和时间分辨光致发光光谱的结合,表明有机卤化物钙钛矿中的电荷复合中心几乎完全位于晶体表面而非体相中。这些表面缺陷的钝化使得纳米晶薄膜中的平均电荷载流子寿命接近单晶有机卤化物钙钛矿报道的体相极限。这些发现表明,钙钛矿的电荷载流子寿命通过其对纳米晶体表面化学的影响与其薄膜加工条件和形态相关。因此,表面钝化可能提供一种手段,使有机卤化物钙钛矿的电子特性与其薄膜加工条件和相应形态脱钩。