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双金属纳米结构增强型卤化甲基铵铅钙钛矿中的超快载流子动力学。

Ultrafast carrier dynamics in bimetallic nanostructure-enhanced methylammonium lead bromide perovskites.

机构信息

Department of Chemical and Biomolecular Engineering, Vanderbilt University, Nashville, TN 37235, USA.

Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.

出版信息

Nanoscale. 2017 Jan 26;9(4):1475-1483. doi: 10.1039/c6nr08347a.

Abstract

In this work, we examine the impact of hybrid bimetallic Au/Ag core/shell nanostructures on the carrier dynamics of methylammonium lead tribromide (MAPbBr) mesoporous perovskite solar cells (PSCs). Plasmon-enhanced PSCs incorporated with Au/Ag nanostructures demonstrated improved light harvesting and increased power conversion efficiency by 26% relative to reference devices. Two complementary spectral techniques, transient absorption spectroscopy (TAS) and time-resolved photoluminescence (trPL), were employed to gain a mechanistic understanding of plasmonic enhancement processes. TAS revealed a decrease in the photobleach formation time, which suggests that the nanostructures improve hot carrier thermalization to an equilibrium distribution, relieving hot phonon bottleneck in MAPbBr perovskites. TAS also showed a decrease in carrier decay lifetimes, indicating that nanostructures enhance photoinduced carrier generation and promote efficient electron injection into TiO prior to bulk recombination. Furthermore, nanostructure-incorporated perovskite films demonstrated quenching in steady-state PL and decreases in trPL carrier lifetimes, providing further evidence of improved carrier injection in plasmon-enhanced mesoporous PSCs.

摘要

在这项工作中,我们研究了杂化双金属 Au/Ag 核/壳纳米结构对甲脒铅三溴化物(MAPbBr)介孔钙钛矿太阳能电池(PSC)载流子动力学的影响。与参考器件相比,掺入 Au/Ag 纳米结构的等离子体增强型 PSCs 表现出更好的光捕获和 26%的功率转换效率提高。两种互补的光谱技术,瞬态吸收光谱(TAS)和时间分辨光致发光(trPL),被用来深入了解等离子体增强过程。TAS 揭示了光漂白形成时间的减少,这表明纳米结构改善了热载流子热化到平衡分布,缓解了 MAPbBr 钙钛矿中的热声子瓶颈。TAS 还显示出载流子衰减寿命的减少,这表明纳米结构增强了光致载流子的产生,并促进了在体复合之前将电子有效注入 TiO。此外,掺入纳米结构的钙钛矿薄膜在稳态 PL 中表现出猝灭,trPL 载流子寿命减少,进一步证明了等离子体增强介孔 PSC 中载流子注入的改善。

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