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A mechanistic study of the dopant-induced breakdown in halide perovskites using solid state energy storage devices
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2022-09-06 , DOI: 10.1039/d2ee01754g
Angus G M Mathieson 1, 2, 3 , Wesley M Dose 1, 4 , Hans-Georg Steinrück 5, 6 , Christopher J Takacs 6 , Sascha Feldmann 2, 7 , Raj Pandya 2 , Alice J Merryweather 2, 4 , David Mackanic 6 , Akshay Rao 2 , Felix Deschler 2, 8 , Michael De Volder 1
Affiliation  

Doping halide perovskites (HPs) with extrinsic species, such as alkali metal ions, plays a critical, albeit often elusive role in optimising optoelectronic devices. Here, we use solid state lithium ion battery inspired devices with a polyethylene oxide-based polymer electrolyte to dope HPs controllably with lithium ions. We perform a suite of operando material analysis techniques while dynamically varying Li doping concentrations. We determine and quantify three doping regimes; a safe regime, with doping concentrations of <1020 cm−3 (2% Li : Pb mol%) in which the HP may be modified without detrimental effect to its structure; a minor decomposition regime, in which the HP is partially transformed but remains the dominant species; and a major decomposition regime in which the perovskite is superseded by new phases. We provide a mechanistic description of the processes mediating between each stage and find evidence for metallic Pb(0), LiBr and LiPbBr2 as final decomposition products. Combining results from synchrotron X-ray diffraction measurements with in situ photoluminescence and optical reflection microscopy studies, we distinguish the influences of free charge carriers and intercalated lithium independently. We find that the charge density is equally as important as the geometric considerations of the dopant species and thereby provide a quantitative framework upon which the future design of doped-perovskite energy devices should be based.

中文翻译:

使用固态储能装置对卤化物钙钛矿中掺杂剂诱导击穿的机理研究

用外在物质(如碱金属离子)掺杂卤化物钙钛矿(HPs)在优化光电器件方面发挥着关键作用,尽管通常难以捉摸。在这里,我们使用固态锂离子电池启发设备和基于聚环氧乙烷的聚合物电解质,以可控地用锂离子掺杂 HP。我们执行一套操作材料分析技术,同时动态改变锂掺杂浓度。我们确定并量化了三种兴奋剂方案;一个安全的方案,掺杂浓度<10 20 cm -3(2% Li:Pb mol%),其中 HP 可以被改性而不会对其结构产生不利影响;一个次要的分解机制,其中 HP 被部分转化,但仍然是优势物种;以及钙钛矿被新相取代的主要分解方式。我们对每个阶段之间的过程进行了机械描述,并找到了金属 Pb (0)、LiBr 和 LiPbBr 2作为最终分解产物的证据。将同步加速器 X 射线衍射测量结果与原位相结合通过光致发光和光学反射显微镜研究,我们独立区分了自由电荷载体和嵌入锂的影响。我们发现电荷密度与掺杂剂种类的几何考虑同样重要,从而提供了一个定量框架,未来掺杂钙钛矿能源器件的设计应以此为基础。
更新日期:2022-09-06
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