Understanding Power-Law Photoluminescence Decays and Bimolecular Recombination in Lead-Halide Perovskites

IF 8.2 1区 化学 Q1 CHEMISTRY, ANALYTICAL ACS Sensors Pub Date : 2024-09-11 DOI:10.1002/aenm.202403279
Ye Yuan, Genghua Yan, Chris Dreessen, Thomas Kirchartz
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Abstract

Transient photoluminescence is a frequently used method in the field of halide perovskite photovoltaics to quantify recombination by determining the characteristic decay time of an exponential decay. This decay time is often considered to be a single value for a certain perovskite film. However, there are many mechanisms that lead to non-exponential decays. Here, it is shown that photoluminescence decays in many lead-halide perovskites are non-exponential and follow a power-law relation between PL intensity and time that is caused by shallow defects. Decay times therefore vary continuously as a function of time and injection level. In situations where recombination is bimolecular and decays follow a power law, the differential decay time equals the time delay after the laser pulse for long time delays and therefore completely lacks quantitative information about the recombination rate. Quantifying recombination using transient PL measurements, therefore, requires analyzing the lifetime as a function of injection level rather than time. As an alternative to the continuously varying decay time, a bimolecular recombination coefficient can also be determined, which correlates with the photoluminescence quantum efficiency. Finally, the influence of the repetition rate and the background subtraction method on the analysis of power-law type PL decays is discussed.
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了解铅卤化物过氧化物中的功率定律光致发光衰减和双分子重组
瞬态光致发光是卤化物包晶光伏领域常用的一种方法,通过确定指数衰减的特征衰减时间来量化重组。这种衰减时间通常被认为是某种过氧化物薄膜的单一值。然而,有许多机制会导致非指数衰减。这里的研究表明,许多卤化铅包晶石的光致发光衰减都是非指数衰减,并且遵循光致发光强度与时间之间的幂律关系,这是由浅缺陷引起的。因此,衰减时间作为时间和注入水平的函数不断变化。在双分子重组和衰减遵循幂律的情况下,差分衰减时间等于激光脉冲后的长延时,因此完全缺乏有关重组速率的定量信息。因此,利用瞬态聚光测量来量化重组需要分析作为注入水平而非时间函数的寿命。作为连续变化衰减时间的替代方法,还可以测定双分子重组系数,该系数与光致发光量子效率相关。最后,还讨论了重复率和背景减除法对幂律型聚光衰减分析的影响。
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来源期刊
ACS Sensors
ACS Sensors Chemical Engineering-Bioengineering
CiteScore
14.50
自引率
3.40%
发文量
372
期刊介绍: ACS Sensors is a peer-reviewed research journal that focuses on the dissemination of new and original knowledge in the field of sensor science, particularly those that selectively sense chemical or biological species or processes. The journal covers a broad range of topics, including but not limited to biosensors, chemical sensors, gas sensors, intracellular sensors, single molecule sensors, cell chips, and microfluidic devices. It aims to publish articles that address conceptual advances in sensing technology applicable to various types of analytes or application papers that report on the use of existing sensing concepts in new ways or for new analytes.
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