Lim Jia Wei Melvin, Giovanni David, Righetto Marcello, Feng Minjun, Mhaisalkar Subodh Gautam, Mathews Nripan, Sum Tze Chien
Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore 637371, Singapore.
Energy Research Institute @NTU (ERI@N), Interdisciplinary Graduate Programme, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore.
J Phys Chem Lett. 2020 Apr 2;11(7):2743-2750. doi: 10.1021/acs.jpclett.0c00504. Epub 2020 Mar 24.
Slow hot carrier cooling in halide perovskites holds the key to the development of hot carrier (HC) perovskite solar cells. For accurate modeling and pragmatic design of HC materials and devices, it is essential that HC temperatures are reliably determined. A common approach involves fitting the high-energy tail of the main photobleaching peak in a transient absorption spectrum with a Maxwell-Boltzmann distribution. However, this approach is problematic because of complications from the overlap of several photophysical phenomena and a lack of consensus in the community on the fitting procedures. Herein, we propose a simple approach that circumvents these challenges. Through tracking the broadband spectral evolution and accounting for bandgap renormalization and spectral line width broadening effects, our method extracts not only accurate and consistent carrier temperatures but also other important parameters such as the quasi-Fermi levels, bandgap renormalization constant, Establishing a reliable method for the carrier temperature determination is a step forward in the study of HCs for next-generation perovskite optoelectronics.
卤化物钙钛矿中缓慢的热载流子冷却对于热载流子(HC)钙钛矿太阳能电池的发展至关重要。为了对HC材料和器件进行准确建模和务实设计,可靠地确定HC温度至关重要。一种常见的方法是用麦克斯韦-玻尔兹曼分布拟合瞬态吸收光谱中主光漂白峰的高能尾部。然而,由于几种光物理现象的重叠以及该领域在拟合程序上缺乏共识,这种方法存在问题。在此,我们提出一种简单的方法来规避这些挑战。通过跟踪宽带光谱演化并考虑带隙重整化和光谱线宽展宽效应,我们的方法不仅能提取准确且一致的载流子温度,还能提取其他重要参数,如准费米能级、带隙重整化常数。建立一种可靠的载流子温度测定方法是下一代钙钛矿光电器件热载流子研究向前迈出的一步。