Excitation pulse repetition rate variation method for studying carrier recombination kinetics in perovskite thin films
Pavel A. Frantsuzov a, Alexander Kiligaridis b, Aymen Yangui b, Sudipta Seth b, Jun Li b, Yana Vaynzof c, Ivan G. Scheblykin b
a Voevodsky Institute of Chemical Kinetics and Combustion, SB RAS, Novosibirsk, Russia
b Lund University, Department of Chemical Physics and NanoLund, Sweden, Lund, Sweden
c Institute of Applied Physics, TU Dresden, Nöthnitzer Straße, 61, Dresden, Germany
Oral, Pavel A. Frantsuzov, presentation 117
DOI: https://doi.org/10.29363/nanoge.nipho.2020.117
Publication date: 25th November 2019

Despite tremendous efforts in recent years to study the kinetics of charge recombination in metal-halide perovskite films, the detailed molecular mechanism of these processes is still not fully understood. As an example, photoluminescence (PL) intensity of the perovskite thin films shows greatly varying dependencies on the excitation fluence when measured by different laboratories at different experimental conditions [1-4]. We performed a systematic study of a photoluminescence intensity of the CH3NH3PbI3 thin film at a wide range of the excitation pulse energies with the repetition rate changed from 80MHz to 1 Hz. It was found that for all pulse energies, the dependence of the photoluminescence intensity on the averaged excitation power density lies on one curve corresponding to the high repetition frequency case (quasi-CW regime). With a decrease in the repetition rate, the PL intensity deviates from the quasi-CW dependence and ultimately becomes independent of the frequency (single-pulse regime). We have shown that the frequency of the transition from the quasi-CW regime to the single-pulse regime strongly depends on the pulse energy. In other words, lower charge carrier concentration requires much lower repetition rate to reach the single-pulse regime. It means that by varying the pulse energy at a given repetition rate one can move from the CW-regime to the single-pulse regime. This explains variations of the PL intensity dependences on the pulse energy and the general difficulty to explain them quantitatively. Numerical simulations were carried out to fit the experimental dependencies by several theoretical models.


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