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Although methylammonium lead iodide (CH$_3$NH$_3$PbI$_3$) perovskite hasattracted enormous scientific attention over the last decade or so, importantinformation on the charge extraction dynamics and recombination processes inperovskite devices is still missing. Herein we present a novel approach toevaluate the quality of CH$_3$NH$_3$PbI$_3$ layers, via in-situ monitoring ofthe perovskite layer charge carrier dynamics during the thermal annealingcrystallization process, by means of time-resolved femtosecond transientabsorption spectroscopy (TAS). In particular, CH$_3$NH$_3$PbI$_3$ films weredeposited on two types of polymeric hole transport layers (HTL),poly(3,4-ethylenedioxythiophene)-poly-(styrenesulfonate) (PEDOT:PSS) andpoly-(triarylamine) (PTAA), that are known to provide different carriertransport characteristics in perovskite solar cells. In order to monitor theevolution of the perovskite charge carrier dynamics during the crystallizationprocess, the so-formed CH$_3$NH$_3$PbI$_3$/HTL architectures were studiedin-situ by TAS at three different annealing temperatures, i.e. 90, 100 and 110oC. It is revealed that the annealing time period required in order to achievethe optimum perovskite film quality in terms of the decay dynamics stronglydepends on the annealing temperature, as well as, on the employed HTL. For bothHTLs, the required period decreases as higher annealing temperature is used,while, for the more hydrophobic PTAA polymer, longer annealing periods wererequired in order to obtain the optimum charge carrier dynamics. Thecorrelation of the TAS finding with the structural and morphological featuresof the perovskite films is analysed and provides useful insights on the chargeextraction dynamics and recombination processes in perovskite optoelectronicdevices.

In-Situ Monitoring of the Charge Carrier Dynamics of CH$_3$NH$_3$PbI$_3$ Perovskite Crystallization Process