Elbert Chia, Chan Lao-o-vorakiat, Teddy Salim, Jeannette Kadro, M.-T. Khuc, R. Haselsberger, Liang Cheng, Huanxin Xia, Gagik Gurzadyan, H. B. Su, Yeng Ming Lam, R. A. Marcus, Maria-Elisabeth Michel-Beyerle
Apart from broadband absorption of solar radiation, the performance of photovoltaic devices is governed by the density and mobility of photogenerated charge carriers. The latter parameters indicate how many free carriers move away from their origin, and how fast, before loss mechanisms such as carrier recombination occur. However, only lower bounds of these parameters are usually obtained. Here we independently determine both density and mobility of charge carriers in the organometallic halide perovskite film CH3NH3PbI3 by use of time-resolved terahertz (THz) spectroscopy (TRTS). Our data reveal the modification of the free carrier response by strong backscattering expected from these heavily disordered perovskite films. The results for different phases and different temperatures show a change of kinetics from two-body recombination at room temperature to three-body recombination at low temperatures. Our results suggest that perovskite-based solar cells can perform well even at low temperatures as long as the three-body recombination has not become predominant.
Various tetraphenylporphyrins (zinc, magnesium, free base) were excited to the upper electronic levels of the Soret band with the second harmonic of a mode-locked Ti-sapphire laser (394 nm). An up-conversion fluorescence set-up with the time resolution of 120 fs was used to measure the decay times of the S2 fluorescence in conjunction with the risetime of the S1 fluorescence. The depopulation of the excited electronic state S2 was studied as a function of the metal ion and the solvent. The lifetimes of the electronic S2 level, measured for ZnTPP and MgTPP in different solvents were (tau) equals 1.4 - 3.4 ps. The depopulation channel from S2 to S1 was studied by measuring simultaneously the decay of S2 and the rise of S1 fluorescence. The rate constant of the process can be correlated to the energy gap between the S2 and S1 levels, which depends on the nature of the metal ions and solvents. The rotational dynamics in the Soret band was also studied by measuring the anisotropy of S2 ---> S0 fluorescence. The anisotropy decay of S2 fluorescence was found to be biexponential, with a fast component around 100 fs and a slow one (t >> 10 ps), attributed to the partial dephasing of the degenerate energy levels of the S2 state and to rotational diffusion, respectively.
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