Proceedings of International Conference on Perovskite Thin Film Photovoltaics, Photonics and Optoelectronics (ABXPV18PEROPTO)
DOI: https://doi.org/10.29363/nanoge.abxpvperopto.2018.013
Publication date: 11th December 2017
Photovoltaic devices based on hybrid metal halide perovskites are rapidly improving in power conversion efficiency. At the Shockley-Queisser limit, the recombination and mobility of charge-carriers will be limited only by intrinsic properties. Yet, the mechanisms for these parameters, and their link with material stoichiometry, is still poorly understood.
We show that bimolecular (band-to-band) recombination of charge-carriers in methylammonium lead triiodide perovskite can be fully explained as the inverse process of absorption. The sharpening of photon, electron and hole distribution functions therefore significantly enhances bimolecular charge recombination as the temperature is lowered, mirroring trends in transient spectroscopy [1]. We show that typical measurements of the radiative bimolecular recombination constant in CH3NH3PbI3 are also strongly affected by photon reabsorption that masks a much larger intrinsic bimolecular recombination rate constant [2]. By investigating films whose thickness varies between 50 and 533 nm, we show that the bimolecular charge recombination rate indeed appears to slow by an order of magnitude as the film thickness increases. However, by using a dynamical model that accounts for photon reabsorption and charge-carrier diffusion we determine that a single intrinsic bimolecular recombination coefficient of value 6.8×10−10cm3s−1 is common to all samples irrespective of film thickness [2]. We also examine the critical role of photon confinement on free charge-carrier retention in thin photovoltaic layers.
We further discuss the role of Fröhlich interaction is the dominant source of electron-phonon coupling determining the charge-carrier mobility in high-quality perovskites near room temperature [3]. We show that while mobilities in some of these hybrid perovskites are near the intrinsic limit of what is fundamentally achievable, others are still dominated by effects of alloying, structural instabilities and doping [4,5].
[1] R. L. Milot, G. E. Eperon, H. J. Snaith, M. B. Johnston, and L. M. Herz, Adv. Func. Mater., 25, 6218 (2015).
[2] T. W. Crothers, R. L. Milot, J. B. Patel, E. S. Parrott, J. Schlipf, P. Müller-Buschbaum, M. B. Johnston, and L. M. Herz, Nano Lett. 17, 5782 (2017).
[3] A. D. Wright, C. Verdi, R. L. Milot, G. E. Eperon, M. A. Pérez-Osorio, H. J. Snaith, F. Giustino, M. B. Johnston, and L. M. Herz, Nature Communications 7, 11755 (2016).
[4] L. M. Herz, ACS Energy Lett. 2, 1539 (2017).
[5] W. Rehman, D. P. McMeekin, J. B. Patel, R. L. Milot, M. B. Johnston, H. J. Snaith, and L. M. Herz, Energy Environ. Sci. 10, 361 (2017).
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