Proceedings of September Meeting 2016 (NFM16)
Publication date: 14th June 2016
Organic-inorganic hybrid perovskites, such as methylammonium lead iodide (MAPbI3), are promising materials for solar light harvesting and optoelectronics applications. We investigated the charge carrier dynamics of (MAI)x(PbI2)1-x for the mole fraction range x = 0.32-0.90.1,2 Ultrafast pump - supercontinuum probe spectroscopy was employed to study cooling and recombination processes at different initial carrier densities. Low-dimensional perovskites (LDPs) were formed at high methylammonium iodide excess (x = 0.90), and their luminescence spectra exhibited a significant blue-shift and broadening compared to 3D perovskites. The spectral shift arises from the confined perovskite structure, and the inhomogeneous broadening is due to the presence of different low-dimensional structures. Accurate transient carrier cooling curves were extracted from the broadband absorption spectra, and different carrier relaxation regimes were distinguished. Perovskites with x <= 0.71 exhibited extremely fast carrier cooling (300 fs) at low carrier densities (5.0 x 1017 cm-3), however cooling slowed down considerably at high carrier densities (1.3 x 1019 cm-3) due to a "phonon bottleneck" effect (2.8 ps). A kinetic analysis of the electron-hole recombination dynamics provided second-order recombination rate constants in the range (1.5-5.3) x 10-9 cm3 s-1 for a mole fraction up to x = 0.71. Recombination in the LDPs was more than one order of magnitude faster, 6.4 x 10-8 cm3 s-1, which is related to the confined perovskite structure. This should be still slow enough for their application as efficient broadband emitters and solar light harvesting materials.
(1) J. R. Klein, O. Flender, M. Scholz, K. Oum and T. Lenzer, Phys. Chem. Chem. Phys., 2016, 18, 10800.
(2) O. Flender, J. R. Klein, T. Lenzer and K. Oum, Phys. Chem. Chem. Phys., 2015, 17, 19238.
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