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Serpetzoglou E, Konidakis I, Kourmoulakis G, Demeridou I, Chatzimanolis K et al. Charge carrier dynamics in different crystal phases of CH3NH3PbI3 perovskite. Opto-Electron Sci 1, 210005 (2022). doi: 10.29026/oes.2022.210005
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Original Article Open Access
Charge carrier dynamics in different crystal phases of CH3NH3PbI3 perovskite
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Abstract
Despite that organic-inorganic lead halide perovskites have attracted enormous scientific attention for energy conversion applications over the recent years, the influence of temperature and the type of the employed hole transport layer (HTL) on the charge carrier dynamics and recombination processes in perovskite photovoltaic devices is still largely unexplored. In particular, significant knowledge is missing on how these crucial parameters for radiative and non-radiative recombinations, as well as for efficient charge extraction vary among different perovskite crystalline phases that are induced by temperature variation. Herein, we perform micro photoluminescence (μPL) and ultrafast time resolved transient absorption spectroscopy (TAS) in Glass/Perovskite and two different Glass/ITO/HTL/Perovskite configurations at temperatures below room temperature, in order to probe the charge carrier dynamics of different perovskite crystalline phases, while considering also the effect of the employed HTL polymer. Namely, CH3NH3PbI3 films were deposited on Glass, PEDOT:PSS and PTAA polymers, and the developed Glass/CH3NH3PbI3 and Glass/ITO/HTL/CH3NH3PbI3 architectures were studied from 85 K up to 215 K in order to explore the charge extraction dynamics of the CH3NH3PbI3 orthorhombic and tetragonal crystalline phases. It is observed an unusual blueshift of the bandgap with temperature and the dual emission at temperature below of 100 K and also, that the charge carrier dynamics, as expressed by hole injection times and free carrier recombination rates, are strongly depended on the actual pervoskite crystal phase, as well as, from the selected hole transport material. -
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References
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Supplementary information for Charge carrier dynamics in different crystal phases of CH3NH3PbI3 perovskite
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Serpetzoglou E, Konidakis I, Kourmoulakis G, Demeridou I, Chatzimanolis K et al. Charge carrier dynamics in different crystal phases of CH3NH3PbI3 perovskite. Opto-Electron Sci 1, 210005 (2022). doi: 10.29026/oes.2022.210005
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Figure 1.
μPL spectra following excitation at 543 nm of the (a) Glass/CH3NH3PbI3, (b) Glass/ITO/PEDOT:PSS/CH3NH3PbI3 and (c) Glass/ITO/PTAA/CH3NH3PbI3 architectures.
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Figure 2.
Shift of the μPL emission peak as a function of temperature for (a) Glass/CH3NH3PbI3, (b) Glass/ITO/PEDOT:PSS/CH3NH3PbI3 and (c) Glass/ITO/PTAA/CH3NH3PbI3 architectures for the orthorhombic (red solid circles) and tetragonal (blue solid circles) perovskite crystal phases.
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Figure 3.
FWHM of the PL peaks corresponding to the orthorhombic (black diamonds) and tetragonal (red circles) phases of CH3NH3PbI3 as a function of temperature (a) Glass/CH3NH3PbI3, (b) Glass/ITO/PEDOT:PSS/CH3NH3PbI3 and (c) Glass/ITO/PTAA/CH3NH3PbI3. Green solid lines show the fitting acquired by the temperature-independent inhomogeneous broadening (Γ0) and the interaction between charge carriers and longitudinal optical phonons (LO-phonons), as described by the Fröhlich Hamiltonian.
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Figure 4.
Optical density (ΔOD) vs. wavelength at various delay times for Glass/ITO/PEDOT:PSS/CH3NH3PbI3 architecture at (a) 85 K, (b) 120 K and (c) 180 K.
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Figure 5.
Optical density ΔOD vs. wavelength at various delay times for Glass/ITO/PTAA/CH3NH3PbI3 configuration at (a) 85 K, (b) 120 K and (c) 180 K.
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Figure 6.
Optical density (ΔOD) peaks wavelength as a function of temperature for Glass/ITO/PEDOT:PSS/CH3NH3PbI3 architecture and Glass/ITO/PTAA/CH3NH3PbI3 configurations, as extracted from TAS spectra at t = 0 ps (see Fig. 4 and Fig. 5 blue lines).
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Figure 7.
Normalized optical density (ΔOD) vs. delay time for Glass/ITO/PEDOT:PSS/CH3NH3PbI3 and Glass/ITO/PTAA/CH3NH3PbI3 configurations for the orthorhombic phase at (a) 85 K, (b) 120 K and for the tetragonal phase at (c) 120 K and (d) 180 K. Symbols present the transient band edge bleach kinetics, while solid lined present the decay exponential fitting. Insets are shown the initial time scale for Glass/ITO/PTAA/CH3NH3PbI3.
