Proceedings of Online International Conference on Hybrid and Organic Photovoltaics (OnlineHOPV20)
Publication date: 22nd May 2020
The analysis of the temperature dependent EXAFS Debye-Waller factor of chlorine-substituted methylammonium (MA) lead triiodide allows a direct determination of the influence of chlorine substitution on the anharmonicity of the lead-halid bond. In the ordered orthorhombic crystal structure, chlorine substitution leads to a reduction of the anharmonic fraction (cumulant C3) of the radial pair distribution function. Here, the behavior of C3 can be described in a classical approximation by the force constants k0 (harmonic fraction) and k3 (anharmonic fraction). Also, the perpendicular part of the EXAFS Debye-Waller factor σ┴, whose temperature-dependence can be described by the Einstein temperature E (MAPbI3 E = 38.9(5) K; MAPbI2.94Cl0.06 E = 43.3(6) K; MAPbCl3 E = 94(2) K) shows that chlorine substitution in MAPbI3 in the orthorhombic phase leads to a reduction of the anharmonicity. FTIR [1] and quasi-elastic neutron scattering (QENS) [2] studies showed that chlorine substitution has a large influence on the rotational dynamics of the MA molecule in MAPbI3-xClx perovskites[1] since the chlorine substitution leads to a weakening of the hydrogen bridge bonds (these bonds connect the MA molecules with the [PbX6]- octahedra host structure).[2] Here, we discuss the results of the cumulant analysis in the context of the MA molecule rotational dynamics changes due to chlorine substitution, which we already investigated with QENS.
[1] G. Schuck, et. al., J. Phys. Chem. C, 2018, 122, 5227
[2] G. Schuck, et. al., J. Phys. Chem. C, 2019, 123, 11436
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