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The hybrid halide perovskites MAPbI$_{3}$, MAPbI$_{2.94}$Cl$_{0.06}$, andMAPbCl$_{3}$ (MA - methylammonium) have been investigated using inelastic andquasielastic neutron scattering (QENS) with the aim of elucidating the impactof chloride substitution on the rotational dynamics of MA. In this context, wediscuss the influence of the inelastic neutron scattering caused by low-energyphonons on the QENS resulting from the MA rotational dynamics inMAPbI$_{3-x}$Cl$_{x}$. Through a comparative temperature-dependent QENSinvestigation with different energy resolutions, which allow a wide Fouriertime window, we achieved a consistent description of the influence of chlorinesubstitution in MAPbI$_{3}$ on to the MA dynamics. Our results show thatchlorine substitution in the low temperature orthorhombic phase leads to aweakening of the hydrogen bridge bonds since the characteristic relaxationtimes of C$_{3}$ rotation at 70 K in MAPbCl$_{3}$ (135 ps) andMAPbI$_{2.94}$Cl$_{0.06}$ (485 ps) are much shorter than in MAPbI$_{3}$ (1635ps). For the orthorhombic phase, we obtained the activation energies from thetemperature-dependent characteristic relaxation times ${\tau}$C$_{3}$ byArrhenius fits indicating lower values of E$_{a}$ for MAPbCl$_{3}$ andMAPbI$_{2.94}$Cl$_{0.06}$ compared to MAPbI$_{3}$. We also performed QENSanalyses at 190 K for all three samples. Here we observed that MAPbCl$_{3}$shows slower MA rotational dynamics than MAPbI$_{3}$ in the disorderedstructure.

Influence of Chloride Substitution on the Rotational Dynamics of Methylammonium in MAPbI$_{3-x}$Cl$_{x}$ Perovskites