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The lead-halide perovskites, including CH$_{3}$NH$_{3}$PbBr$_{3}$, are components in cost effective, highly efficient photovoltaics, where the interactions of the molecular cations with the inorganic framework are suggested to influence the electronic and ferroelectric properties. CH$_{3}$NH$_{3}$PbBr$_{3}$ undergoes a series of structural transitions associated with orientational order of the CH$_{3}$NH$_{3}$ (MA) molecular cation and tilting of the PbBr$_{3}$ host framework. We apply high-resolution neutron scattering to study the soft harmonic phonons associated with these transitions, and find a strong coupling between the PbBr$_{3}$ framework and the quasistatic CH$_{3}$NH$_{3}$ dynamics at low energy transfers. At higher energy transfers, we observe a PbBr$_{6}$ octahedra soft mode driving a transition at 150 K from bound molecular excitations at low temperatures to relatively fast relaxational excitations that extend up to $sim$ 50-100 meV. We suggest that these temporally overdamped dynamics enables possible indirect band gap processes in these materials that are related to the enhanced photovoltaic properties.
Halide perovskite (HP) semiconductors exhibit unique strong coupling between the electronic and structural dynamics. The high-temperature cubic phase of HPs is known to be entropically stabilized, with imaginary frequencies in the calculated phonon d
Hybrid halide perovskites exhibit nearly 20% power conversion efficiency, but the origin of their high efficiency is still unknown. Here, we compute the shift current, a dominant mechanism of bulk photovoltaic (PV) effect for ferroelectric photovolta
We measure temperature-dependent one-photon and two-photon induced photoluminescence from (CH3NH3)PbBr3 single crystals cleaved in ultrahigh vacuum. An approach is presented to extract absorption spectra from a comparison of both measurements. Cleave
We report the spontaneous decay of a soft, optical phonon in a solid. Using neutron spectroscopy, we find that specific phonon lifetimes in the relaxor PbMg$_{1/3}$Nb$_{2/3}$O$_{3}$ are anomalously short within well-defined ranges of energy and momen
Reflection and transmission as a function of temperature have been measured on a single crystal of the magnetoelectric ferrimagnetic compound Cu$_{2}$OSeO$_{3}$ utilizing light spanning the far infrared to the visible portions of the electromagnetic