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Organic-inorganic coupling in the hybrid lead-halide perovskite is a central issue in rationalizing the outstanding photovoltaic performance of these emerging materials. Here we compare and contrast the evolution of structure and dynamics of the hybrid CH3NH3PbBr3 and the inorganic CsPbBr3 lead-halide perovskites with temperature, using Raman spectroscopy and single-crystal X-ray diffraction. Results reveal a stark contrast between their order-disorder transitions, abrupt for the hybrid whereas smooth for the inorganic perovskite. X-ray diffraction observes an intermediate incommensurate phase between the ordered and the disordered phases in CH3NH3PbBr3. Low-frequency Raman scattering captures the appearance of a sharp soft mode in the incommensurate phase, ascribed to the theoretically predicted amplitudon mode. Our work highlights the interaction between the structural dynamics of organic cation CH3NH3+ and the lead-halide framework, and unravels the competition between tendencies of the organic and inorganic moieties to minimize energy in the incommensurate phase of the hybrid perovskite structure.
Behaving like atomically-precise two-dimensional quantum wells with non-negligible dielectric contrast, the layered HOIPs have strong electronic interactions leading to tightly bound excitons with binding energies on the order of 500 meV. These stron
As they combine decent mobilities with extremely long carrier lifetimes, organic-inorganic perovskites have opened a whole new field in opto-electronics. Measurements of their underlying electronic structure, however, are still lacking. Using angle-r
The acoustic phonons in the organic-inorganic lead halide perovskites have been reported to have anomalously short lifetimes over a large part of the Brillouin zone. The resulting shortened mean free paths of the phonons have been implicated as the o
Despite the imperative importance in solar-cell efficiency, the intriguing phenomena at the interface between perovskite solar-cell and adjacent carrier transfer layers are hardly uncovered. Here we show that PbI$_2$/AI-terminated lead-iodide-perovsk
The unprecedented structural flexibility and diversity of inorganic frameworks of layered hybrid halide perovskites (LHHPs) rise up a wide range of useful optoelectronic properties thus predetermining the extraordinary high interest to this family of