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Decoupled Molecular and Inorganic Framework Dynamics in CH3NH3PbCl3



M. Songvilay, Zitian Wang, Victoria Garcia Sakai, T. Guidi, M. Bari, Zuo-Guang Ye, Guangyong Xu, K. L. Brown, Peter M. Gehring, Christopher Stock


The organic-inorganic lead halide perovskites are composed of organic molecules embedded in an inorganic framework. The compounds with general formula CH3NH3PbX3 (MAPbX2) display large photovoltaic efficiencies for halogens X=Cl, Br, and I in a wide variety of sample geometries and preparation methods. The organic cation and inorganic framework are bound by hydrogen bonds that tether the molecules to the halide anions, and this has been suggested to be important to the optoelectronic properties. We have studied the effects of this bonding using time-of-flight neutron spectroscopy to measure the molecular dynamics in CH3NH3PbCl3 (MAPbCl3). Low-energy/high-resolution neutron backscattering reveals thermally-activated molecular dynamics with a characteristic temperature of 95 K. At this same temperature, higher-energy neutron spectroscopy indicates the presence of an anomalous broadening in energy (reduced lifetime) associated with the molecular vibrations. By contrast, neutron powder diffraction shows that a spatially long-range structural phase transitions occurs at 178K (cubic to tetragonal) and 173K (tetragonal to orthorhombic). The large difference between these two temperature scales suggests that the molecular and inorganic lattice dynamics in MAPbCl3 are actually decoupled. With the assumption that underlying physical mechanisms do not change with differing halogens in the organic-inorganic perovskites, we speculate that the energy scale most relevant to the photovoltaic properties of the lead-halogen perovskites is set by the lead-halide bond, not by the hydrogen bond.
Physical Review Materials


Photovoltaic, perovskites, lattice dynamics, neutron scattering, quasielastic scattering


Songvilay, M. , Wang, Z. , Garcia Sakai, V. , Guidi, T. , Bari, M. , Ye, Z. , Xu, G. , Brown, K. , Gehring, P. and Stock, C. (2019), Decoupled Molecular and Inorganic Framework Dynamics in CH<sub>3</sub>NH<sub>3</sub>PbCl<sub>3</sub>, Physical Review Materials, [online], (Accessed June 12, 2024)


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Created December 29, 2019, Updated October 12, 2021