Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.040
Publication date: 6th July 2018
Three-dimensional lead-halide perovskites combine solution processing with outstanding optoelectronic properties. Despite their soft ionic nature these materials demonstrate a surprisingly low level of electronic disorder. Understanding how structural and dynamic disorder impacts the optoelectronic properties of these perovskites is important for many applications. Here we combine a number of bulk-sensitive and surface-selective spectroscopic techniques to eluscidate the structure and dynamics of organic cations.
We use ultrafast two-dimensional vibrational spectroscopy and molecular dynamics simulations to study the dynamics of the organic cation orientation in a films of pure and mixed tri-halide perovskite materials. For pure MAPbX3 (X=I, Br, Cl) perovskite films, we observe that the cation dynamics accelerate with decreasing size of the halide atom. Much slower dynamics, up to partial immobilisation of the organic cation, are observed in the mixed MAPb(ClxBr1-x)3 and MAPb(BrxI1-x)3 alloys, which we associate with symmetry breaking within the perovskite unit cell.
We also applied surface sensitive vibrtational sum-frequency generation spectroscopy (VSFG) to address the orientation of cations at the perovrkite active layer interfaces with different electron- and hole-extracting materials.We found that at perovskite spiro interface cations are patially immobilised that can be and evidence of high interfacial charge density.
The observed dynamics and structural information are essential for understanding the effects of structural and dynamical disorder in perovskite-based optoelectronics.
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