Angewandte Chemie - International Edition
Angewandte Chemie - International Edition
5 years ago

The Nature of Ion Conduction in Methylammonium Lead Iodide: A Multimethod Approach

The Nature of Ion Conduction in Methylammonium Lead Iodide: A Multimethod Approach
Michael Grätzel, Gee Yeong Kim, Alessandro Senocrate, Tae-Youl Yang, Giuliano Gregori, Igor Moudrakovski, Joachim Maier
By applying a multitude of experimental techniques including 1H, 14N, 207Pb NMR and 127I NMR/NQR, tracer diffusion, reaction cell and doping experiments, as well as stoichiometric variation, conductivity, and polarization experiments, iodine ions are unambiguously shown to be the mobile species in CH3NH3PbI3, with iodine vacancies shown to represent the mechanistic centers under equilibrium conditions. Pb2+ and CH3NH3+ ions do not significantly contribute to the long range transport (upper limits for their contributions are given), whereby the latter exhibit substantial local motion. The decisive electronic contribution to the mixed conductivity in the experimental window stems from electron holes. As holes can be associated with iodine orbitals, local variations of the iodine stoichiometry may be fast and enable light effects on ion transport. Keep calm and carry charge: Using NMR/NQR techniques, tracer diffusion, reaction cell, and doping experiments, as well as stoichiometric variation, conductivity, and polarization experiments, iodine ions are shown to be the mobile species in CH3NH3PbI3, with iodine vacancies being the mechanistic centers under equilibrium conditions. The decisive electronic contribution to the mixed conductivity stems is shown to be from electron holes.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201701724

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