Synthesis of Polycrystalline Ruddlesden-Popper Organic Lead Halides and Their Growth Dynamics
Ana Flavia Nogueira a, Raphael F. Moral a, Luiz Gustavo Bonato a, José Carlos Germino a, Willian Xerxes de Oliveira Coelho b, §Rupini Kamat c, Junwei Xu c, Christopher J. Tassone c, Michael F. Toney c, Rupini Kamat d, Samuel D. Stranks e
a Laboratory of Nanotechnology and Solar Energy, Institute of Chemistry, University of Campinas – UNICAMP, P.O. Box 6154, Campinas, 13083-970, Brazil
b Departamento de Química, Institudo de Ciencias Exatas, Universidade Federal de Minas Gerais, Belo Horizonte 31270-901, Minas Gerais, Brazil
c SLAC National Accelerator Laboratory, Stanford Synchrotron Radiation Lightsource, Menlo Park, California 94025, United States
d Department of Applied Physics, Stanford University, Stanford, California 94305, United States
e Cavendish Laboratory, University of Cambridge, 19 JJ Thomson Avenue, Cambridge CB3 0HE, United Kingdom
nanoGe Perovskite Conferences
Proceedings of International Conference on Perovskite Thin Film Photovoltaics and Perovskite Photonics and Optoelectronics (NIPHO20)
Sevilla, Spain, 2020 February 23rd - 25th
Organizer: Hernán Míguez
Oral, Ana Flavia Nogueira, presentation 043
Publication date: 25th November 2019

In this talk, we will present a new synthetic method for Ruddlesden-Popper Organic Lead Halides (RPOLHs). This new protocol allows a low-cost, room-temperature preparation of polycrystalline materials with general composition L2[FAPbI3]n-1PbI4, where L is a primary ammonium cation, FA is formamidinium [HC(NH2)2]+, and n is the number of inorganic octahedron slabs. The butylammonium-based materials presented phase purity above 99% and, in the benzylammonium-based one, some impurities are present in the final product. These polycrystalline materials are easily processed and can be used for thin film fabrication, which is appealing for optoelectronic devices.

In addition to the new synthesis, we also studied the reaction dynamics of one of the materials in situ. We used small angle X-ray scattering (SAXS) to probe the initial and final stages of the formation reaction of BA2[FAPbI3]PbI4. Our results suggest that the formation of the individual slabs is quite fast (within the first 10 s) and, then, these slabs self-assemble into bulk crystallites during the next 40 minutes. By analyzing the variation of the reciprocal space with time and relating these changes with the Scherrer equation, we could calculate the rate and the average velocity of this self-assemble of the slabs. This work offers the material community a new avenue for the synthesis and investigation of RPOLHs, as well as the possibility of their utilization for optoelectronic devices.

Fapesp, Shell, CNPq, INEO (Instituto Nacional de Eletrônica Orgânica) and CNPEM.

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