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

^aLaboratory of Nanotechnology and Solar Energy, Institute of Chemistry, University of Campinas – UNICAMP, P.O. Box 6154, Campinas, 13083-970, Brazil

^bUniversidade Federal de Minas Gerais, Departamento de Química, Institudo de Ciencias Exatas, Brazil, Belo Horizonte - Minas Gerais, 31270-901, Brasil, Brazil

^cSLAC National Accelerator Laboratory, Stanford Synchrotron Radiation Lightsource, Menlo Park, California, EE. UU., Menlo Park, United States

^dDepartment of Applied Physics, Stanford University, Stanford, California, EE. UU., Stanford, United States

^eCavendish Laboratory, University of Cambridge - UK, JJ Thomson Avenue, 9, Cambridge, United Kingdom

NIPHO
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
DOI: https://doi.org/10.29363/nanoge.nipho.2020.043
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.

Acknowledgements:

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

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