A-Site Management for Highly Crystalline Perovskites
© 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 32(2020), 4 vom: 23. Jan., Seite e1904702 |
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1. Verfasser: | |
Weitere Verfasser: | , , , , , , , , |
Format: | Online-Aufsatz |
Sprache: | English |
Veröffentlicht: |
2020
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Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
Schlagworte: | Journal Article A-site management A-site-related defects highly crystalline perovskites placeholder cations transient phases |
Zusammenfassung: | © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. An in-depth understanding and effective suppression of nonradiative recombination pathways in perovskites are crucial to their crystallization process, in which supersaturation discrepancies at different time scales between CH3 NH3 I (MAI, methylammonium iodide) and PbI2 remain a key issue. Here, an A-site management strategy via the introduction of an A-site placeholder cation, NH4 + , to offset the deficient MA+ precipitation by occupying the cavity of Pb-I framework, is proposed. The temporarily remaining NH4 + is substituted by subsequently precipitated MA+ . The temperature-dependent crystallization process with the generation and consumption of a transient phase is sufficiently demonstrated by the dynamic changes in crystal structure characteristic peaks through in situ grazing-incidence X-ray diffraction and the surface potential difference evolution through temperature-dependent Kelvin probe force microscopy. A highly crystalline perovskite is consequently acquired, indicated by the enlarged grain size, lowered nonradiative defect density, prolonged carrier lifetime, and fluorescence lifetime imaging. Most importantly, it is identified that the A-site IMA defect is responsible for such crystal quality optimization based on theoretical calculations, transient absorption, and deep-level transient spectroscopy. Furthermore, the universality of the proposed A-site management strategy is demonstrated with other mixed-cation perovskite systems, indicating that this methodology successfully provides guidance for synthesis route design of highly crystalline perovskites |
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Beschreibung: | Date Completed 29.01.2020 Date Revised 30.09.2020 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
ISSN: | 1521-4095 |
DOI: | 10.1002/adma.201904702 |