Proceedings of nanoGe Spring Meeting 2022 (NSM22)
DOI: https://doi.org/10.29363/nanoge.nsm.2022.321
Publication date: 7th February 2022
Investigating halide perovskites’ optoelectronics properties for stimuli-responsive materials (SRMs) opens new avenues in smart chromic windows, switchable optoelectronics, and information display applications. Here, we carried out an in-depth study of the structural transformation of FAn+2PbnBr3n+2 (2≤ n ≤∞) layered halide perovskite using excess organic cation (FA/Pb>1), strain, optical and thermal input. Initially as FA/Pb ratio increases, three-dimensional (3D, FA/Pb=1, n=∞) (FAPbBr3) perovskite transform to two-dimensional (2D, FA/Pb=1, n=2) (FA2PbBr4) layered halide perovskite and is aligned in <110> orientation. The intermediate n phases (2≤ n ≤∞) in FAn+2PbnBr3n+2 system stabilize in metastable states and are accessible via strain, optical or thermal input. These results were supported by X-ray diffraction, solid-state nuclear magnetic response (ssNMR), in-situ temperature-dependent Raman spectroscopy, optical spectroscopy, and ab initio simulation techniques. Furthermore, upon photo-decomposition of FABr, the <110> oriented 2D perovskite transforms to 3D perovskite. Therefore, a metal oxide mesoporous substrate has been introduced to prevent FA decomposition and impart reversibility (2D to 3D and vice versa), which facilitate as a reservoir for FA cations. Shuttling of FABr between the reservoir and the HP film under light and moisture ensure reversible chromism. We realised that the transformation in the FAn+2PbnBr3n+2 structure is governed by the H-bonds strength of the intermediate n phase (lower n phases to higher n phases or vice versa). Additionally, the remnant organic solvent in the film (observed using proton transfer reaction-mass spectroscopy (PTR-MS)) is crucial to realize structural transformation and, therefore, the reversible chromism. Finally, we relate photo-induced reconfigurability with photo-adaptable intelligent sensors. The realization of structural configurability using just one cation is not only employable in solar cells and LEDs but simultaneously can be utilized in artificially intelligent sensors by optimizing their operating parameters according to the ambient environment.
Reversible photochromism in <110> oriented layered halide perovskiteReversible photochromism in <110> oriented layered halide perovskiteReversible photochromism in <110> oriented layered halide perovskiteThis research was funded by National Research Foundation, Prime Minister’s Office, Singapore under its Competitive Research Programme (CRP Award No. NRF-CRP14-2014-03) and Ministry of Education, Singapore (MOE2019-T2-2-097). We would also like to acknowledge the NTU Centre of High Field NMR Spectroscopy and Imaging for the use of their NMR facilities. PTR-MS characterization was supported by the National Research Foundation (NRF), Prime Minister's Office, Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) programme through the eCO2EP project operated by the Cambridge Centre for Advanced Research and Education in Singapore (CARES) and the Berkeley Educational Alliance for Research in Singapore (BEARS).
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