In this work, the ligand-to-metal charge transition and Förster resonance energy transfer process is exploited to derive lanthanide-organic framework (Tb-cpon) modified perovskite solar cells (PSCs) with enhanced performance under UV irradiation. Tb-cpon-modified PSCs exhibit rapid response and reduced degradation due to energy downconversion facilitated by effective coupling of UV-sensitive chromophores to lanthanide luminescent centers, enhancing the spectral response range of the composite films. Furthermore, the characteristic changes of precursor particle sizes suggest formation of Tb-cpon adducts as intermediate products, leading to enhanced crystallinity and reduced defect concentrations in the Tb-cpon-perovskite hybrid film. Accordingly, the Tb-cpon-modified PSC devices obtain a champion efficiency up to 23.72% as well as a sensitive photovoltaic conversion even under pure UV irradiation. Moreover, the unencapsulated devices maintain more than 80% of the initial efficiency after continuous irradiation under a 310 nm UV lamp for 24 h (from the Au electrode side), compared to 21% for the control devices.
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