期刊
COMMUNICATIONS MATERIALS
卷 2, 期 1, 页码 -出版社
SPRINGERNATURE
DOI: 10.1038/s43246-021-00175-6
关键词
-
资金
- Ministry of Education, Singapore [MOE2014-T3-1-004, MOE2018-T2-1-088, MOE2016-T2-1-052, MOE2019-T2-1-163, MOE2019-T1-002-063]
- NRF-NSFC grant [R-144-000-405-281]
- Institut Teknologi Bandung through the Riset Unggulan Pusat Penelitian ITB 2020 program
- [079 /SP2H/LT/DRPM/2021]
This study investigates the optical and electronic properties of 2D copper-based hybrid perovskites, revealing the presence of the Zhang-Rice singlet state and exotic electronic transitions. Experimental observations and theoretical calculations demonstrate the impact of different alkylammonium spacers on the electronic features and optical responses of the perovskites. The findings provide insights into tuning the properties of hybrid perovskites for efficient photoactive devices.
Intensive effort to tailor photophysics of lead-free perovskites is appealing in recent years. However, their combined electronic and optical property elucidations remain elusive. Here, we report spectroscopic observations of the coexistence Zhang-Rice singlet state and exotic electronic transitions in two-dimensional copper-based perovskites. Herein, several perovskites with different alkylammonium spacers are investigated to unravel their correlated electronic systems and optical responses. Namely, methylammonium, ethylammonium, phenylmethylammonium and phenethylammonium. Using temperature dependent high-resolution X-ray absorption spectroscopy, we observe distinct electronic features highlighting the impact of short spacer chains compared to long-conjugated ligands, demonstrating a pronounced 3d(9) and 3d(9)L signature linewidth variation. Corroborated by density functional theory calculations, the transient dynamics evolution of copper-based hybrid perovskites is influenced by the strong interplay of electron-phonon interactions and geometric constrictions. This finding sheds light on tuning the electronic and optical properties of hybrid perovskites towards efficient photoactive-based devices. Hybrid organic-inorganic perovskites are known to display unique optical properties. Here, electronic transitions in 2D copper-based hybrid perovskites are studied experimentally and theoretically, revealing how ligand size can be used to tune electronic and optical behavior.
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