Abstract
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 3d9 and 3d9L 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.
Highlights
Intensive effort to tailor photophysics of lead-free perovskites is appealing in recent years
Apart from those well-known absorption electronic transitions, we observed other emergent peaks that centered at ~936.6 eV, ~939.9 eV, ~942.4 eV, and ~946.0 eV labeled as A1-A4, respectively
We tentatively proposed that the additional –CH2 moiety span the organic ligand length inducing extra s states in this lead-free correlated hybrid perovskite electronic system
Summary
Intensive effort to tailor photophysics of lead-free perovskites is appealing in recent years. 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. 1234567890():,; Two-dimensional hybrid organic–inorganic perovskites (2DHOIPs) materials have demonstrated promising progress in photovoltaics and light-emitting diodes applications, such as their excellent performance as active-light absorbers and carrier transporters[1,2,3,4,5]. These materials deserve special attention in the field of unconventional 2D hybrid materials due to their tunable dielectric confinements, charge carrier dynamics, and their structural diversities. Polyakov et al.[22] and Nugroho et al.[23] investigated copper-based
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