Publication date: 8th July 2026
In recent years, perovskites have emerged as promising candidates for next-generation scintillators [1] owing to their structural versatility, tunable electronic properties, and efficient radiative processes [2, 3]. While Pb-based systems have been extensively investigated [4], the optical and scintillation properties of Pb-free Ni-based layered perovskites remain largely underexplored. In this work, we present a comprehensive experimental and theoretical study of the Ni-based perovskite family (A)2NiCl4, where A = phenylmethylammonium (PMA), phenylethylammonium (PEA), and phenylpropylammonium (PPA).
High-quality single crystals were synthesized and structurally characterized by X-ray diffraction, confirming their layered crystal structure and excellent crystallinity. Their optical properties were investigated using photoacoustic spectroscopy, photoluminescence, and radioluminescence measurements, while density functional theory calculations were employed to elucidate the electronic structure. Two characteristic optical features were identified across the series: a high-energy emission centered at approximately 300 nm, attributed to ligand-surface-related states, and a broad band near 500 nm originating from Ni-derived d-states that define the electronic bandgap of these materials. The combined experimental and theoretical results demonstrate that both the inorganic [NiCl4]2- layers and the organic spacer cations govern the electronic structure and radiative recombination pathways.
Radioluminescence measurements reveal that (PPA)2NiCl4 exhibits the most promising scintillation performance, achieving a light yield of approximately 23,000 photons/MeV at 80 K [5]. The observed dependence of the optical response on the organic cation highlights the effectiveness of A-site engineering for tailoring the scintillation properties of layered hybrid perovskites. These findings establish Pb-free Ni-based perovskites as a promising platform for environmentally friendly low-temperature scintillators and provide new insights into the relationship between crystal structure, electronic states, and luminescence mechanisms in hybrid perovskite materials.
All authors acknowledge research funds from the National Science Center, Poland, under grant OPUS-24 no. 2022/47/B/ST5/01966. This research is funded by the Indonesian Endowment Fund for Education (LPDP) on behalf of the Indonesian Ministry of Higher Education, Science and Technology and managed under the EQUITY Program (Contract No. 4298/B3/DT.03.08/2025). All authors acknowledge Sri Hartati who was responsible for the Rietveld analysis.
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