4.2 Article

Revealing Weak Dimensional Confinement Effects in Excitonic Silver/Bismuth Double Perovskites

Journal

JACS AU
Volume 2, Issue 1, Pages 136-149

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jacsau.1c00429

Keywords

halide perovskite; lead-free perovskites; low-dimensional perovskites; electron-phonon coupling; Cs-based perovskites; quantum confinement; nontoxic perovskites

Funding

  1. European Union [EFRE-0800120, NW-1-1-040h]
  2. Deutsche Forschungsgemeinschaft [424708448]
  3. COMETE project (COnception in silico de Materiaux pour l'EnvironnemenT et l'Energie) - European Union under the program FEDER-FSE Lorraine et Massif des Vosges 2014-2020
  4. Zenobe/CENAERO (Walloon region) [1117545]
  5. European Research Council (ERC) Starting Grant 2018 under the European Union's Horizon 2020 research and innovation programme [802862]
  6. Fondazione Cariplo-Progetto Economia Circolare 2020 [2020-1067]

Ask authors/readers for more resources

Lead-free perovskites with lower dimensionality, such as (PEA)4AgBiBr8 and (PEA)2CsAgBiBr7, exhibit strong excitonic effects and a large Stokes shift, attributed to the soft character of the double-perovskite lattices. These findings have implications for the use of double perovskites in light-emitting applications, highlighting their potential in advanced optoelectronic devices.
Lead-free perovskites are attracting increasing interest as nontoxic materials for advanced optoelectronic applications. Here, we report on a family of silver/bismuth bromide double perovskites with lower dimensionality obtained by incorporating phenethylammonium (PEA) as an organic spacer, leading to the realization of two-dimensional double perovskites in the form of (PEA)(4)AgBiBr8 (n = 1) and the first reported (PEA)(2)CsAgBiBr7 (n = 2). In contrast to the situation prevailing in lead halide perovskites, we find a rather weak influence of electronic and dielectric confinement on the photophysics of the lead-free double perovskites, with both the 3D Cs2AgBiBr6 and the 2D n = 1 and n = 2 materials being dominated by strong excitonic effects. The large measured Stokes shift is explained by the inherent soft character of the double-perovskite lattices, rather than by the often-invoked band to band indirect recombination. We discuss the implications of these results for the use of double perovskites in light-emitting applications.

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