Publication date: 15th December 2025
Metal halide perovskites have revolutionized next-generation optoelectronics and photovoltaics due to their exceptional semiconducting properties and low-cost processing.[1] Yet, their widespread deployment remains hindered by long-term instability and the environmental concerns associated with lead-based compositions.[2]To overcome these limitations, low-dimensional (2D) halide perovskites have emerged as promising alternatives based on incorporation of tailored organic spacer cations that enhance structural robustness. Building on this concept, layered double perovskites (LDPs) introduce a lead-free framework based on general formula of S’mAn-1(MIMIII)nX3n+1 (S’ organic spacer cation, A central cation (e.g., Cs+), MI monovalent cation (e.g., Ag+), MIII trivalent cation (e.g., Bi3+, In3+, Cu3+), and X halide anion), forming Ruddelsden-Popper or Dion-Jacobson phases that are comprised of mono (m = 2) or bifunctional (m = 1) organic spacer layers templating inorganic perovskite layers (n).[3] Their properties can be tailored by relying on supramolecular engineering (Figure 1), enabling precise molecular control over their structure and functionality, which remain underexploited.[4] In this work, we develop a new generation of lead-free 2D LDPs through supramolecular design and mechanochemical synthesis, enabling precise molecular control over their structure and functionality. We investigate their structural, electronic, and optical characteristics through a suite of complementary techniques, uncovering key design principles that dictate stability and performance. The versatility of spacer molecules opens pathways not only for more sustainable and stable perovskite photovoltaics, but also for broader optoelectronic applications such as neuromorphic computing.[5]
M.G., M.R.G., M.M., P.K., and J.V.M. appreciate the support from the Research Council of Finland (Project No. 362642). M.R.G. and J.V.M. were supported by the European Research Council (ERC) under the European Union’s Horizon research and innovation programme (Grant agreement No.101114653,SmartHyMat).
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