Publication date: 15th December 2025
The stability of perovskite materials remains one of the central challenges for their practical implementation. While lead halide perovskites often degrade under mild thermal or environmental stress, our recent work on their metal-free analogues reveals a very different picture. These fully molecular perovskite frameworks, composed entirely of organic cations and halide anions, display an unexpected structural resilience that challenges common assumptions about the fragility of organic lattices.
In this talk, I will discuss how mechanosynthesis, i.e., the solvent-free synthesis of solids through controlled mechanical impact, acts not only as a sustainable preparation method but also as a tool to encode different structural states and defect landscapes into MFPs. By tuning the milling frequency, we access materials with distinct microstrain and metastability, whose responses to temperature reveal the interplay between processing history and intrinsic lattice resilience.
Temperature-dependent synchrotron X-ray diffraction (T-XRD) and differential scanning calorimetry (DSC) provide complementary perspectives on these transformations. The diffraction data show that mechanochemically generated strain strongly influences the thermal evolution of DABCONH₄X₃ (X = Cl, Br, I): samples produced under lower-energy milling undergo cooperative phase rearrangements on first heating, whereas those prepared at higher energy relax gradually through defect annealing and domain coarsening. Despite these transformations, the perovskite frameworks remain crystalline and recover their symmetry without decomposition.
Subtle variations in peak broadening and line-shape asymmetry indicate microstructural healing rather than breakdown, pointing to hydrogen-bond-mediated flexibility as a stabilizing factor. Together, these results highlight mechanosynthesis as a powerful platform for directing phase stability and show that all-organic perovskites can be more resilient than expected, an observation that redefines the boundaries of structural robustness in organic-based perovskite materials.
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