Weis, Andreas ; Ganswindt, Patrick ; Kaiser, Waldemar ; Illner, Hannah ; Maheu, Clément ; Glück, Nadja ; Dörflinger, Patrick ; Armer, Melina ; Dyakonov, Vladimir ; Hofmann, Jan P. ; Mosconi, Edoardo ; De Angelis, Filippo ; Bein, Thomas (2022)
Heterovalent Tin Alloying in Layered MA₃Sb₂I₉ Thin Films: Assessing the Origin of Enhanced Absorption and Self-Stabilizing Charge States.
In: The Journal of Physical Chemistry C, 126 (49)
doi: 10.1021/acs.jpcc.2c06106
Artikel, Bibliographie

Kurzbeschreibung (Abstract)

Heteroatom alloying of lead-free perovskite derivatives is a highly promising route to tailor their optoelectronic properties and stability for multiple applications. Here, we demonstrate the facile solution-based synthesis of Sn-alloyed layered MA₃Sb₂I₉ thin films by precursor engineering, combining acetate and halide salts. An increasing concentration of tin halides in different oxidation states leads to a strong boost in absorption over the whole visible spectrum. We demonstrate phase-pure synthesis and elucidate the heterovalent incorporation of Sn into the MA₃Sb₂I₉ lattice, proving the formation of additional electronic states in the bandgap by theoretical calculations. On this basis, we dissect the strong absorption increase into three components that we attribute to intervalence and heteroatom-induced interband absorption. Finally, we show the charge-stabilizing effect of the system through robustness toward precursors in mixed oxidation states and trace the improved ambient stability of this material back to this feature.

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