Pulsed Laser Deposition of CsPbBr3 Films: Impact of the Composition of the Target and Mass Distribution in the Plasma Plume

All-inorganic cesium lead bromine (CsPbBr3) perovskites have gained a tremendous potential in optoelectronics due to interesting photophysical properties and much better stability than the hybrid counterparts. Although pulsed laser deposition (PLD) is a promising alternative to solvent-based and/or thermal deposition approaches due to its versatility in depositing multi-elemental materials, deep understanding of the implications of both target composition and PLD mechanisms on the properties of CsPbBr3 films is still missing. In this paper, we deal with thermally assisted preparation of mechano-chemically synthesized CsPbBr3 ablation targets to grow CsPbBr3 films by PLD at the fluence 2 J/cm2. We study both Cs rich- and stoichiometric PbBr2-CsBr mixture-based ablation targets and point out compositional deviations of the associated films resulting from the mass distribution of the PLD-generated plasma plume. Contrary to the conventional meaning that PLD guarantees congruent elemental transfer from the target to the substrate, our study demonstrates cation off-stoichiometry of PLD-grown CsPbBr3 films depending on composition and thermal treatment of the ablation target. The implications of the observed enrichment in the heavier element (Pb) and deficiency in the lighter element (Br) of the PLD-grown films are discussed in terms of optical response and with the perspective of providing operative guidelines and future PLD-deposition strategies of inorganic perovskites.