A method for making a layered perovskite structure comprises: a) performing a vapor assisted surface treatment (VAST) of a substrate with a surface passivating agent; b) applying a layer of PbI2 to the passivating agent; c) exposing the PbI2 to methylammonium iodide (CH3NH3I) in an orthogonal solvent; and d) annealing the structure. A PEDOT:PSS coated ITO glass substrate may be used. The surface passivation agent may be one a chalcogenide-containing species with the general chemical formula (E3E4)N(E1E2)N′C═X where any one of E1, E2, E3 and E4 is independently selected from C1-C15 organic substituents comprising from 0 to 15 heteroatoms or hydrogen, and X is S, Se or Te, thiourea, thioacetamide, selenoacetamide, selenourea, H2S, H2Se, H2Te or LXH wherein L is a Cn organic substituent comprising heteroatoms and X═S, Se, or Te. The passivating agent may be applied by spin-coating, inkjet-printing, slot-die-coating, aerosol-jet printing, PVD, CVD, and electrochemical deposition.
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