The growth of methylammonium lead iodide perovskites by close space vapor transport

Vapor deposition processes have shown promise for high-quality perovskite solar cells with potential pathways for scale-up to large area manufacturing. Here, we present a sequential close space vapor transport process to deposit CH3NH3PbI3 (MAPI) perovskite thin films by depositing a layer of PbI2 then reacting it with CH3NH3I (MAI) vapor. We find that, at T = 100 degrees C and pressure = 9 torr, a similar to 225 nm-thick PbI2 film requires >= 125 minutes in MAI vapor to form a fully-reacted MAPI film. Raising the temperature to 160 degrees C increases the rate of reaction, such that MAPI forms within 15 minutes, but with reduced surface coverage. The reaction kinetics can be approximated as roughly first-order with respect to PbI2, though there is evidence for a more complicated functional relation. Perovskite films reacted at 100 degrees C for 150 minutes were fabricated into solar cells with an SLG/ITO/CdS/MAPI/Spiro-OMeTAD/Au structure, and a device efficiency of 12.1% was achieved. These results validate the close space vapor transport process and serve as an advance toward scaled-up, vapor-phase perovskite manufacturing through continuous vapor transport deposition.