Remnant PbI2, an unforeseen necessity in high-efficiency hybrid perovskite-based solar cells?

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Abstract
Perovskite-containing solar cells were fabricated in a two-step procedure in which PbI2 is deposited via spin-coating and subsequently converted to the CH3NH3PbI3 perovskite by dipping in a solution of CH3NH3I. By varying the dipping time from 5 s to 2 h, we observe that the device performance shows an unexpectedly remarkable trend. At dipping times below 15 min the current density and voltage of the device are enhanced from 10.1 mA/cm2 and 933 mV (5 s) to 15.1 mA/cm2 and 1036 mV (15 min). However, upon further conversion, the current density decreases to 9.7 mA/cm2 and 846 mV after 2 h. Based on X-ray diffraction data, we determined that remnant PbI2 is always present in these devices. Work function and dark current measurements showed that the remnant PbI2 has a beneficial effect and acts as a blocking layer between the TiO2 semiconductor and the perovskite itself reducing the probability of back electron transfer (charge recombination). Furthermore, we find that increased dipping time leads to an increase in the size of perovskite crystals at the perovskite-hole-transporting material interface. Overall, approximately 15 min dipping time (∼2% unconverted PbI2) is necessary for achieving optimal device efficiency.
Funding Information
  • DOE (DE-SC0001059)

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