We investigated triple-halide perovskite (THP) absorber
layers
with 5 mol % MAPbCl3 added to the double-halide perovskite
(Cs0.22FA0.78)Pb(I0.85Br0.15)3. As a deposition method, a highly scalable printing
technique, slot-die coating, with a subsequent annealing step was
used. We found a strong power conversion efficiency (PCE) dependence
of the corresponding solar cells on the annealing temperature. The
device performance deteriorated when increasing the annealing temperature
from 125 to 170 °C, mainly via losses in the open-circuit voltage
(V
oc) and in the fill factor (FF). To
understand the mechanisms behind this performance loss, extensive
characterizations were performed on both, the THP thin films and the
completed solar-cell stacks, as a function of annealing temperature.
Correlative scanning electron microscopy analyses, i.e., electron
backscatter diffraction, energy-dispersive X-ray spectroscopy, and
cathodoluminescence, in addition to X-ray diffraction and photoluminescence,
confirmed the presence of PbI2 platelets on the surface
of the THP thin films. Moreover, the area fraction of the PbI2 platelets on the film surface increased with increasing annealing
temperature. The deteriorated device performance when the annealing
temperature is increased from 125 to 170 °C is explained by the
increased series resistance and increased interface recombination
caused by the PbI2 platelets, leading to decreased V
oc and FF values of the solar-cell devices.
Thus, the correlative analyses provided insight into microscopic origins
of the efficiency losses.