Predicting Perovskite Photovoltaics Performance

Wide band gap FA_0.8Cs_0.2Pb(I_0.6Br_0.4)₃ perovskite photovoltaic (PV) devices are measured by spectroscopic ellipsometry in the through-the-glass configuration and analyzed to determine the complex optical property spectra of the perovskite absorber as well as the structural properties of all constituent layers. This information is used to simulate external quantum efficiency (EQE) spectra, to calculate PV device performance parameters such as short circuit current density, open circuit voltage, fill factor, and power conversion efficiency, and to develop strategies for increasing the accuracy of predictions. Simulations and calculations tend to overestimate PV device performance parameters, undermining the accuracy and usefulness of those simulations. Mapping spectroscopic ellipsometry measurements of an incomplete device are also collected from the perovskite film side to obtain layer thicknesses, perovskite band gap energies, and Urbach energies at each mapping point. The incomplete device stacks feature the perovskite absorber as the final deposited layer, while the complete devices add electron transport layers and silverback electrical contacts. When simulations are based on structural and optical properties obtained from spectroscopic ellipsometry measurements of incomplete PV device stacks, further inaccuracies arise as characteristics of the exposed perovskite film are not necessarily the same as those of an absorber in a complete, protected PV device. Predictions for PV performance parameters fall within 5% of the experiment for three of four baseline devices. The usefulness of this is apparent in situations where experimentally measuring PV device performance is unfeasible or overly tedious, as well as during intermediate steps during production.