Hempel, H.; Savenjie, T.J.; Stolterfoht, M.; Neu, J.; Failla, M.; Paingad, V.C.; Kuzel, P.; Heilweil, E.J.; Spies, J.A.; Schleuning, M.; Zhao, J.; Friedrich, D.; Schwarzburg, K.; Siebbeles, L.D.A.; Dörflinger, P.; Dyakonov, V.; Katoh, R.; Hong, M.J.; Labram, J.G.; Monti, M.; Butler-Caddle, E.; Lloyd-Hughes, J.; Taheri, M.M.; Baxter, J.B.; Magnanelli, T.J.; Luo, S.; Cardon, J.M.; Ardo, S.; Unold, T.: Predicting Solar Cell Performance from Terahertz and Microwave Spectroscopy. Advanced Energy Materials 12 (2022), p. 2102776/1-16
10.1002/aenm.202102776
Open Access Version
Abstract:
Mobilities and lifetimes of photogenerated charge carriers are core properties of photovoltaic materials and can both be characterized by contactless terahertz or microwave measurements. Here, the expertise from fifteen laboratories is combined to quantitatively model the current-voltage characteristics of a solar cell from such measurements. To this end, the impact of measurement conditions, alternate interpretations, and experimental inter-laboratory variations are discussed using a (Cs,FA,MA)Pb(I,Br)3 halide perovskite thin-film as a case study. At 1 sun equivalent excitation, neither transport nor recombination is significantly affected by exciton formation or trapping. Terahertz, microwave, and photoluminescence transients for the neat material yield consistent effective lifetimes implying a resistance-free JV-curve with a potential power conversion efficiency of 24.6 %. For grainsizes above ≈20 nm, intra-grain charge transport is characterized by terahertz sum mobilities of ≈32 cm2 V−1 s−1. Drift-diffusion simulations indicate that these intra-grain mobilities can slightly reduce the fill factor of perovskite solar cells to 0.82, in accordance with the best-realized devices in the literature. Beyond perovskites, this work can guide a highly predictive characterization of any emerging semiconductor for photovoltaic or photoelectrochemical energy conversion. A best practice for the interpretation of terahertz and microwave measurements on photovoltaic materials is presented.