Insights from transient absorption spectroscopy into electron dynamics along the Ga-gradient in Cu(In,Ga)Se2 solar cells

Abstract

Cu(In,Ga)Se2 solar cells have markedly increased their efficiency over the last decades currently reaching a record power conversion efficiency of 23.3%. Key aspects to this efficiency progress are the engineered bandgap gradient profile across the absorber depth, along with controlled incorporation of alkali atoms via post-deposition treatments. Whereas the impact of these treatments on the carrier lifetime has been extensively studied in ungraded Cu(In,Ga)Se2 films, the role of the Ga-gradient on carrier mobility has been less explored. Here, transient absorption spectroscopy (TAS) is utilized to investigate the impact of the Ga-gradient profile on charge carrier dynamics. Minority carriers excited in large Cu(In,Ga)Se2 grains with a [Ga]/([Ga]+[In]) ratio between 0.2–0.5 are found to drift-diffuse across ≈1/3 of the absorber layer to the engineered bandgap minimum within 2 ns, which corresponds to a mobility range of 8.7–58.9 cm2 V−1 s−1. In addition, the recombination times strongly depend on the Ga-content, ranging from 19.1 ns in the energy minimum to 85 ps in the high Ga-content region near the Mo-back contact. An analytical model, as well as drift-diffusion numerical simulations, fully decouple carrier transport and recombination behaviour in this complex composition-graded absorber structure, demonstrating the potential of TAS.