Proceedings of nanoGe Spring Meeting 2022 (NSM22)
DOI: https://doi.org/10.29363/nanoge.nsm.2022.191
Publication date: 7th February 2022
Ternary I-III-VI2 NCs, such as CuInS2 and AgInS2 are receiving attention as heavy-metals-free materials for solar cells, luminescent solar concentrators (LSCs), LEDs, and bio-imaging. The origin of the optical properties of NCs are however not fully understood. A recent theoretical model suggests that their characteristic Stokes-shifted and long-lived luminescence arises from the structure of the valence band (VB) and predicts distinctive optical behaviors in defect-free NCs: the quadratic dependence of the radiative decay rate and the Stokes shift on the NC radius. If confirmed, this would have crucial implications for LSCs as the solar spectral coverage ensured by low-bandgap NCs would be accompanied by increased re-absorption losses. In this work, we performed spectroscopic studies on stoichiometric CuInS2 and AgInS2 NCs, and in the process it was revealed for the first time, the spectroscopic signatures predicted for the free band-edge exciton, thus supporting the VB-structure model. At very low temperatures, we also observed dark-state emission from these NCs likely originating from enhanced electron-hole spin interaction. The impact of the observed optical behaviors on LSCs was evaluated by Monte Carlo ray-tracing simulations. Based on the emerging device design guidelines, optical-grade large-area (30×30 cm2) LSCs with optical power efficiency (OPE) as high as 6.8% were fabricated, corresponding to the highest value reported to date for large-area devices.
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