Evidence for the Band‐Edge Exciton of CuInS2 Nanocrystals Enables Record Efficient Large‐Area Luminescent Solar Concentrators. (15th November 2019)

• Record Type: Journal Article
• Authors: Anand, Abhinav; Zaffalon, Matteo L.; Gariano, Graziella; Camellini, Andrea; Gandini, Marina; Brescia, Rosaria; Capitani, Chiara; Bruni, Francesco; Pinchetti, Valerio; Zavelani‐Rossi, Margherita; Meinardi, Francesco; Crooker, Scott A.; Brovelli, Sergio
• Is Part Of: Advanced functional materials. Volume 30:Number 4(2020)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2019-11-15
• Subjects: CuInS2 -- luminescent solar concentrators -- Monte Carlo modeling -- semiconductor nanocrystals -- spectroscopy; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adfm.201906629
• Languages: English
• ISSNs: 1616-301X

Abstract

Abstract: Ternary I‐III‐VI2 nanocrystals (NCs), such as CuInS2, 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 CuInS2 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 behaviours 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. Here, by studying stoichiometric CuInS2 NCs, it is 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, the NCs also show dark‐state emission likely originating from enhanced electron‐hole spin interaction. The impact of the observed optical behaviours on LSCs is evaluated by Monte Carlo ray‐tracing simulations. Based on the emerging device design guidelines, optical‐grade large‐area (30×30 cm 2 ) LSCs with optical power efficiency (OPE) as high as 6.8% are fabricated, corresponding to the highest value reported to date for large‐area devices. Abstract : Ternary I–III–VI2 nanocrystals are interesting nontoxic materials for numerous optoelectronic and photonic technologies, and in particular, for luminescent solar concentrators (LSCs). The mechanisms underpinning their optical properties are not fully understood. Here, a recent theory suggesting that the characteristic Stokes‐shifted, long‐lived luminescence of CuInS2 nanocrystals is due to their valence‐band structure is endorsed experimentally. Based on these findings, large‐area semitransparent LSCs (30 cm × 30 cm) with a record efficiency of 6.8% are fabricated.