Evidence for the Band-Edge Exciton of CuInS2 Nanocrystals Enables Record Efficient Large-Area Luminescent Solar Concentrators

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

doi:10.1002/adfm.201906629

Title: Evidence for the Band-Edge Exciton of CuInS₂ Nanocrystals Enables Record Efficient Large-Area Luminescent Solar Concentrators

Journal Article · Fri Nov 15 00:00:00 EST 2019 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.201906629· OSTI ID:2337651

Anand, Abhinav ^[1]; Zaffalon, Matteo L. ^[1]; Gariano, Graziella ^[2]; Camellini, Andrea ^[3]; Gandini, Marina ^[2]; Brescia, Rosaria ^[4]; Capitani, Chiara ^[5]; Bruni, Francesco ^[2]; Pinchetti, Valerio ^[1]; Zavelani‐Rossi, Margherita ^[6]; Meinardi, Francesco ^[1];

^[7];

^[1]

Univ. degli Studi di Milano (Italy)
Glass to Power SpA, Rovereto (Italy)
Politecnico di Milano (Italy)
Istituto Italiano di Tecnologia (IIT), Genova (Italy)
Univ. degli Studi di Milano (Italy); Glass to Power SpA, Rovereto (Italy)
Politecnico di Milano (Italy); Istituto di Fotonica e Nanotecnologie (IFN), Milan (Italy); National Research Council (CNR), Milan (Italy)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). National High Magnetic Field Lab. (MagLab)

Abstract Ternary I‐III‐VI ₂ nanocrystals (NCs), such as CuInS ₂ , 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 CuInS ₂ 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 CuInS ₂ 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.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)

Grant/Contract Number:: 89233218CNA000001; DMR-1644779

OSTI ID:: 2337651

Alternate ID(s):: OSTI ID: 1593164

Report Number(s):: LA-UR-19-23794

Journal Information:: Advanced Functional Materials, Vol. 30, Issue 4; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 59 works

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Monte Carlo modeling
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Title: Evidence for the Band-Edge Exciton of CuInS2 Nanocrystals Enables Record Efficient Large-Area Luminescent Solar Concentrators

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Title: Evidence for the Band-Edge Exciton of CuInS₂ Nanocrystals Enables Record Efficient Large-Area Luminescent Solar Concentrators