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Semi-monolithic Integration of All-Chalcopyrite Multijunction Solar Conversion Devices via Thin-Film Bonding and Exfoliation

Cite this: ACS Appl. Mater. Interfaces 2022, 14, 49, 54607–54615
Publication Date (Web):December 5, 2022
https://doi.org/10.1021/acsami.2c10578
Copyright © 2022 American Chemical Society

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    Abstract

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    We report on a semi-monolithic integration method to circumvent processing incompatibility between materials of dissimilar classes and combine them into multijunction devices for photovoltaic and photoelectrochemical applications. Proof-of-concept all-chalcopyrite tandems were obtained by consecutive transfer of fully integrated unpatterned 1.85 eV CuGa3Se5 and 1.13 eV CuInGaSe2 PV stacks from their Mo/soda lime glass substrates onto a new single host substrate. This transfer approach consists of two key steps: (1) bonding of the solar stack (face down) onto a handle (e.g., SnO2:F, FTO) using a transparent conductive composite and (2) delamination of the solar stack at the chalcopyrite/Mo interface by employing a wedge-based exfoliation technique. Upon transfer onto FTO, a CuGa3Se5 champion device demonstrated near-coincident photocurrent density–voltage characteristic with a baseline measurement. Then, the exfoliated CuGa3Se5 single-junction stack transferred onto FTO served as the new host onto which a second fully processed CuInGaSe2 stack was bonded (face down) onto and liberated from its Mo/SLG substrate, leading to a complete transfer of both sub-cells onto one FTO substrate. A champion semi-monolithic tandem device exhibited a power conversion efficiency of 5.04% with an open-circuit voltage, a short-circuit current density, and a fill factor of 1.24 V, 7.19 mA/cm2, and 56.7%, respectively. This first-time demonstration of a fully operational semi-monolithic device provides a new avenue to combine thermally, mechanically, and/or chemically incompatible thin-film material classes into tandem photovoltaic and photoelectrochemical devices while maintaining state-of-the-art sub-cell processing.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.2c10578.

    • Image of the mechanical exfoliation device; optical image of a defect in a transferred CuGa3Se5 device; dark JV response of the CuGa3Se5 layer with ohmic ITO contacts; transferred CuGa3Se5 device with 0.12cm2 ITO back contacts; performance of a transferred CuGa3Se5 device with ITO back contact compared to the same device integrated with an additional Mo back contact layer; area-dependent performance of a non-gridded CuGa3Se5 and CIGSe reference devices; area-dependent performance of a transferred CuGa3Se5 device integrated with an ITO back contact; tabulated performance data of transferred CuGa3Se5 champion device; transferred CIGSe device performance data; area-dependent performance of semi-monolithic tandem devices; cross-sectional SEM of a CuGa3Se5/CIGSe semi-monolithic device; and tabulated performance data of the semi-monolithic tandem device and sub-cells (PDF)

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