Over 15% efficient wide-band-gap Cu(In,Ga)S2 solar cell: Suppressing bulk and interface recombination through composition engineering

2021 
Summary The progress of Cu(In,Ga)S2 remains significantly limited mainly due to photovoltage (Voc) losses in the bulk and at the interfaces. Here, via a combination of photoluminescence, cathodoluminescence, electrical measurements, and ab initio modeling, we address the bulk and interface losses to improve ∼1.6-eV-band-gap (Eg) Cu(In,Ga)S2. The optoelectronic quality of the absorber improves upon reducing the [Cu]/[Ga+In] (CGI) ratio, as manifested by the suppression of deep defects, higher quasi-Fermi level splitting (QFLS), improved charge-carrier lifetime, and higher Voc. We identify antisite CuIn/CuGa as a major performance-limiting deep defect by comparing the formation energies of various intrinsic defects. Interface recombination is suppressed using a Zn(O,S) buffer layer in Cu-poor devices, which leads to the activation energy of recombination equal to the Eg. We demonstrate an efficiency of 15.2% with Voc of 902 mV from a H2S-free, Cd-free, and KCN-free process.
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