期刊
ADVANCED MATERIALS
卷 29, 期 24, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201606945
关键词
cationic disordering; Cu2BaSn(S,Se)(4); earth-abundant chalcogenides; photovoltaic devices; trigonal crystal structures
类别
资金
- National Science Foundation [1511737]
- National Science Foundation as part of the National Nanotechnology Coordinated Infrastructure (NNCI) [ECCS-1542015]
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [1511737] Funding Source: National Science Foundation
In recent years, Cu2ZnSn(S,Se)(4) (CZTSSe) materials have enabled important progress in associated thin-film photovoltaic (PV) technology, while avoiding scarce and/or toxic metals; however, cationic disorder and associated band tailing fundamentally limit device performance. Cu2BaSnS4 (CBTS) has recently been proposed as a prospective alternative large bandgap (similar to 2 eV), environmentally friendly PV material, with similar to 2% power conversion efficiency (PCE) already demonstrated in corresponding devices. In this study, a two-step process (i.e., precursor sputter deposition followed by successive sulfurization/selenization) yields high-quality nominally pinhole-free films with large (>1 mu m) grains of selenium-incorporated (x = 3) Cu2BaSnS4-xSex (CBTSSe) for high-efficiency PV devices. By incorporating Se in the sulfide film, absorber layers with 1.55 eV bandgap, ideal for single-junction PV, have been achieved within the CBTSSe trigonal structural family. The abrupt transition in quantum efficiency data for wavelengths above the absorption edge, coupled with a strong sharp photoluminescence feature, confirms the relative absence of band tailing in CBTSSe compared to CZTSSe. For the first time, by combining bandgap tuning with an air-annealing step, a CBTSSe-based PV device with 5.2% PCE (total area 0.425 cm(2)) is reported, >2.5x better than the previous champion pure sulfide device. These results suggest substantial promise for the emerging Se-rich Cu2BaSnS4-xSex family for high-efficiency and earth-abundant PV.
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