Polycrystalline thin film copper chalcogenide solar cells show remarkable efficiencies, and analogous but less-explored semiconducting materials may hold similar promise. With consideration of elemental abundance and process scalability, we explore the potential of the Cu-Sb-S material system for photovoltaic applications. Using a high-throughput combinatorial approach, Cu-Sb-S libraries were synthesized by magnetron co-sputtering of Cu 2 S and Sb 2 S 3 targets and evaluated by a suite of spatially resolved characterization techniques. The resulting compounds include Cu 1.8 S (digenite), Cu 12 Sb 4 S 13 (tetrahedrite), CuSbS 2 (chalcostibite), and Sb 2 S 3 (stibnite). Of the two ternary phases synthesized, CuSbS 2 was found to have the most potential, however, when deposited at low temperatures its electrical conductivity varied by several orders of magnitude due to the presence of impurities. To address this issue, we developed a self-regulated approach to synthesize stoichiometric CuSbS 2 films using excess Sb 2 S 3 vapor at elevated substrate temperatures. Theoretical calculations explain that phase-pure CuSbS 2 is expected to be formed over a relatively wide range of temperatures and pressures, bound by the sublimation of Sb 2 S 3 and decomposition of CuSbS 2. The carrier concentration of CuSbS 2 films produced within this regime was tunable from 10 16 − 10 18 cm −3 through appropriate control of Sb 2 S 3 flux rate and substrate temperature. CuSbS 2 displayed a sharp optical absorption onset indicative of a direct transition at 1.5 eV and an absorption coefficient of 10 5 cm −1 within 0.3 eV of the onset. The results of this study suggest that CuSbS 2 holds promise for solar energy conversion due to its tolerant processing window, tunable carrier concentration, solar-matched band gap, and high absorption coefficient.
The earth-abundant material CuSbS (CAS) has shown good optical properties as a photovoltaic solar absorber material, but has seen relatively poor solar cell performance. To investigate the reason for this anomaly, the core levels of the constituent elements, surface contaminants, ionization potential, and valence-band spectra are studied by X-ray photoemission spectroscopy. The ionization potential and electron affinity for this material (4.98 and 3.43 eV) are lower than those for other common absorbers, including CuInGaSe (CIGS). Experimentally corroborated density functional theory (DFT) calculations show that the valence band maximum is raised by the lone pair electrons from the antimony cations contributing additional states when compared with indium or gallium cations in CIGS. The resulting conduction band misalignment with CdS is a reason for the poor performance of cells incorporating a CAS/CdS heterojunction, supporting the idea that using a cell design analogous to CIGS is unhelpful. These findings underline the critical importance of considering the electronic structure when selecting cell architectures that optimize open-circuit voltages and cell efficiencies.
Development of alternative thin film photovoltaic technologies is an important research topic due to the potential for low-cost, large-scale fabrication of high-efficiency solar cells. Despite the large number of promising alternative absorbers and corresponding contacts, the rate of progress is limited by complications that arise during solar cell fabrication. One potential solution to this problem is the high-throughput combinatorial method, which has been extensively used for research and development of individual absorber and contact materials. Here, we demonstrate an accelerated approach to development of thin film photovoltaic device prototypes based on the novel CuSbS 2 absorber, using the device architecture employed for CuIn x Ga (1-x) Se 2 (CIGS). The newly developed three-stage, self-regulated CuSbS 2 growth process enables the study of PV device performance trends as a function of phase purity, crystallographic orientation, layer thickness of the absorber, and numerous back contacts. This exploration results in initial CuSbS 2 device prototypes with ~1% conversion efficiency, currently limited by low short-circuit current due to poor collection of photoexcited electrons, and a small open-circuit voltage due to a theoretically predicted, cliff-type conduction band offset between CuSbS 2 and CdS. Overall, these results illustrate the potential of combinatorial methods to accelerate the development of thin film photovoltaic devices with this and other novel absorbers.
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