Cu2ZnSnS4 (CZTS) shows great potential for cheap, efficient photovoltaic devices. However, one problem during synthesis of CZTS films is the loss of Sn as a result of decomposition and evaporation of SnS. This paper uses kinetic models to show that the mechanism of the decomposition reaction probably occurs in at least two stages; first, a loss of sulfur which causes dissociation of the structure into binary sulfides, and only then the evaporation of SnS. Knowledge of the reaction mechanism helps to identify the driving force for decomposition as arising from the relative instability of Sn(IV) in CZTS against reduction; this theory is backed up by thermodynamic data. The volatility of SnS further exaggerates the decomposition by rendering it irreversible. This insight, alongside experimental data, allows prediction of the annealing conditions required to stabilize CZTS surfaces. A fundamental incompatibility of CZTS with high-temperature, vacuum-based processing is exposed, distinguishing it from related indium-containing compounds. This offers an explanation as to why the most efficient CZTS devices to-date all arise from “two-stage” fabrication processes involving low temperature deposition followed by annealing at high pressure, and provides key information for designing successful annealing strategies.
International audienceCu2ZnSnS4 (CZTS) is an interesting material for sustainable photovoltaics, but efficiencies are limited by the low open-circuit voltage. A possible cause of this is disorder among the Cu and Zn cations, a phenomenon which is difficult to detect by standard techniques. We show that this issue can be overcome using near-resonant Raman scattering, which lets us estimate a critical temperature of 533 +/- 10K for the transition between ordered and disordered CZTS. These findings have deep significance for the synthesis of high-quality material, and pave the way for quantitative investigation of the impact of disorder on the performance of CZTS-based solar cells. (C) 2014 AIP Publishing LLC
Experimental proof is presented for a hitherto undetected solid-state reaction between the solar cell material Cu(2)ZnSn(S,Se)(4) (CZTS(e)) and the standard metallic back contact, molybdenum. Annealing experiments combined with Raman and transmission electron microscopy studies show that this aggressive reaction causes formation of MoS(2) and secondary phases at the CZTS|Mo interface during thermal processing. A reaction scheme is presented and discussed in the context of current state-of-the-art synthesis methods for CZTS(e). It is concluded that alternative back contacts will be important for future improvements in CZTS(e) quality.
Cu 2 ZnSnS 4 (CZTS) is a promising material for thin film solar cells based on sustainable resources. This paper explores some consequences of the chemical instability between CZTS and the standard Mo "back contact" layer used in the solar cell. Chemical passivation of the back contact interface using titanium nitride (TiN) diffusion barriers, combined with variations in the CZTS annealing process, enables us to isolate the effects of back contact chemistry on the electrical properties of the CZTS layer that result from the synthesis, as determined by measurements on completed solar cells. It is found that instability in the back contact is responsible for large current losses in the finished solar cell, which can be distinguished from other losses that arise from instabilities in the surface of the CZTS layer during annealing. The TiN-passivated back contact is an effective barrier to sulfur atoms and therefore prevents reactions between CZTS and Mo. However, it also results in a high series resistance and thus a reduced fill factor in the solar cell. The need for high chalcogen pressure during CZTS annealing can be linked to suppression of the back contact reactions and could potentially be avoided if better inert back contacts were to be developed.
Tandem solar cells based on hybrid organic−inorganic metal halide perovskites have reached efficiencies up to 28%, but major concerns for long-term stability and the presence of Pb have raised interest in searching for fully earth-abundant, intrinsic chemically stable, and nontoxic alternatives. With a direct band gap around 1.8 eV and stability in air up to at least 500 °C, BaZrS 3 is a promising candidate. This work presents the first approach of synthesizing a thin film of such compound by sputtering at ambient temperature with a subsequent rapid thermal process. Despite the short fabrication time, the width of the XRD diffraction peaks and the energy and distribution of the photoluminescence response show comparable crystalline quality to that from bulk synthesis methods. Good crystallization required around 900 °C. Such a high temperature could be incompatible with fabrication of tandem solar cells.
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