To replace the conventionally used CdS buffers in Cu2ZnSn(S,Se)4 (CZTSSe) based thin-film solar cells, sputtered Zn(O,S) buffer layers have been investigated. Zn(O,S) layers with three different [O]/([O] + [S]) ratios (0.4, 0.7, and 0.8)—and a combination of Zn(O,S) and CdS (“hybrid buffer layer”) were studied. In comparison to the CdS reference, the external quantum efficiency (EQE) of the Zn(O,S)-buffered devices increases in the short- and long-wavelength regions of the spectrum. However, the average EQE ranges below that of the CdS reference, and the devices show a low open-circuit voltage (VOC). By adding a very thin CdS layer (5 nm) between the absorber and the Zn(O,S) buffer, the VOC loss is completely avoided. Using thicker intermediate CdS layers result in a further device improvement, with VOC values above those of the CdS reference. X-ray photoelectron spectroscopy (XPS) measurements suggest that the thin CdS layer prevents damage to the absorber surface during the sputter deposition of the Zn(O,S) buffer. With the hybrid buffer configuration, a record VOC deficit, i.e., a minimum difference between bandgap energy Eg (divided by the elementary charge q) and VOC (Eg/q – VOC) of 519 mV could be obtained, i.e., the lowest value reported for kesterite solar cells to date. Thus, the hybrid buffer configuration is a promising approach to overcome one of the main bottlenecks of kesterite-based solar cells, while simultaneously also reducing the amount of cadmium needed in the device.
Currently, the use of Zn(O,S) as buffer material for Cu(In,Ga)Se2 (CIGS) solar cells is intensely studied in order to further boost the performance of these devices. In this context, nondestructive analytical tools are needed that enable the determination of buffer bandgap energies in the complete device. To this end, we developed a spectroscopic approach based on electroreflectance (ER). From a set of measured angle-resolved ER (ARER) spectra, an averaged modulus spectrum is numerically calculated. This method suppresses the commonly observed detrimental line-shape distortions due to interference effects in the layered device structure and thus enables the determination of bandgap energies even for thin buffer layers. To verify the working principle of ARER, we first apply it to CIGS absorber and CdS buffer layers. Then, we utilize it to investigate CIGS solar cells with Zn(O,S) buffers. All ARER results are compared to the results of diffuse ER, a technique previously developed for the suppression of interference fringes. We demonstrate that ARER is the superior ER method for nondestructive bandgap determination of thin buffer layers in complete CIGS solar cells. Moreover, a Cu containing compound was determined as a secondary phase in the Zn(O,S) buffer by combined ARER studies, scanning transmission electron microscopy, and energy-dispersive X-ray spectroscopy.
Post-deposition treatment (PDT) of the absorber layer with alkali fluorides has led to a significant increase in the efficiency of Cu(In,Ga)Se2 (CIGS) thin-film solar cells. In this contribution, we investigate the influence of alkali PDTs on the absorber's surface potential by means of Kelvin probe force microscopy (KPFM). To this end, we perform KPFM on cross sections of complete CIGS solar cells. To improve the reliability of the measurement procedure, we deposit a gold layer on top of the solar cell as a reference layer. Using this approach, we study the influence of RbF and KF PDT on the absorber's surface potential for CIGS solar cells with different absorber and buffer compositions. In all cases, an increased surface potential of the cross section of the absorber layer is measured for the cells with PDT.
Thin-film solar cells with Cu(In,Ga)Se2 (CIGS) absorber layers have been intensively studied due to their high power conversion efficiencies. CIGS solar cells with Zn(O,S) buffer layers achieved record efficiencies due to their reduced parasitic absorption compared with the more commonly used CdS buffer. Accordingly, we have studied solution-grown Zn(O,S) buffer layers on polycrystalline CIGS absorber layers by complementary techniques. A bandgap energy Eg of 2.9 eV is detected by means of angle-resolved electroreflectance spectroscopy corresponding to Zn(O,S), whereas an additional Eg of 2.3 eV clearly appeared for a post-annealed CIGS solar cell (250 °C in air) compared with the as-grown state. To identify the chemical phase that contributes to the Eg of 2.3 eV, the microstructure and microchemistry of the Zn(O,S) buffer layers in the as-grown state and after annealing were analyzed by different transmission electron microscopic techniques on the submicrometer scale and energy-dispersive x-ray spectroscopy. We demonstrate that the combination of these methods facilitates a comprehensive analysis of the complex phase constitution of nanoscaled buffer layers. The results show that after annealing, the Cu concentration in Zn(O,S) is increased. This observation indicates the existence of an additional Cu-containing phase with Eg close to 2.3 eV, such as Cu2Se (2.23 eV) or CuS (2.36 eV), which could be one possible origin of the low power conversion efficiency and low fill factor of the solar cell under investigation.
The impact of multiple‐selenization of wet‐chemical precursors for kesterite‐type Cu2ZnSn(S,Se)4 solar cells is reported. The absorber forms a compact layer with mostly big grains. Gaps between the big grains are filled with smaller grains. Also the absorber lacks the common trilayer/multilayer structure. As a result the layer thickness is more homogeneous and the morphology is more evened out. This is the basis for a more homogeneous device parameter distribution across large samples and a better reproducibility of CZTSSe solar cells.
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