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Kesterite is an earth‐abundant energy material with high predicted power conversion efficiency, making it a sustainable and promising option for photovoltaics. However, a large open circuit voltage Voc deficit due to non‐radiative recombination at intrinsic defects remains a major hurdle, limiting device performance. Incorporating Ge into the kesterite structure emerges as an effective approach for enhancing performance by manipulating defects and morphology. Herein, how different amounts of Ge affect the kesterite growth pathways through the combination of advanced microscopy characterization techniques are systematically investigated. The results demonstrate the significance of incorporating Ge during the selenization process of the CZTSSe thin film. At high temperature, the Ge incorporation effectively delays the selenization process due to the formation of a ZnSe layer on top of the metal alloys through decomposition of the Cu‐Zn alloy and formation of Cu‐Sn alloy, subsequently forming of Cu‐Sn‐Se phase. Such an effect is compounded by more Ge incorporation that further postpones kesterite formation. Furthermore, introducing Ge mitigates detrimental "horizontal" grain boundaries by increasing the grain size on upper layer. The Ge incorporation strategy discussed in this study holds great promise for improving device performance and grain quality in CZTSSe and other polycrystalline chalcogenide solar cells. [ABSTRACT FROM AUTHOR]

Earth‐abundant and air‐stable Cu2BaSnS4−xSex (CBTSSe) and related thin‐film absorbers are regarded as prospective options to meet the increasing demand for low‐cost solar cell deployment. Devices based on vacuum‐deposited CBTSSe absorbers have achieved record power conversion efficiency (PCE) of 5.2% based on a conventional device structure using CdS buffer and i‐ZnO/indium tin oxide (ITO) window layers, with open‐circuit voltage (VOC) posing the major bottleneck for improving solar cell performance. The current study demonstrates a >20% improvement in VOC (from 0.62 to 0.75 V) and corresponding enhancement in PCE (from 5.1% to 6.2% without antireflection coating; to 6.5% with MgF2 antireflection coating) for solution‐deposited CBTSSe solar cells. This performance improvement is realized by introducing an alternative successive ionic layer adsorption and reaction‐deposited Zn1−xCdxS buffer combined with sputtered Zn1−xMgxO/Al‐doped ZnO window/top contact layer, which offers lower electron affinities relative to the conventional CdS/i‐ZnO/ITO stack and better matching with the low electron affinity of CBTSSe. A combined experimental (temperature‐ and light intensity‐dependent VOC measurements) and device simulation (SCAPS‐1D) evaluation points to the importance of addressing relative band offsets for both the buffer and window layers relative to the absorber in mitigating interfacial recombination and optimizing CBTSSe solar cell performance. [ABSTRACT FROM AUTHOR]

Antimony sulfide (Sb2S3) is a promising wide‐bandgap photovoltaic material, and a potential top‐cell candidate for next‐generation Si‐based tandem solar cells. The most widely used electron transport layers in Sb2S3 solar cells are TiO2 and CdS, which present an obvious performance variation in open‐circuit voltage (VOC) and short current (Jsc). However, the mechanisms behind the performance disparity because of the electron transport layer (ETL) have not been disclosed. Herein, a comprehensive comparative study of using TiO2 and CdS as the electron transport layers in Sb2S3 solar cells is presented, which covers their influence on preferential crystal orientation, band alignment, interface, and bulk defects. It is found that the CdS ETL results in less interfacial defects and more favorable band alignment, enabling a higher VOC, while the high resistance of the CdS film and parasitic light absorption restricts the JSC. The findings provide a substantial guidance on device optimization for Sb2S3 solar cells. [ABSTRACT FROM AUTHOR]

Kesterite Cu2ZnSnS4 (CZTS) solar cell has emerged as one of the most promising thin‐film photovoltaic technologies that allows for cheap, clean, and efficient renewable power in the future. Nevertheless, limited by the large photovoltage deficit caused by severe interface recombination, the potential of CZTS solar cells is far from being fully tapped. Herein, it is demonstrated that the carrier density of the CZTS absorber and the acceptor‐like interface defects are two critical factors governing the interface recombination in addition to the unfavorable conduction band alignment. Results of device simulation suggest that passivating the acceptor‐like interface defects combined with appropriate absorber carrier density is the essential way to promote the photovoltage and efficiency of CZTS solar cells to a more competitive level. It is believed that these results could be generally applicable to the interface recombination of other heterojunction solar cells. [ABSTRACT FROM AUTHOR]

The performance of kesterite Cu2ZnSn(S,Se)4 (CZTSSe) solar cell is known to be severely limited by the nonradiative recombination near the heterojunction interface and within the bulk of the CZTSSe absorber resulting from abundant recombination centers and limited carrier collection efficiency. Herein, nonradiative recombination is simultaneously reduced by incorporating small amounts of Ge and Cd into the CZTSSe absorber. Incorporation of Ge effectively increases the p‐type doping, thus successfully improving the bulk conductance and reducing the recombination in the CZTSSe bulk via enhanced quasi‐Fermi level splitting, while the incorporation of Cd greatly reduces defects near the junction region, enabling larger depletion region width and better carrier collection efficiency. The combined effects of Cd and Ge incorporation give rise to systematic improvement in open‐circuit voltage (VOC), short‐circuit current density (JSC), and fill factor (FF), enabling a high conversion efficiency of 11.6%. This study highlights the multiple cation incorporation strategy for systematically manipulating the opto‐electronic properties of kesterite materials, which may also be applicable to other semiconductors. [ABSTRACT FROM AUTHOR]

Lithium incorporation in kesterite Cu2ZnSn(S,Se)4 (CZTSSe) materials has been experimentally proven effective in improving electronic quality for application in photovoltaic devices. Herein, a feasible and effective solution‐based lithium post‐deposition treatment (PDT), enabling further efficiency improvement on the high‐performance baseline is reported and the dominant mechanism for this improvement is proposed. In this way, lithium is uniformly incorporated into grain interiors (GIs) without segregation at grain boundaries (GBs), which can occupy the Zn sites with a high solubility in the CZTSSe matrix, producing high density of LiZn antisites with shallower acceptor levels than the intrinsic dominant defect (CuZn antisites). As a result, CZTSSe absorber with better p‐type doping is obtained, leading to a pronounced enhancement in fill factor and a corresponding gain in open‐circuit voltage and short‐circuit current and consequently a significant efficiency boost from 9.3% to 10.7%. This work provides a feasible alternative alkali‐PDT treatment for chalcogenide semiconductors and promotes a better understanding of the mechanism of Li incorporation in kesterite materials. [ABSTRACT FROM AUTHOR]

The earth‐abundant and environmentally‐friendly CuSbS2 solar cells have been struggling with low device performance, especially poor open circuit voltage (Voc). In this work, post‐annealing treatment of the CuSbS2/CdS heterojunction performed on CuSbS2‐based solar cells was firstly reported. With this treatment, we demonstrated CuSbS2 solar cells with a record Voc of 622 mV. The improvement of device performance was found peaked at 250°C post‐annealing which mainly benefits from the significantly boosted open‐circuit voltage and short‐circuit current. The study of microstructure by high‐resolution transmission electron microscopy revealed that such improvement could be attributed to the formation of epitaxial CuSbS2/CdS hetero‐interface upon heat treatment, which reduces the interface defect density that may lead to reduced Voc deficit. Besides, results of photoluminescence and time‐resolved photoluminescence measurements also indicated improved electrical properties of completed devices with higher photoluminescence intensity and longer minority carrier lifetime. We demonstrated significant improvement in efficiency (particularly in the Voc and Jsc) for CuSbS2 solar cells by post‐heat treatment of the CuSbS2/CdS heterojunction. The underlying correlation between post‐heat treatment and device performance reveals that the post‐heat treatment on the heterojunction leads to (1) the transformation from amorphous to epitaxial relationship of CuSbS2/CdS hetero‐interface and (2) simultaneously improved absorber quality. [ABSTRACT FROM AUTHOR]

Antimony sulfide (Sb2S3) as a wide‐bandgap, nontoxic, and stable photovoltaic material reveals great potential for the uppermost cells in Si‐based tandem cell stacks. Sb2S3 solar cells with a compatible process, acceptable cost, and high efficiency therefore become the mandatory prerequisites to match silicon bottom cells. The performance of vacuum processed Sb2S3 device is pinned by bulk and interfacial recombination. Herein, a thermally treated TiO2 buffer layer induces quasiepitaxial growth of vertical orientation Sb2S3 absorber overcoming interface defects and absorber transport loss. Such novel growth could pronouncedly improve the open‐circuit voltage (Voc) due to the superior interface quality and intraribbon transport. The epitaxial rough Sb2S3 surface shows a texturized‐like morphology. It is optimized by tuning the grain sizes to form strong light trapping effect, which further enhances the short‐circuit current density (Jsc) with a 16% improvement. The final optimal device with high stability obtains a power conversion efficiency of 5.4%, which is the best efficiency for full‐inorganic Sb2S3 solar cells. The present developed quasiepitaxy strategy supports a superior interface, vertical orientation, and surface light trapping effect, which provides a new perspective for efficient noncubic material thin film solar cells. [ABSTRACT FROM AUTHOR]

The large open circuit voltage (Voc) deficit (Eg/ q -Voc) is the key factor limiting the current efficiency of pure sulfide Cu 2 ZnSnS 4 (CZTS) thin film solar cells. This present work reports CZTS devices with a Voc of over 710 mV by utilizing either In 2 S 3 buffer or In 2 S 3 /CdS hybrid buffer. The improvement in Voc mainly results from (i) an increased carrier concentration in CZTS due to In-doping when the In 2 S 3 buffer is adjacent to the CZTS absorber and (ii) favorable conduction band alignments at the CZTS/buffer interface. However, devices with In 2 S 3 buffers suffer from having a lower Fill Factor (FF) and short circuit current density (Jsc) when compared with those with CdS buffers. In contrast devices with In 2 S 3 /CdS hybrid buffers not only yield an enhancement in Voc, but also give the same level of FF and an even higher Jsc relative to CdS buffers, thereby increasing the efficiency from 5.5% to 6.6%. These hybrid In 2 S 3 /CdS buffers provide a promising way to reduce the Voc deficit and further boost the efficiency of pure sulfide CZTS solar cells. [ABSTRACT FROM AUTHOR]

Perovskite solar cells (PSCs) have now achieved power conversion efficiencies (PCEs) over 25%, but their long-term stability under illumination and thermal stress is still a major barrier to commercialisation. Herein, we demonstrate the evaluation of light-induced degradation activation energy (E a) of encapsulated semi-transparent PSCs by using the commonly employed method in crystalline silicon solar cells. Different parameters showed different activation energies where primary degradation is due to increase in series resistance, which also led to reduction in short-circuit current. Open-circuit voltage and shunt resistance also change with different E a , suggesting the mechanism of the reduction is likely to be due to different reasons. Despite each parameter exhibiting slight variation over time for each temperature, the overall trend converges, indicating that each parameter is likely to be primarily reduced by a single dominant reaction. We also report the main cause of irreversible device degradation is not due to the decomposition of the perovskite layer as confirmed by X-ray diffraction characterisation. Instead, our pole figure map and absorption spectra analysis indicate that a loss of crystal symmetry occurs due to ion migration within the device that induce oxidation of 2,2′,7,7′-tetrakis-(N , N -di-4-methoxyphenylamino)-9,9′-spirobifluorene (Spiro-OMeTAD). Our work provides a better understanding through quantification of the degradation processes of encapsulated semi-transparent PSCs over time, which is essential for further progress and development of stable perovskite-Si tandem solar cells. • The light-induced degradation in semi-transparent solar cell is investigated. • The primary loss of PCEs in PSCs was due to an increase in series resistance. • XRD results indicate stability of perovskite layer, with degradation occurring in other layers. • Diffusion of ions back into the perovskite layer results in a recovery from LID. [ABSTRACT FROM AUTHOR]