10.24% Efficiency of Flexible Cu2 ZnSn(S,Se)4 Solar Cells by Pre-Evaporation Selenization Technique.

Flexible Cu2 ZnSn(S,Se)4 (CZTSSe) solar cells show great potential due to non-toxicity and low cost. The quality of CZTSSe absorber suffering from the high-temperature selenization process is the key to overcoming open-circuit voltage (VOC ) deficit and obtaining high efficiency. In this work, the authors develop a selenization technique to improve the quality of the CZTSSe layer by pre-evaporation selenization. This method provides saturated selenium vapor at the beginning of the selenization process to promote the crystallization process. The oversaturated selenium source greatly shortens the annealing time at high temperatures. The prepared CZTSSe films have larger grains and fewer voids. The measurement of the space charge limited current shows that the defect density of the CZTSSe absorber is significantly reduced from 4.43 × 1013  cm-3 to 3.46 × 1013 cm-3 . Electrical tests show that the devices have better charge separation at the interface, resulting in a charge recombination lifetime, increasing from 133 to 197 µs. The power conversion efficiency of the flexible CZTSSe solar cell reaches 10.24% with VOC and the fill factor enhances to 463 mV and 62%, respectively. The safe non-toxicity and efficient selenization method is expected to provide a new strategy for high-efficiency flexible CZTSSe solar cells.

Defect Synergistic Regulations of Li&Na Co-Doped Flexible Cu2 ZnSn(S,Se)4 Solar Cells Achieving over 10% Certified Efficiency.

Ion doping is an effective strategy for achieving high-performance flexible Cu2 ZnSn(S,Se)4 (CZTSSe) solar cells by defect regulations. Here, a Li&Na co-doped strategy is applied to synergistically regulate defects in CZTSSe bulks. The quality absorbers with the uniformly distributed Li and Na elements are obtained using the solution method, where the acetates (LiAc and NaAc) are as additives. The concentration of the harmful CuZn anti-site defects is decreased by 8.13% after Li incorporation, and that of the benign NaZn defects is increased by 36.91% after Na incorporation. Synergistic Li&Na co-doping enhances the carrier concentration and reduces the interfacial defects concentration by one order of magnitude. As a result, the flexible CZTSSe solar cell achieves a power conversion efficiency (PCE) of 10.53% with certified 10.12%. Because of the high PCE and the homogeneous property, the Li&Na co-doped device is fabricated to a large area (2.38 cm2 ) and obtains 9.41% PCE. The co-doping investigation to synergistically regulate defects provides a new perspective for efficient flexible CZTSSe solar cells.

Efficient Environmentally Friendly Flexible CZTSSe/ZnO Solar Cells by Optimizing ZnO Buffer Layers.

Flexible CZTSSe solar cells have attracted much attention due to their earth-abundant elements, high stability, and wide application prospects. However, the environmental problems caused by the high toxicity of the Cd in the buffer layers restrict the development of flexible CZTSSe solar cells. Herein, we develop a Cd-free flexible CZTSSe/ZnO solar cell. The influences of the ZnO films on device performances are investigated. The light absorption capacity of flexible CZTSSe solar cells is enhanced due to the removal of the CdS layer. The optimal thickness of the ZnO buffer layers and the appropriate annealing temperature of the CZTSSe/ZnO are 100 nm and 200 °C. Ultimately, the optimum flexible CZTSSe/ZnO device achieves an efficiency of 5.0%, which is the highest efficiency for flexible CZTSSe/ZnO solar cells. The systematic characterizations indicate that the flexible CZTSSe/ZnO solar cells based on the optimal conditions achieved quality heterojunction, low defect density and better charge transfer capability. This work provides a new strategy for the development of the environmentally friendly and low-cost flexible CZTSSe solar cells.

CdS Induced Passivation toward High Efficiency and Stable Planar Perovskite Solar Cells.

In perovskite solar cells, the halide vacancy defects on the perovskite film surface/interface will instigate charge recombination, leading to a decrease in cell performance. In this study, cadmium sulfide (CdS) has been introduced into the precursor solution to reduce the halide vacancy defects and improve the cell performance. The highest efficiency of the device reaches 21.62%. Density functional theory calculation reveals that the incorporated Cd2+ ions can partially replace Pb2+ ions, thus forming a strong Cd-I bond and effectively reducing iodide vacancy defects (VI); at the same time, the loss of the charge recombination is significantly reduced because VI is filled by S2- ions. Besides, the substitution of Cd2+ for Pb2+ could increase the generation of PbI2, which can further passivate the grain boundary. Therefore, the stability of the cells, together with the efficiency of the power conversion efficiencies (PCEs), is also improved, maintaining 87.5% of its initial PCEs after being irradiated over 410 h. This work provides a very effective strategy to passivate the surface/interface defects of perovskite films for more efficient and stable optoelectronic devices.

Coordination engineering of Cu-Zn-Sn-S aqueous precursor for efficient kesterite solar cells.

Aqueous precursors provide an alluring approach for low-cost and environmentally friendly production of earth-abundant Cu2ZnSn(S, Se)4 (CZTSSe) solar cells. The key is to find an appropriate molecular agent to prepare a stable solution and optimize the coordination structure to facilitate the subsequent crystallization process. Herein, we introduce thioglycolic acid (TGA), which possesses strong coordination (SH) and hydrophilic (COOH) groups, as the agent and use deprotonation to regulate the coordination competition within the aqueous solution. Ultimately, metal cations are adequately coordinated with thiolate anions, and carboxylate anions are released to become hydrated to form an ultrastable aqueous solution. These factors have contributed to achieving CZTSSe solar cells with an efficiency as high as 12.3% (a certified efficiency of 12.0%) and providing an extremely wide time window for precursor storage and usage. This work represents significant progress in the non-toxic solution fabrication of CZTSSe solar cells and holds great potential for the development of CZTSSe and other metal sulfide solar cells.

Intermolecular π-π Conjugation Self-Assembly to Stabilize Surface Passivation of Highly Efficient Perovskite Solar Cells.

Surface passivation is an effective approach to eliminate defects and thus to achieve efficient perovskite solar cells, while the stability of the passivation effect is a new concern for device stability engineering. Herein, tribenzylphosphine oxide (TBPO) is introduced to stably passivate the perovskite surface. A high efficiency exceeding 22%, with steady-state efficiency of 21.6%, is achieved, which is among the highest performances for TiO2 planar cells, and the hysteresis is significantly suppressed. Further density functional theory (DFT) calculation reveals that the surface molecule superstructure induced by TBPO intermolecular π-π conjugation, such as the periodic interconnected structure, results in a high stability of TBPO-perovskite coordination and passivation. The passivated cell exhibits significantly improved stability, with sustaining 92% of initial efficiency after 250 h maximum-power-point tracking. Therefore, the construction of a stabilized surface passivation in this work represents great progress in the stability engineering of perovskite solar cells.

Enhanced Perovskite Solar Cell Efficiency Via the Electric-Field-Induced Approach.

The stability issue hinders the commercialization of the perovskite solar cells (PSCs), which is widely recognized. The efficiency generally decreases over time during the working condition. Here, we report an efficiency enhancement phenomenon of PSCs in the stability test at the maximum power point, which is speculated to be related to the electric-field-induced ion migration. The defect density and efficiency-related parameters were traced in situ by admittance spectroscopy and transient photovoltage when the cell works under bias voltage. The performance enhancement was revealed to be attributed to the reduction of the cell defects owing to ion migration. An efficiency of 22.3% can be achieved after the bias voltage was kept for 8 h. These findings suggest that ion migration is a double-edged sword that affects the electrical stability of PSCs, which presents a potential approach to improve the device's stability by appropriately controlling the defect states.

Application of Cesium on the Restriction of Precursor Crystallization for Highly Reproducible Perovskite Solar Cells Exceeding 20% Efficiency.

In this study, we systematically explored the mixed-cation perovskite Cs x(MA0.4FA0.6)1- xPbI3 fabricated via sequential introduction of cations. The details of the effects of Cs+ on the fabrication and performance of inorganic-organic mixed-cation perovskite solar cells examined in detail in this study are beyond the normal understanding of the adjusting band gap. It is found that a combined intercalation of Cs+ and dimethyl sulfoxide (DMSO) in PbI2-DMSO precursor film formed a strong and steady coordinated intermediate phase to retard PbI2 crystallization, suppress yellow nonperovskite δ-phase, and obtain a highly reproducible perovskite film with less defects and larger grains. The Cs-contained triple-cation-mixed perovskite Cs0.1(MA0.4FA0.6)0.9PbI3 devices yield over 20% reproducible efficiencies, superior stabilities, and fill factors of around 0.8 with a very narrow distribution.

Electropolymerization Porous Aromatic Framework Film As a Hole-Transport Layer for Inverted Perovskite Solar Cells with Superior Stability.

PAF-86 film is electropolymerized (EP) by targeted monomer M1 tethered bifunctional carbozolyl moieties which not only serve in electron donation but also provide effective electrochemical (EC) active sites. The resulting PAF-86 film possesses a fairly compact surface, remarkable stability, efficient hole extraction capacity, and hole-transporting materials (HTMs) for inverted heterojunction perovskite solar cells (PSCs). Likewise, our investigation shows that PAF-86 film based perovskite solar cells (PSCs) retained about 80% power conversion efficiency (PCE) without encapsulation in air, and poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) based PSCs devices reduce to 4% under the same conditions. More impressively, the electropolymerization approach is convenient, controlled, and operated at ambient conditions which elude post heat-treatments and are appropriate for industrial application.

DMF as an Additive in a Two-Step Spin-Coating Method for 20% Conversion Efficiency in Perovskite Solar Cells.

DMF as an additive has been employed in FAI/MAI/IPA (FA= CH2(NH2)2, MA = CH3NH3, IPA = isopropanol) solution for a two-step multicycle spin-coating method in order to prepare high-quality FAxMA1-xPbI2.55Br0.45 perovskite films. Further investigation reveals that the existence of DMF in the FAI/MAI/IPA solution can facilitate perovskite conversion, improve the film morphology, and reduce crystal defects, thus enhancing charge-transfer efficiency. By optimization of the DMF amount and spin-coating cycles, compact, pinhole-free perovskite films are obtained. The nucleation mechanisms of perovskite films in our multicycle spin-coating process are suggested; that is, the introduction of DMF in the spin-coating FAI/MAI/IPA solution can lead to the formation of an amorphous phase PbX2-AI-DMSO-DMF (X = I, Br; A = FA, MA) instead of intermediate phase (MA)2Pb3I8·2DMSO. This amorphous phase, similar to that in the one-step method, can help FAI/MAI penetrate into the PbI2 framework to completely convert into the perovskite. As high as 20.1% power conversion efficiency (PCE) has been achieved with a steady-state PCE of 19.1%. Our work offers a simple repeatable method to prepare high-quality perovskite films for high-performance PSCs and also help further understand the perovskite-crystallization process.