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Register a new userCoordination Engineering of Cu-Zn-Sn-S Aqueous Precursor for Efficient Kesterite Solar Cells
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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, 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 efficiency of as high as 12.2% (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.
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The thermodynamic limit of photovoltaic efficiency for a single-junction solar cell can be readily predicted using the bandgap of the active light absorbing material. Such an approach overlooks the energy loss due to non-radiative electron-hole processes. We propose a practical ab initio procedure to determine the maximum efficiency of a thin-film solar cell that takes into account both radiative and non-radiative recombination. The required input includes the frequency-dependent optical absorption coefficient, as well as the capture cross-sections and equilibrium populations of point defects. For kesterite-structured Cu$_2$ZnSnS$_4$, the radiative limit is reached for a film thickness of around 2.6 micrometer, where the efficiency gain due to light absorption is counterbalanced by losses due to the increase in recombination current.
Various thin-film I$_2$-II-IV-VI$_4$ photovoltaic absorbers derived from kesterite Cu$_2$ZnSn(S,Se)$_4$ have been synthesized, characterized, and theoretically investigated in the past few years. The availability of this homogeneous materials dataset is an opportunity to examine trends in their defect properties and identify criteria to find new defect-tolerant materials in this vast chemical space. We find that substitutions on the Zn site lead to a smooth decrease in band tailing as the ionic radius of the substituting cation increases. Unfortunately, this substitution strategy does not ensure the suppression of deeper defects and non-radiative recombination. Trends across the full dataset suggest that Gaussian and Urbach band tails in kesterite-inspired semiconductors are two separate phenomena caused by two different antisite defect types. Deep Urbach tails are correlated with the calculated band gap narrowing caused by the (2I$_mathrm{II}$+IV$_mathrm{II}$) defect cluster. Shallow Gaussian tails are correlated with the energy difference between the kesterite and stannite polymorphs, which points to the role of (I$_mathrm{II}$+II$_mathrm{I}$) defect clusters involving Group IB and Group IIB atoms swapping across textit{different} cation planes. This finding can explain why textit{in-plane} cation disorder and band tailing are uncorrelated in kesterites. Our results provide quantitative criteria for discovering new kesterite-inspired photovoltaic materials with low band tailing.
Solution-processed quantum dots (QDs) have a high potential for fabricating low cost, flexible and large-scale solar energy harvesting devices. It has recently been demonstrated that hybrid devices employing a single monovalent cation perovskite solution for PbS QD surface passivation exhibit enhanced photovoltaic performance when compared to standard ligand passivation. Herein we demonstrate that the use of a triple cation Cs0.05(MA0.17FA0.83)0.95Pb(I0.9Br0.1)3 perovskite composition for surface passivation of the quantum dots results in highly efficient solar cells, which maintain 96 % of their initial performance after 1200h shelf storage. We confirm perovskite shell formation around the PbS nanocrystals by a range of spectroscopic techniques as well as high-resolution transmission electron microscopy. We find that the triple cation shell results in a favorable energetic alignment to the core of the dot, resulting in reduced recombination due to charge confinement without limiting transport in the active layer. Consequently, photovoltaic devices fabricated via a single-step film deposition reached a maximum AM1.5G power conversion efficiency of 11.3 % surpassing most previous reports of PbS solar cells employing perovskite passivation.
Solution-processed intrinsic ZnO and Al doped ZnO (ZnO:Al) were spin coated on textured n-type c-Si wafer to replace the phosphorus doped amorphous silicon as the electron selective transport layer (ESTL) of the Si heterojunction (SHJ) solar cells. Besides the function of electron selective transportation, the non-doped ZnO was found to possess certain passivation effect on c-Si wafer. The SHJ solar cells with different combinations of passivation layer (intrinsic a-Si:H, SiOx and non-doped ZnO) and electron transport layer (non-doped ZnO and ZnO:Al ) were fabricated and compared. An efficiency up to 18.46% was achieved on a SHJ solar cell with an a-Si:H/ZnO:Al double layer back structure. And, the all solution-processed non-doped ZnO/ZnO:Al combination layer presents fairly good electron selective transportation property for SHJ solar cell, resulting in an efficiency of 17.13%. The carrier transport based on energy band diagrams of the rear side of the solar cells has been discussed related to the performance of the SHJ solar cells.
We explore the degradation behaviour under continuous illumination and direct oxygen exposure of inverted unencapsulated formamidinium(FA)0.83Cs0.17Pb(I0.8Br0.2)3, CH3NH3PbI3, and CH3NH3PbI3-xClx perovskite solar cells. We continuously test the devices in-situ and in-operando with current-voltage sweeps, transient photocurrent, and transient photovoltage measurements, and find that degradation in the CH3NH3PbI3-xClx solar cells due to oxygen exposure occurs over shorter timescales than FA0.83Cs0.17Pb(I0.8Br0.2)3 mixed-cation devices. We attribute these oxygen-induced losses in the power conversion efficiencies to the formation of electron traps within the perovskite photoactive layer. Our results highlight that the formamidinium-caesium mixed-cation perovskites are much less sensitive to oxygen-induced degradation than the methylammonium-based perovskite cells, and that further improvements in perovskite solar cell stability should focus on the mitigation of trap generation during ageing.
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