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Pulsed laser deposition (PLD) has already been adopted as a low damage deposition technique of transparent conducting oxides on top of sensitive organic charge transport layers in optoelectronic devices. Herein, SnO2 deposition is demonstrated as buffer layer in p–i–n perovskite solar cells (PSCs) via wafer-scale (4 inch) PLD at room temperature. The PLD SnO2 properties, its interface with perovskite/C60, and device performance are compared to atomic layer deposited (ALD) SnO2, i.e., state-of-the-art buffer layer in perovskite-based single junction and tandem photovoltaics. The PLD SnO2-based solar cells exhibit on par efficiencies (17.8%) with that of SnO2 fabricated using ALD. The solvent-free room temperature processing and wafer-scale approach of PLD open up possibilities for buffer layer formation with increased deposition rates while mitigating potential thermal or physical damage to the top organic layers. This is a promising outlook for fully physical vapor-processed halide PSCs and optoelectronic devices requiring low thermal budget.

The inverted p-i-n perovskite solar cells hold high promise for scale-up toward commercialization. However, the interfaces between the perovskite and the charge transport layers contribute to major power conversion efficiency (PCE) loss and instability. Here, we use a single material of 2-thiopheneethylammonium chloride (TEACl) to molecularly engineer both the interface between the perovskite and fullerene-C60 electron transport layer and the buried interface between the perovskite and NiOx-based hole transport layer. The dual interface modification results in optimized band alignment, suppressed nonradiative recombination, and improved interfacial contact. A PCE of 24.3% is demonstrated, with open-circuit voltage (Voc) and fill factor (FF) of 1.17 V and 84.6%, respectively. The unencapsulated device retains >97.0% of the initial performance after 1000 h of maximum power point tracking under illumination. Moreover, a PCE of 22.6% and a remarkable FF of 82.4% are obtained for a mini-module with an active area of 3.63

Perovskite photovoltaics has achieved conversion efficiencies of 26.0% by optimizing the optoelectronic properties of the absorber and its interfaces with charge transport layers (CTLs). However, commonly adopted organic CTLs can lead to parasitic absorption and device instability. Therefore, metal oxides like atomic layer-deposited (ALD) SnO2 in combination with fullerene-based electron transport layers have been introduced to enhance mechanical and thermal stability. Instead, when ALD SnO2 is directly processed on the absorber, i.e., without the fullerene layer, chemical modifications of the inorganic fraction of the perovskite occur, compromising the device performance. This study focuses on the organic fraction, particularly the formamidinium cation (FA+), in a CsFAPb(I,Br)3 perovskite. By employing in situ infrared spectroscopy, we investigate the impact of ALD processing on the perovskite, such as vacuum level, temperature, and exposure to half and full ALD cycles using tetrakis(dimethylamido)-Sn(IV) (TDMA-Sn) and H2O. We observe that exposing the absorber to vacuum conditions or water half-cycles has a negligible effect on the chemistry of the perovskite. However, prolonged exposure at 100 °C for 90 min results in a loss of 0.7% of the total formamidinium-related vibrational features compared to the pristine perovskite. Supported by density functional theory calculations, we speculate that FA+ deprotonates and that formamidine desorbs from the perovskite surface. Furthermore, the interaction between TDMA-Sn and FA+ induces more decomposition of the perovskite surface compared to vacuum, temperature, or H2O exposure. During the exposure to 10 ALD half-cycles of TDMA-Sn, 4% of the total FA+-related infrared features are lost compared to the pristine perovskite. Additionally, IR spectroscopy suggests the formation and trapping of sym-triazine, i.e., a decomposition product of FA+. These studies enable to decouple the effects occurring during direct ALD processin

Single junction crystalline silicon (c-Si) solar cells are reaching their practical efficiency limit whereas perovskite/c-Si tandem solar cells have achieved efficiencies above the theoretical limit of single junction c-Si solar cells. Next to low-thermal budget silicon heterojunction architecture, high-thermal budget carrier-selective passivating contacts (CSPCs) based on polycrystalline-SiOx (poly-SiOx) also constitute a promising architecture for high efficiency perovskite/c-Si tandem solar cells. In this work, we present the development of c-Si bottom cells based on high temperature poly-SiOx CSPCs and demonstrate novel high efficiency four-terminal (4T) and two-terminal (2T) perovskite/c-Si tandem solar cells. First, we tuned the ultra-thin, thermally grown SiOx. Then we optimized the passivation properties of p-type and n-type doped poly-SiOx CSPCs. Here, we have optimized the p-type doped poly-SiOx CSPC on textured interfaces via a two-step annealing process. Finally, we integrated such bottom solar cells in both 4T and 2T tandems, achieving 28.1% and 23.2% conversion efficiency, respectively.

Monolithic perovskite/c-Si tandem solar cells have attracted enormous research attention and have achieved efficiencies above 30%. This work describes the development of monolithic tandem solar cells based on silicon heterojunction (SHJ) bottom- and perovskite top-cells and highlights light management techniques assisted by optical simulation. We first engineered (i)a-Si:H passivating layers for (100)-oriented flat c-Si surfaces and combined them with various (n)a-Si:H, (n)nc-Si:H, and (n)nc-SiOx:H interfacial layers for SHJ bottom-cells. In a symmetrical configuration, a long minority carrier lifetime of 16.9 ms was achieved when combining (i)a-Si:H bilayers with (n)nc-Si:H (extracted at the minority carrier density of 1015 cm–3). The perovskite sub-cell uses a photostable mixed-halide composition and surface passivation strategies to minimize energetic losses at charge-transport interfaces. This allows tandem efficiencies above 23% (a maximum of 24.6%) to be achieved using all three types of (n)-layers. Observations from experimentally prepared devices and optical simulations indicate that both (n)nc-SiOx:H and (n)nc-Si:H are promising for use in high-efficiency tandem solar cells. This is possible due to minimized reflection at the interfaces between the perovskite and SHJ sub-cells by optimized interference effects, demonstrating the applicability of such light management techniques to various tandem structures.

Solar-assisted water electrolysis is a promising technology for storing the energy of incident solar irradiation into hydrogen as a fuel. Here, an integrated continuous flow electrochemical reactor coupled to a monolithic perovskite-silicon tandem solar cell is demonstrated that provides light-driven electrochemical solar-to-hydrogen conversion with an energy conversion efficiency exceeding 21% at 1-Sun equivalent light intensity and stable operation during three simulated day-night cycles.

The metal halide perovskite absorbers are prone to surface defects, which severely limit the power conversion efficiencies (PCEs) and the operational stability of the perovskite solar cells (PSCs). Herein, trace amounts of bithiophene propylammonium iodide (bi-TPAI) are applied to modulate the surface properties of the gas-quenched perovskite. It is found that the bi-TPAI surface treatment has negligible impact on the perovskite morphology, but it can induce a defect passivation effect and facilitate the charge carrier extraction, contributing to the gain in the open-circuit voltage (Voc) and fill factor. As a result, the PCE of the gas-quenched sputtered NiOx-based inverted PSCs is enhanced from the initial 20.0% to 22.0%. Most importantly, the bi-TPAI treatment can largely alleviate or even eliminate the burn-in process during the maximum power point tracking measurement, improving the operational stability of the devices.

In this work, atomic layer deposition (ALD) has been employed to prepare titanium oxysulfide (TiOxSy) thin films. Compositional control was achieved through a supercycle approach, where the ALD processes of TiOx and TiSx were interleaved. ALD was performed at 100, 150, and 200 °C, and tetrakis(dimethylamino)titanium (TDMAT), H2S, and H2O were used as precursors. It is shown that the conductivity and transparency of the film are highly tunable by controlling the composition of TiOxSy between pure TiSx and TiOx. Specifically, the incorporation of S enables the film resistivity to be reduced by up to 6 orders of magnitude, while the visible light absorption is increased significantly. It is furthermore shown that the resulting films are significantly more oxygen-rich than would be expected on the basis of the supercycle ratio, an effect which is more pronounced at higher deposition temperatures. Through mass spectrometry and in situ ellipsometry studies, this low S content is shown to originate from exchange reactions where S is replaced by O on the growth (sub)surface during H2O exposure. This is contrary to the common finding for ALD zinc, indium, and tin oxysulfide films, for which exchange reactions are known to favor S-rich films. These exchange reactions are shown to be more prominent at higher deposition temperatures and to persist until approximately 3–5 Å of TiOx has formed.

Solar-assisted water electrolysis is a promising technology for storing the energy of incident solar irradiation into hydrogen as a fuel. Here, an integrated continuous flow electrochemical reactor coupled to a monolithic perovskite-silicon tandem solar cell is demonstrated that provides light-driven electrochemical solar-to-hydrogen conversion with an energy conversion efficiency exceeding 21% at 1-Sun equivalent light intensity and stable operation during three simulated day-night cycles., Photovoltaic Materials and Devices

The chemistry of the interface between the metal halide perovskite absorber and the charge transport layer affects the performance and stability of metal halide perovskite solar cells (PSCs). The literature provides several examples of poor PSC conversion efficiency values, when electron transport layers (ETLs), such as SnO2 and TiO2, are processed by atomic layer deposition (ALD) directly on the perovskite absorber. In the present work, we shed light on the chemical modifications occurring at the perovskite surface, during ALD processing of SnO2 and TiO2, in parallel with the evaluation of the PSC cell performance. The ALD processes are carried out on a (Cs,FA)Pb(I,Br)3 perovskite by adopting tetrakis(dimethylamino)tin(IV) and tetrakis(dimethylamino)titanium(IV) as metal precursors and H2O as the coreactant for SnO2 and TiO2, respectively. Perovskite surface modification occurs in the form of an ultrathin PbBr2 layer. Furthermore, in the case of SnO2, halogen molecules are detected at the interface, in parallel with the initial growth of an oxygen-deficient SnO2. Subgap defect states just above the valence band maximum of SnO2 are also detected. These states act as hole traps at the perovskite/SnO2 interface, subsequently promoting charge recombination and deteriorating the performance of the cell. We hypothesize that a redox reaction between the perovskite, or its decomposition products, and the Sn metal center of the ALD precursor takes place: I− and Br− are oxidized to I2 and Br2, respectively, and Sn(IV) is reduced to Sn(II). In contrast, the Ti(IV) metal center does not undergo any redox process, and, as a result, a promising 11% power conversion efficiency is measured with TiO2 as the ETL. This result strongly suggests that TiO2 may be a more suitable ETL, when processed directly on the perovskite absorber.