Transition metal oxide (TMO) thin films exhibit large bandgap and hold great potential for enhancing the performance of silicon heterojunction (SHJ) solar cells by increasing the short-circuit current density significantly. On the other hand, achieving precise control over the electrical properties of TMO layers is crucial for optimizing their function as efficient carrier-selective layer. This study demonstrates a general and feasible approach for manipulating the quality of several TMO films, aimed at enhancing their applicability in silicon heterojunction (SHJ) solar cells. The core of our method involves precise engineering of the interface between the TMO film and the underlying hydrogenated intrinsic amorphous silicon passivation layer by managing the reaction of the TMO on the surface. X-ray photoelectron spectroscopy spectra demonstrate that our methods can modify the oxygen content in TMO films, thereby adjusting their electronic properties. By applying this method, we have successfully fabricated WO_x-based SHJ solar cells with 23.30 % conversion efficiency and V₂O_x-based SHJ solar cells with 22.04 % conversion efficiency, while keeping n-type silicon-based electron-transport layer at the rear side. This research paves the way for extending such interface engineering methods to other TMO materials used as hole-transport layers in SHJ solar cells.

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To increase the open-circuit voltage in solar cells based on triple cation, mixed halide perovskites, reducing recombination processes at the interfaces with transport layers (TLs) is key. Here, we investigated the charge carrier dynamics in bilayers and trilayers of Cs_0.05MA_0.10FA_0.85Pb(I_0.97Br_0.03)₃ (CsMAFA) combined with TLs using time-resolved microwave conductance (TRMC) measurements without and with bias illumination (BI). In the bilayers, we find balanced mobilities for electrons and holes in CsMAFA and nearly quantitative carrier extraction. The small, rapidly decaying TRMC signals for n-i-p- and p-i-n triple layers indicate both carriers are extracted. Applying BI leads to the charging of the TLs and the corresponding electric field prevents additional charge extraction, which demonstrates long-lived charge separation over the CsMAFA/TLs. Most importantly, for all bilayer combinations showing long-lived charge separation, an increase of the quasi-Fermi level splitting with respect to that of the CsMAFA layer is found.

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Passivating contacts are crucial for realizing high-performance crystalline silicon solar cells. Herein, contact formation by plasma-enhanced chemical vapor deposition (PECVD) followed by an annealing step is focused on. Poly-SiO_x passivating contacts by combining plasma-assisted N₂O-based oxidation of silicon (PANO-SiO_x) with a thin film of phosphorus (n⁺) or boron (p⁺)-doped hydrogenated amorphous silicon oxide (a-SiO_x:H) are manufactured. Postannealing is conducted for transitioning a-SiO_x:H into poly-SiO_x. The aim is to achieve a contact with low absorption and high-quality passivation. It is demonstrated that by tuning the plasma oxidation process time and power, the PANO-SiO_x thickness and its passivation quality can be controlled. A higher SiO₂ content is observed in PANO-SiO_x than in the nitric acid oxidation of silicon (NAOS-SiO_x) counterpart. PANO-SiO_x acts as a stronger diffusion barrier for both boron and phosphorus atoms compared to NAOS-SiO_x, affecting the dopant distribution during annealing. Implied open-circuit voltages up to 751 and 710 mV for n⁺ and p⁺ flat symmetric samples, respectively, are demonstrated. With respect to standard thermally grown SiO₂ tunneling oxide combined with (in/ex)situ-doped low-pressure chemical vapor deposition poly-Si, this study presents a simple alternative for manufacturing passivating contact fully based on PECVD processes.

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The preferential orientation of the perovskite (PVK) is typically accomplished by manipulation of the mixed cation/halide composition of the solution used for wet processing. However, for PVKs grown by thermal evaporation, this has been rarely addressed. It is unclear how variation in crystal orientation affects the optoelectronic properties of thermally evaporated films, including the charge carrier mobility, lifetime, and trap densities. In this study, we use different intermediate annealing temperatures Tinter between two sequential evaporation cycles to control the Cs0.15FA0.85PbI2.85Br0.15 orientation of the final PVK layer. XRD and 2D-XRD measurements reveal that when using no intermediate annealing primarily the (110) orientation is obtained, while when using Tinter = 100 °C a nearly isotropic orientation is found. Most interestingly for Tinter > 130 °C a highly oriented PVK (100) is formed. We found that although bulk electronic properties like photoconductivity are independent of the preferential orientation, surface related properties differ substantially. The highly oriented PVK (100) exhibits improved photoluminescence in terms of yield and lifetime. In addition, high spatial resolution mappings of the contact potential difference (CPD) as measured by KPFM for the highly oriented PVK show a more homogeneous surface potential distribution than those of the nonoriented PVK. These observations suggest that a highly oriented growth of thermally evaporated PVK is preferred to improve the charge extraction at the device level.@en

Multiple-source thermal evaporation is emerging as an excellent technique to obtain perovskite (PVK) materials for solar cell applications due to its solvent-free processing, accurate control of stoichiometric ratio, and potential for scalability. Nevertheless, the currently reported layer-by-layer deposition approach is afflicted by long processing times caused by the multiple repetitions of thin films, which hinder industrial uptake. On the other hand, the coevaporation entails higher complexity due to the challenges of controlling the sublimation of multiple sources simultaneously. In this work, we propose a simplified approach consisting of a single-cycle deposition (SCD) of three thick precursor layers to obtain high-quality Cs0.15FA0.85PbI2.85Br0.15 (CsFAPbIBr) films. After annealing, the optimized PVK film exhibits comparable properties to the one deposited by multicycle deposition in terms of crystal structure, in-depth uniformity, and optoelectrical properties. Also, the formation and evolution of SCD PVK during annealing are investigated. We found that, in the competitive processes of precursor diffusion and reaction, the presence of cesium bromide can assist precursor mixing driven by the annealing treatment, demonstrating a reaction-limited process in the PVK conversion. With this simplified SCD approach, a PVK film is obtained with expected optical and opto-electronic properties, providing an appealing way for future thermally evaporated PVK device preparation.

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Since the first application of a metal halide perovskite (PVK) absorber in a solar cell, these materials have drawn a great deal of attention in the photovoltaic (PV) community, showing exceptional rapid progress in power conversion efficiency. The potential advantages of low-cost, high efficiency, easy processability, and wide range of applications make PVK solar cells (PSCs) a desirable candidate for future uptake in the PV market over traditional semiconductors such as silicon. Furthermore, PVK thin-film technology holds a concrete potential to closely approach the theoretical efficiency limit for single-junction solar cells via unique control of the optoelectronic properties. However, for a disruptive breakthrough of PVK technology from fundamental research to industry, systematic research efforts are required to unravel the poor long-term stability and to reach a reliable large area fabrication process. In this review, we examine in detail recent progress on large-scale PSCs and we discuss challenges for commercialization touching upon the following aspects: material properties, fabrication technology, and industrialization challenges. Besides, the long-term stability and efficiency of large-area PSCs as well as PVK-based two-terminal tandem devices are discussed. In addition, strategies for PSC upscaling are further studied for scalable deposition technologies. Finally, we review the most recent literature on costs and environmental assessment.@en

Thin films of transition metal oxides such as molybdenum oxide (MoO_x) are attractive for application in silicon heterojunction solar cells for their potential to yield large short-circuit current density. However, full control of electrical properties of thin MoO_x layers must be mastered to obtain an efficient hole collector. Here, we show that the key to control the MoO_x layer quality is the interface between the MoO_x and the hydrogenated intrinsic amorphous silicon passivation layer underneath. By means of ab initio modelling, we demonstrate a dipole at such interface and study its minimization in terms of work function variation to enable high performance hole transport. We apply this knowledge to experimentally tailor the oxygen content in MoO_x by plasma treatments (PTs). PTs act as a barrier to oxygen diffusion/reaction and result in optimal electrical properties of the MoO_x hole collector. With this approach, we can thin down the MoO_x thickness to 1.7 nm and demonstrate short-circuit current density well above 40 mA/cm² and a champion device exhibiting 23.83% conversion efficiency.

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A high-quality perovskite film is critical to realize high-efficiency and hysteresis-less perovskite solar cells (PSCs). However, a solution-processed perovskite layer presents many ionic vacancies on grain boundaries, which serve as nonradiative recombination centers that cause a loss of photocurrent. Herein, a trace amount of Lewis base tert-butyl acrylate (TBA) with both effective C=O and C=C functional groups is introduced to synergistically control the crystallization process and saturate surface dangling bonds. The C=O groups of TBA strongly bond to the uncoordinated Pb2+ to be a more stable TBA-PbI2 Lewis adduct, slowing down the perovskite crystallization to form a high-crystalline quality film and suppressing the formation of nonradiative recombination defects at perovskite boundaries. In addition, the π-σ and π-πconjugated bonds of C=C and -C=O in TBA show a strong delocalized electron-rich structure, promoting the photogenerated charge carrier diffusion in the perovskite layer. As a consequence, the open-circuit voltage of a TBA-PSC is significantly increased from 1.07 to 1.12 V and the fill factor is improved from 78.20 to 81.56%. Thus, the TBA-PSC achieves a high power conversion efficiency of 22.82% with negligible hysteresis. Therefore, the TBA additive is a feasible and efficient method to improve the perovskite crystalline quality for high-performance PSCs.

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