Hybrid organic-inorganic perovskites (PVKs) offer exceptional optoelectronic performance, yet reproducible and scalable co-evaporation remains challenging. This study examines the interplay of factors affecting compositional control during three-source PVK deposition. We identify chamber pressure, precursor cross-contamination, and flux instability – especially from organic salts such as formamidinium iodide (FAI) – as major sources of variability. A critical influence is the occurrence of cross-reading, where omnidirectional evaporation of FAI contributes to the reading on the quartz crystal microbalance (QCM) sensors monitoring the inorganic precursors like caesium bromide (CsBr) and lead iodide (PbI₂) even though shielding is present. This effect, strongly dependent on FAI load, deposition rate, and QCM sensor position, erroneously inflates measured fluxes, leading to inaccurate rate control and unintentional compositional drift. Maintaining A-, B- and X-site stoichiometry therefore requires dynamic adjustment of precursor rates, particularly at higher deposition speeds where mean free path limitations come into play. We demonstrate the successful deposition of perovskite layers at a deposition speed of 27.8 nm min⁻¹ as the practical ceiling for the investigated Cs_xFA_1-xPb(I_1-xBr_x)₃ composition within our experimental framework. These findings highlight the delicate balance between deposition speed, precursor stability, and film quality, underscoring the need for improved delivery systems - such as continuous precursor feedthrough, multiple organic sources, alternative vapor transport or flash evaporation methods – to achieve reproducible, fast and large-scale fabrication of high-performance PVK films.

Polycrystalline silicon (poly-Si) carrier-selective passivating contacts (CSPCs), featuring high photoconversion efficiency (PCE) and cost-effectiveness, have emerged as a promising approach for high-efficiency crystalline silicon (c-Si) solar cells. To minimize parasitic absorption losses induced by doped poly-Si window layers, wide bandgap oxygen-alloyed poly-Si (poly-SiO_x) layers are developed. However, challenges persist in achieving excellent surface passivation for boron-doped poly-SiO_x contact stacks, likely caused by boron diffusion during annealing and the reduced doping concentration resulting from lower crystallinity as oxygen content increases. In this study, we investigate the impact on the passivating contact structure and solar cell performance of a 10-nm thick intrinsic hydrogenated amorphous silicon buffer layer with varying oxygen content (a-Si (O_x):H) deposited by plasma-enhanced chemical vapor deposition (PECVD), and placed between the tunneling silicon oxide (SiO_x) and the poly-SiO_x (p⁺). After the hydrogenation step, we obtain both high passivation quality with implied open circuit voltage (iV_oc) of 728.3 mV and low contact resistivity (ρ_c) of 59.18 mΩ cm² on polished surface for oxygen-free a-Si:H buffer layer. These improvements can be attributed to the appropriate thickness of the tunnel oxide and confirmed by transmission electron microscopy (TEM) images, to higher crystallinity of the buffer layer, which facilitates more efficient doping in the buffer layer. This is evidenced by energy dispersive X-ray spectroscopy (EDX), and X-ray photoelectron spectroscopy (XPS) results. At the device level, a front-side textured, rear-side flat, rear junction poly-SiO_x/poly-SiO_x solar cell on n-type c-Si wafer, an efficiency improvement can be observed from 3.55 % without a PECVD buffer layer to 18.9 % with an oxygen-free a-Si:H PECVD buffer layer. The impact of the buffer layer crystallinity on cell performance is further demonstrated by deploying a 10-nm thick LPCVD buffer layer, which facilitates an efficiency of 21.15 % for the same device structure.

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.

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.

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.

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.

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.

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.