For methylammonium lead iodide perovskite solar cells prepared by co-evaporation, power conversion efficiencies of over 20% have been already demonstrated, however, so far, only in n-i-p ...configuration. Currently, the overall major challenges are the complex evaporation characteristics of organic precursors that strongly depend on the underlying charge selective contacts and the insufficient reproducibility of the co-evaporation process. To ensure a reliable co-evaporation process, it is important to identify the impact of different parameters in order to develop a more detailed understanding. In this work, we study the influence of the substrate temperature, underlying hole-transport layer (polymer PTAA versus self-assembling monolayer molecule MeO-2PACz), and perovskite precursor ratio on the morphology, composition, and performance of co-evaporated p-i-n perovskite solar cells. We first analyze the evaporation of pure precursor materials and show that the adhesion of methylammonium iodide (MAI) is significantly reduced with increased substrate temperature, while it remains almost unaffected for lead iodide (PbI2). This substrate temperature-dependent evaporation behavior of MAI is also transferred to the co-evaporation process and can directly influence the perovskite composition. We demonstrate that the optimal substrate temperature window for perovskite deposition is close to room temperature. At high temperature, not enough MAI for precise stoichiometry is incorporated even with very high MAI rates. While, at temperatures below −25 °C, the conversion of MAI with PbI2 is inhibited, and an amorphous yet unreacted film is formed. We observe that perovskite composition and morphology vary widely between the organic hole-transport layers (HTLs) PTAA and MeO-2PACz. For all substrate temperatures, MeO-2PACz enables higher solar cell PCEs than PTAA. Through the combination of vapor-deposited perovskites and a self-assembled monolayer, we achieve a stabilized power conversion efficiency of 20.6%, which is the first reported PCE above 20% for evaporated perovskite solar cells in p-i-n architecture.
Hybrid lead halide perovskites are promising materials for future photovoltaics applications. Their spectral response can be readily tuned by controlling the halide composition, while their stability ...is strongly dependent on the film morphology and on the type of organic cation used. Mixed cation and mixed halide systems have led to the most efficient and stable perovskite solar cells reported, so far they are prepared exclusively by solution‐processing. This might be due to the technical difficulties associated with the vacuum deposition from multiple thermal sources, requiring a high level of control over the deposition rate of each precursor during the film formation. In this report, thermal vacuum deposition with multiple sources (3 and 4) is used to prepare for the first time, multications/anions perovskite compounds. These thin‐film absorbers are implemented into fully vacuum deposited solar cells using doped organic semiconductors. A maximum power conversion efficiency of 16% is obtained, with promising device stability. The importance of the control over the film morphology is highlighted, which differs substantially when these compounds are vacuum processed. Avenues to improve the morphology and hence the performance of fully vacuum processed multications/anions perovskite solar cells are proposed.
Multiple‐source (up to 4) thermal vacuum deposition is used to prepare for the first time multications/anions perovskite compounds. These thin‐film absorbers are implemented into fully vacuum deposited solar cells using doped organic semiconductors. A maximum power conversion efficiency of 16% is obtained, with promising device stability.
Trap-assisted recombination, despite being lower as compared with traditional inorganic solar cells, is still the dominant recombination mechanism in perovskite solar cells (PSCs) and limits their ...efficiency. We investigate the attributes of the primary trap-assisted recombination channels (grain boundaries and interfaces) and their correlation to defect ions in PSCs. We achieve this by using a validated device model to fit the simulations to the experimental data of efficient vacuum-deposited p–i–n and n–i–p CH3NH3PbI3 solar cells, including the light intensity dependence of the open-circuit voltage and fill factor. We find that, despite the presence of traps at interfaces and grain boundaries (GBs), their neutral (when filled with photogenerated charges) disposition along with the long-lived nature of holes leads to the high performance of PSCs. The sign of the traps (when filled) is of little importance in efficient solar cells with compact morphologies (fused GBs, low trap density). On the other hand, solar cells with noncompact morphologies (open GBs, high trap density) are sensitive to the sign of the traps and hence to the cell preparation methods. Even in the presence of traps at GBs, trap-assisted recombination at interfaces (between the transport layers and the perovskite) is the dominant loss mechanism. We find a direct correlation between the density of traps, the density of mobile ionic defects, and the degree of hysteresis observed in the current–voltage (J–V) characteristics. The presence of defect states or mobile ions not only limits the device performance but also plays a role in the J–V hysteresis.
Efficient monolithic perovskite/perovskite tandem solar cells are fabricated using two perovskite absorbers with complementary bandgaps. By employing doped organic semiconductors, an efficient and ...selective extraction of the charge carriers is ensured. This study demonstrates perovskite/perovskite tandem cells delivering a maximum efficiency of 18%, highlighting the potential of vacuum‐deposited multilayer structures in overcoming the efficiency of single‐junction perovskite devices.
Halide perovskites have generated considerable research interest due to their excellent optoelectronic properties in the past decade. To ensure the formation of high-quality semiconductors, the ...deposition process for the perovskite film is a critical issue. Vacuum-based processing is considered to be a promising method, allowing, in principle, for uniform deposition on a large area. One of the benefits of vacuum processing is the control over the film composition through the use of quartz crystal microbalances (QCMs) that monitor the rates of the components in situ. In metal halide perovskites, however, one frequently employed component or precursor, CH3NH3I, exhibits nonstandard sublimation properties. Here, we study in detail the sublimation properties of CH3NH3I and demonstrate that by correcting for its complex adsorption properties and by modeling the film growth, accurate predictions of the stoichiometry of the final perovskite film can be obtained.
To improve the efficiency of existing perovskite solar cells (PSCs), a detailed understanding of the underlying device physics during their operation is essential. Here, a device model has been ...developed and validated that describes the operation of PSCs and quantitatively explains the role of contacts, the electron and hole transport layers, charge generation, drift and diffusion of charge carriers and recombination. The simulation to the experimental data of vacuum‐deposited CH3NH3PbI3 solar cells over multiple thicknesses has been fit and the device behavior under different operating conditions has been studied to delineate the influence of the external bias, charge‐carrier mobilities, energetic barriers for charge injection/extraction and, different recombination channels on the solar cell performance. By doing so, a unique set of material parameters and physical processes that describe these solar cells is identified. Trap‐assisted recombination at material interfaces is the dominant recombination channel limiting device performance and passivation of traps increases the power conversion efficiency (PCE) of these devices by 40%. Finally, guidelines to increase their performance have been issued and it is shown that a PCE beyond 25% is within reach.
A numerical model is developed and validated that describes the operation of perovskite solar cells and quantitatively explains the role of contacts, the charge transport layers, charge generation, drift and diffusion of carriers and recombination. By doing so, a unique set of material parameters and physical processes is identified that describes these solar cells. To increase their performance, some guidelines are issued.
Vacuum deposition techniques are used to prepare mixed iodide–bromide methylammonium lead perovskite diodes via an intermediate double layer of the pure iodide and bromide perovskites. The diodes ...lead to bright electroluminescence, whose emission spectra maxima shift from the infrared toward the visible with increasing bromide content. When illuminated with AM1.5 simulated sunlight the devices function as efficient solar cells with power conversion efficiencies as high as 12.9%.
Wide bandgap perovskites are being widely studied in view of their potential applications in tandem devices and other semitransparent photovoltaics. Vacuum deposition of perovskite thin films is ...advantageous as it allows the fabrication of multilayer devices, fine control over thickness and purity, and it can be upscaled to meet production needs. However, the vacuum processing of multicomponent perovskites (typically used to achieve wide bandgaps) is not straightforward, because one needs to simultaneously control several thermal sources during the deposition. Here a simplified dual‐source vacuum deposition method to obtain wide bandgap perovskite films is shown. The solar cells obtained with these materials have similar or even larger efficiency as those including multiple A‐cations, but are much more thermally stable, up to 3500 h at 85 °C for a perovskite with a bandgap of 1.64 eV. With optimized thickness, record efficiency of >19% and semitransparent devices with stabilized power output in excess of 17% are achieved.
A simplified vacuum deposition method to deposit wide bandgap perovskites is reported. The solar cells have similar or even larger efficiency as those including multiple A‐cations, and are much more thermally stable, up to 3500 h at 85 °C for a bandgap of 1.64 eV. Record efficiency of >19% and semi‐transparent devices with stabilized power output >17% are achieved.
Vacuum deposition methods are increasingly applied to the preparation of perovskite films and devices, in view of the possibility to prepare multilayer structures at low temperature. ...Vacuum-deposited, wide-bandgap solar cells based on mixed-cation and mixed-anion perovskites have been scarcely reported, due to the challenges associated with the multiple-source processing of perovskite thin films. In this work, we describe a four-source vacuum deposition process to prepare wide-bandgap perovskites of the type FA1–n Cs n Pb(I1–x Br x )3 with a tunable bandgap and controlled morphology, using FAI, CsI, PbI2, and PbBr2 as the precursors. The simultaneous sublimation of PbI2 and PbBr2 allows the relative Br/Cs content to be decoupled and controlled, resulting in homogeneous perovskite films with a bandgap in the 1.7–1.8 eV range and no detectable halide segregation. Solar cells based on 1.75 eV bandgap perovskites show efficiency up to 16.8% and promising stability, maintaining 90% of the initial efficiency after 2 weeks of operation.
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