Interfacial Modification for High-Efficiency Vapor-Phase-Deposited Perovskite Solar Cells Based on a Metal Oxide Buffer Layer.

Vacuum deposition is one of the most technologically relevant techniques for the fabrication of perovskite solar cells. The most efficient vacuum-based devices rely on doped organic contacts, compromising the long-term stability of the system. Here, we introduce an inorganic electron-transporting material to obtain power conversion efficiencies matching the best performing vacuum-deposited devices, with open-circuit potential close to the thermodynamic limit. We analyze the leakage current reduction and the interfacial recombination improvement upon use of a thin (<10 nm) interlayer of C60, as well as a more favorable band alignment after a bias/ultraviolet light activation process. This wo…

Consistent device simulation model describing perovskite solar cells in steady-state, transient, and frequency domain

​This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials & Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acsami.9b04991

Efficient Vacuum Deposited P-I-N Perovskite Solar Cells by Front Contact Optimization.

Hole transport layers HTLs are of fundamental importance in perovskite solar cells PSCs , as they must ensure an efficient and selective hole extraction, and ohmic charge transfer to the corresponding electrodes. In p i n solar cells, the ITO HTL is usually not ohmic, and an additional interlayer such as MoO3 is usually placed in between the two materials by vacuum sublimation. In this work, we evaluated the properties of the MoO3 TaTm TaTm is the HTL N4,N4,N4 amp; 8243;,N4 amp; 8243; tetra [1,1 amp; 8242; biphenyl] 4 yl [1,1 amp; 8242; 4 amp; 8242;,1 amp; 8243; terphenyl] 4,4 amp; 8243; diamine hole extraction interface by selectively annealing either MoO3 prior to the deposition of TaTm o…

Use of Hydrogen Molybdenum Bronze in Vacuum‐Deposited Perovskite Solar Cells

Herein, the dehydration of a hydrogen molybdenum bronze (HYMoO3), converting it to molybdenum oxide (MoOX), is explored toward the development of perovskite solar cells (PSCs) for the first time. H0.11MoO3 bronze is synthesized, characterized, and deposited on indium tin oxide (ITO) under different concentrations and annealing conditions for in situ conversion into MoOX with appropriate oxygen vacancies. Vacuum‐deposited PSCs are fabricated using the as‐produced MoOX hole injection layers, achieving a power conversion efficiency of 17.3% (average) for the optimal device. The latter has its stability and reproducibility tested, proving the robustness and affordability of the developed hole t…

External quantum efficiency measurements used to study the stability of differently deposited perovskite solar cells

The instability exhibited by perovskite solar cells when exposed to the environment under illumination is one of the major obstacles for the entry of perovskite technology in the photovoltaic market. In this work, we use the external quantum efficiency (EQE) technique to study the photoinduced degradation of two types of solar cells having CH3NH3PbI3 as an absorber layer: one deposited by spin coating with an n-i-p architecture and the other deposited by evaporation with an inverted p-i-n structure. We also study the effect of different encapsulants to protect the cells against atmospheric agents. We find that EQE provides information regarding the areas of the cell most susceptible to degr…

Short photoluminescence lifetimes in vacuum-deposited ch3nh3pbI3 perovskite thin films as a result of fast diffusion of photogenerated charge carriers

It is widely accepted that a long photoluminescence (PL) lifetime in metal halide perovskite films is a crucial and favorable factor, as it ensures a large charge diffusion length leading to a high power conversion efficiency (PCE) in solar cells. It has been recently found that vacuumevaporated CH3NH3PbI3 (eMAPI) films show very short PL lifetimes of several nanoseconds. The corresponding solar cells, however, have high photovoltage (>1.1 V) and PCEs (up to 20%). We rationalize this apparent contradiction and show that eMAPI films are characterized by a very high diffusion coefficient D, estimated from modeling the PL kinetics to exceed 1 cm2/s. Such high D values are favorable for long di…

Room-Temperature Cubic Phase Crystallization and High Stability of Vacuum-Deposited Methylammonium Lead Triiodide Thin Films for High-Efficiency Solar Cells

Methylammonium lead triiodide (MAPI) has emerged as a high-performance photovoltaic material. Common understanding is that at room temperature it adopts a tetragonal phase and it only converts to the perfect cubic phase around 50-60 ºC. Most MAPI films are prepared using a solution-based coating process, yet they can also be obtained by vapor phase deposition methods. Vapor phase processed MAPI films have significantly different characteristics compared to their solvent processed analogous, such as a relatively small crystal grain sizes and short excited state lifetimes. Yet solar cells based on vapor phase processed MAPI films exhibit high power conversion efficiencies. Surprisingly, after…

Coating Evaporated MAPI Thin Films with Organic Molecules: Improved Stability at High Temperature and Implementation in High-Efficiency Solar Cells

Methylammonium lead iodide (MAPI) has proven to be an exceptional light-absorber for single-junction thin-film solar cells. Nonetheless, degradation induced by environmental agents (air, moisture, heat) limits the stability of this hybrid perovskite. Here, we demonstrate that coating evaporated MAPI thin films with different hydrophobic molecules leads to a significant improvement in their stability. We especially investigated the degradation of MAPI and the subsequent formation of PbI2 at 150 °C by in situ XRD analysis and showed that this transformation is remarkably slowed down in films coated with trioctyl phosphine oxide and tridodecyl methylammonium iodide. This enhances the processab…

Working mechanisms of vacuum-deposited perovskite solar cells

Molecular Passivation of MoO3: Band Alignment and Protection of Charge Transport Layers in Vacuum-Deposited Perovskite Solar Cells

Vacuum-deposition of perovskite solar cells can achieve efficiencies rivalling solution-based methods and it allows for more complex device stacks. MoO3 has been used to enhance carrier extraction to the transparent bottom electrode in a p-i-n configuration, here we show that by inserting an organic charge transport molecule it can also be used on the top of a perovskite absorber in a n-i-p configuration. This strategy enables the first vacuum-deposited perovskite solar cells with metal oxides as charge transporting layers for both electrons and holes leading to power conversion efficiency > 19 %.

Phosphomolybdic acid as an efficient hole injection material in perovskite optoelectronic devices.

Efficient perovskite devices consist in a perovskite film sandwiched in between charge selective layers, in order to avoid non-radiative recombination. A common metal oxide used as p-type or hole transport layer is molybdenum oxide. MoO3 is of particular interest for its very large work function, which allows it to be used both as an interfacial charge transfer material as well as a dopant for organic semiconductors. However, high quality and high work function MoO3 is typically thermally evaporated in vacuum. An alternative solution-processable high work function material is phosphomolybdic acid (PMA), which is stable, commercially available and environmentally friendly. In this communicat…

Simple approach for an electron extraction layer in all-vacuum processed n-i-p perovskite solar cell

Vacuum processing is considered to be a promising method allowing the scalable fabrication of perovskite solar cells (PSCs). In vacuum processed PSCs, the n-i-p structure employing organic charge transport layers is less common than the p-i-n structure due to limited options to achieve an efficient electron extraction layer (EEL) on indium tin oxide (ITO) with vacuum thermal evaporation. There are a number of specific applications where an n-i-p structure is required and therefore, it is of interest to have alternative solutions for the n-type contact in vacuum processed PSCs. In this work, we report an efficient vacuum deposited EEL using a mixture of conventional organic small molecules, …

Strontium Insertion in Methylammonium Lead Iodide: Long Charge Carrier Lifetime and High Fill-Factor Solar Cells.

The addition of Sr2+ in CH3 NH3 PbI3 perovskite films enhances the charge carrier collection efficiency of solar cells leading to very high fill factors, up to 85%. The charge carrier lifetime of Sr2+ -containing perovskites is in excess of 40 μs, longer than those reported for perovskite single crystals.

Interfacial engineering for single and multijunction vacuum-deposited perovskite solar cells

Radiative and non-radiative losses by voltage-dependent in-situ photoluminescence in perovskite solar cell current-voltage curves

Abstract The rapid development of perovskite solar cells has been based on improvements in materials and device architectures, yet further progress towards their theoretical limit will require a detailed study of the main physical processes determining the photovoltaic performance. Luminescence can be a key parameter for this purpose, as it directly assesses radiative recombination. We present steady-state absolute photoluminescence of an operating device at varying voltages as a tool to study the loss mechanisms in perovskite devices. The calibration to absolute photon numbers gives access to the variation of the relative radiative/non-radiative recombination weighted along the measured po…

Efficient wide band gap double cation – double halide perovskite solar cells

In this work we study the band gap variation and properties of the perovskite compound Cs0.15FA0.85Pb(BrxI1−x)3 as a function of the halide composition, with the aim of developing an efficient complementary absorber for MAPbI3 in all-perovskite tandem devices. We have found the perovskite stoichiometry Cs0.15FA0.85Pb(Br0.7I0.3)3 to be a promising candidate, thanks to its band gap of approximately 2 eV. Single junction devices using this perovskite absorber lead to a maximum PCE of 11.5%, among the highest reported for solar cells using perovskites with a band gap wider than 1.8 eV.

Perovskite Solar Cells: Stable under Space Conditions

Metal halide perovskite solar cells (PSCs) are of interest for high altitude and space applications due to their lightweight and versatile form factor. However, their resilience toward the particle spectrum encountered in space is still of concern. For space cells, the effect of these particles is condensed into an equivalent 1 MeV electron fluence. The effect of high doses of 1 MeV e-beam radiation up to an accumulated fluence to 10^16 e-cm-2 on methylammonium lead iodide perovskite thin films and solar cells is probed. By using substrate and encapsulation materials that are stable under the high energy e-beam radiation, its net effect on the perovskite film and solar cells can be studied.…

Hansen theory applied to the identification of nonhazardous solvents for hybrid perovskite thin-films processing

Abstract Metal-halide perovskites have become the most studied material for efficient next-generation solar cells, in part because of the possibility of depositing high quality semiconducting perovskites by simple solution-based methods. However, the majority of solvent systems implemented in literature for deposition of lead halide perovskites are hazardous to handle. Investigation of alternatives perovskite processing methods are hence key to safely upscale the perovskite photovoltaic manufacturing. In this manuscript we use the Hansen theory to find suitable nonhazardous solvents to solubilize two lead salts, PbBr2 and PbI2, used to fabricate the corresponding methylammonium (MA) lead ha…