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The most studied perovskite-based solar cells reported up to date contain the toxic lead in its composition. Photovoltaic research and development towards non-toxic, lead-free perovskite solar cells are critical to finding alternatives to reduce human health concerns associated with them. Bismuth-based perovskite variants, especially in the form of methylammonium bismuth iodide (MBI), is a good candidate for the non-toxic light absorber. However, the reported perovskite variant MBI thin films prepared by the solution process so far suffers from poor morphology and surface coverage. In this work, we investigate for the first time the optoelectronic, crystallographic and morphological properties of MBI thin films prepared via thermal co-evaporation of MAI and BiI3. We find by modifying the precursor ratio that the layer with pure MBI composition lead to uniform, compact and homogeneous layers, broadening the options of deposition techniques for lead-free based perovskite solar cells. [ABSTRACT FROM AUTHOR]

Efficient perovskite devices consist of a perovskite film sandwiched between charge selective layers, in order to avoid non-radiative recombination. A common metal oxide used as a 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 and a dopant for organic semiconductors. However, high quality and high work function MoO3 is typically thermally evaporated in a vacuum. An alternative solution-processable high work function material is phosphomolybdic acid (PMA), which is stable, commercially available and environmentally friendly. In this Communication, we show the first application of PMA in efficient vacuum processed perovskite devices. We found that the direct growth of perovskite films onto PMA leads to strong charge carrier recombination, hindering the solar cell photovoltage. Using an energetically suitable selective transport layer placed between PMA and the perovskite film, solar cells with efficiency ＞13% as well as LEDs with promising quantum efficiency can be obtained. [ABSTRACT FROM AUTHOR]

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 solutionprocessing. 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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Planar perovskite solar cells using organic charge selective contacts were fabricated. In a vacuum deposited perovskite-based solar cell, dopant and additive free triazatruxene as the hole transport layer was introduced for device fabrication. High open-circuit voltage of 1090 mV was obtained using methylammonium lead iodide ( E g =1.55 eV) as light harvesting material, thus representing a loss of only 460 mV which is in close vicinity of mature silicon technology (400 mV). The devices showed a very competitive photovoltaic performance, monochromatic incident photon-to-electron conversion efficiency of 80% and the power conversion efficiencies in excess of 15% were measured with a negligible degree of hysteresis. [ABSTRACT FROM AUTHOR]

We studied the effect of the charge transport layers in p-i-n perovskite solar cells using vacuum deposited methylammonium lead iodide thin-film absorbers. While solution-processed perovskite films are frequently deposited directly on PEDOT:PSS leading to good solar cell performances, in some cases even to very good V oc values, we show that in devices employing vacuum deposited MAPbI 3 perovskites, the removal of the polyTPD electron blocker substantially reduces the photovoltaic behavior. This is indicative of rather different charge transport properties in the vacuum deposited MAPbI 3 perovskites compared to those prepared from solution. On the other hand, we investigated the use of ionic interlayers as a possible alternative to low work function electrodes, whose reactivity towards air and moisture compromises the device stability. Two different electron extraction materials were evaluated as interlayers between the fullerene electron transport layer and a silver electrode, in particular a perylenediimide derivative and a conjugated polyelectrolyte. By studying the photovoltaic response and the electroluminescence properties of planar diodes using the ionic films and comparing them with devices employing barium, we found that such ionic interlayers can successfully replace the use of reactive electrodes, since they facilitate the electron extraction while reducing the non-radiative recombination at the electron transport interface. [ABSTRACT FROM AUTHOR]

Two novel and simple donor‐π‐bridge‐donor (D‐π‐D) hole‐transporting materials (HTMs) containing two units of the p‐methoxytriphenylamine (TPA) electron donor group covalently bridged by means of the 3,4‐dimethoxyselenophene spacer through single and triple bonds are reported. The optoelectronic and thermal properties of the new selenium‐containing HTMs have been determined using standard experimental techniques and theoretical density functional theory (DFT) calculations. The selenium‐based HTMs have been incorporated in mesoporous perovskite solar cells (PSCs) in combination with the triple‐cation perovskite [(FAPbI3)0.87(MAPbBr3)0.13]0.92 [CsPbI3]0.08. Limited values of power conversion efficiencies, up to 13.4 %, in comparison with the archetype spiro‐OMeTAD (17.8 %), were obtained. The reduced efficiencies showed by the new HTMs are attributed to their poor film‐forming ability, which constrains their photovoltaic performance due to the appearance of structural defects (pinholes). [ABSTRACT FROM AUTHOR]

Three novel donor–π‐bridge–donor (D‐π‐D) hole‐transporting materials (HTMs) featuring triazatruxene electron‐donating units bridged by different 3,4‐ethylenedioxythiophene (EDOT) π‐conjugated linkers have been synthesized, characterized, and implemented in mesoporous perovskite solar cells (PSCs). The optoelectronic properties of the new dumbbell‐shaped derivatives (DTTXs) are highly influenced by the chemical structure of the EDOT‐based linker. Red‐shifted absorption and emission and a stronger donor ability were observed in passing from DTTX‐1 to DTTX‐2 due to the extended π‐conjugation. DTTX‐3 featured an intramolecular charge transfer between the external triazatruxene units and the azomethine–EDOT central scaffold, resulting in a more pronounced redshift. The three new derivatives have been tested in combination with the state‐of‐the‐art triple‐cation perovskite [(FAPbI3)0.87(MAPbBr3)0.13]0.92[CsPbI3]0.08 in standard mesoporous PSCs. Remarkable power conversion efficiencies of 17.48 % and 18.30 % were measured for DTTX‐1 and DTTX‐2, respectively, close to that measured for the benchmarking HTM spiro‐OMeTAD (18.92 %), under 100 mA cm−2 AM 1.5G solar illumination. PSCs with DTTX‐3 reached a PCE value of 12.68 %, which is attributed to the poorer film formation in comparison to DTTX‐1 and DTTX‐2. These PCE values are in perfect agreement with the conductivity and hole mobility values determined for the new compounds and spiro‐OMeTAD. Steady‐state photoluminescence further confirmed the potential of DTTX‐1 and DTTX‐2 for hole‐transport applications as an alternative to spiro‐OMeTAD. [ABSTRACT FROM AUTHOR]

The synthesis of three enamine hole‐transporting materials (HTMs) based on Tröger's base scaffold are reported. These compounds are obtained in a three‐step facile synthesis from commercially available materials without the need of expensive catalysts, inert conditions or time‐consuming purification steps. The best performing material, HTM3, demonstrated 18.62 % PCE in PSCs, rivaling spiro‐OMeTAD in efficiency, and showing markedly superior long‐term stability in non‐encapsulated devices. In dopant‐free PSCs, HTM3 outperformed spiro‐OMeTAD by a factror of 1.6. The high glass‐transition temperature (Tg=176 °C) of HTM3 also suggests promising perspectives in device applications. [ABSTRACT FROM AUTHOR]

The synthesis of three enamine hole‐transporting materials (HTMs) based on Tröger's base scaffold are reported. These compounds are obtained in a three‐step facile synthesis from commercially available materials without the need of expensive catalysts, inert conditions or time‐consuming purification steps. The best performing material, HTM3, demonstrated 18.62 % PCE in PSCs, rivaling spiro‐OMeTAD in efficiency, and showing markedly superior long‐term stability in non‐encapsulated devices. In dopant‐free PSCs, HTM3 outperformed spiro‐OMeTAD by a factror of 1.6. The high glass‐transition temperature (Tg=176 °C) of HTM3 also suggests promising perspectives in device applications. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]