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Low‐temperature sol‐gel prepared ZnCo2O4 spinel‐based thin films are developed as high‐performance hole transporting layer (HTL) for coating perovskite film (NA‐Psk) from the basic MAPbI3/ACN/CH3NH2 solution in air without using anti‐solvent. Inverted PSC based on 2 mole% (vs Zn) Cu2+ doped ZnCo2O4 (2%Cu@ZnCo2O4) HTL and NA‐Psk absorber exhibit the maximum power conversion efficiency (PCE) of 20.0% with no current hysteresis while the cell based on ZnCo2O4 and PEDOT:PSS HTL (using NA‐Psk absorber) achieves the PCE of 15.79% and 12.3% with a current hysteresis index of 9.8% and 32.4%, respectively. Without encapsulation, PSCs based on 2%Cu@ZnCo2O4, ZnCo2O4, and PEDOT:PSS HTLs maintain 90%, 77%, and 12%, respectively of the original efficiency by standing in ambient atmosphere (temperature: 20–25 °C, RH:30%–40%) for 1800 h. Large area (10 cm × 10 cm substrate) perovskite mini‐module (PSM) with PCE over 15% is also demonstrated by using sol‐gel prepared 2%Cu@ZnCo2O4 HTL. The poor photovoltaic performance of PEDOT:PSS HTL is due to the basic MAPbI3/ACN/CH3NH2 solution will deprotonate the acidic PEDOT:PSS to reduce its conductivity whereas ZnCo2O4 HTL are not affected by basic perovskite precursor solution. [ABSTRACT FROM AUTHOR]

High-quality perovskite film is deposited on a 30 cm × 40 cm LiCoO2-coated ITO/glass via newly developed freely falling anti-solvent extraction (FFASE) method followed by post watervapor annealing in an ambient atmosphere. Perovskite solar modules (PSMs, active area of 25.2 cm2 with mask) based on this high-quality film achieve the highest efficiency of 16.04 and 30.76% under 1 sun (100 mW cm-2) and 945 lux fluorescent light illumination, respectively. The encapsulated PSMs are stable at -20 to 80 °C thermal cycling and keep high efficiency at temperature as low as -20 °C and as high as 80 °C. When the encapsulated PSM is heated at 85 °C and 85% relative humidity under room lighting or heated at 60 °C under AM1.5 (100 mW cm-2) illumination for 1000 h, loses only "8% of its original efficiency. The high stability of PSMs is due to very high quality perovskite absorber being used. The underlying concept of the FFASE method for extracting the solvent from the large-area perovskite precursor film is that the whole precursor film contacts with the fresh anti-solvent during the crystallization stage. [ABSTRACT FROM AUTHOR]

The oxide/nitride passivation and the flip‐chip package technology are developed for the perovskite solar cells. The heat resulting from the physical vapor deposition decomposes the active perovskite layer and degrades the efficiency of the perovskite solar cells down by more than 45%. Remarkably, with Si‐nitride passivation processed by plasma‐enhanced vapor deposition, the efficiency of the perovskite solar cell only decays about 9.1%. It is because that the plasma‐enhanced vapor deposition causes much less external energy on the perovskite solar cell. Using the exponential efficiency‐decay curves of the flip‐chip packaged perovskite solar cells, the characteristic time of the reliability‐tested solar cell can be calculated to be 145.8, 390.7, and 4864 h for air‐ambient, glove chamber, and water‐ambient tests, respectively. It is concluded that the concentration of O2(g) in the reliability test ambient is the root cause for the efficiency degradation of the perovskite solar cells. The low mobility of O2(g) under the water‐ambient reliability test results in the low probability of the adsorption of O2(g) on the surface of the flip‐chip package, which is the key factor for the least efficiency degradation of the perovskite solar cells among the three reliability tests. [ABSTRACT FROM AUTHOR]

Room‐temperature‐processed TiO2 (R‐Lt‐TiO2) electron transporting layers (ETLs) possess low conductivity and connectivity, resulting in poor photovoltaic performance. Herein, an ethanol (EtOH)‐soluble, highly conducting fullerene derivative, C60RT6, was used as an additive for Lt‐TiO2 ETLs. Room‐temperature processed nanocomposite ETL (R‐Fu/Lt‐TiO2) is prepared simply by spin coating a C60RT6 and G‐TiO2 NPs (TiO2 nanoparticle prepared by grinding the bulk TiO2 powder) mixture. R‐Fu/Lt‐TiO2 has better aligned with the frontier orbitals of the FAxMA1−xPbI3, better continuity, conductivity, flatness, and higher surface hydrophilicity compared to Lt‐TiO2 ETL. Perovskite films spin coated on R‐Fu/Lt‐TiO2 ETLs also have slightly larger grains and thickness compared to those deposited on Lt‐TiO2. Perovskite solar cells (PSCs) based on a R‐Fu/Lt‐TiO2 ETL possess higher power conversion efficiency (PCE, up to 20% on glass substrate), less (negligible) current hysteresis, and better long‐term stability compared to those using R‐Lt‐TiO2 as an ETL. The flexible PSC (used indium tin oxide/polyethylene terephthalate (ITO/PET) as a substrate) with a R‐Fu/Lt‐TiO2 ETL achieves a PCE of 18.06% and retains 90% of the initial PCE after 500 bending cycles with a bending radius of 6 mm. The PCE of the flexible cell with a Lt‐TiO2 ETL is only 8.2%, and loses 60% of the initial value after 500 bending cycles. [ABSTRACT FROM AUTHOR]

The sequential deposition of a NiOx hole‐transporting layer, one‐step CH3NH3PbI3 perovskite absorber, and blended electron‐transporting layer that comprises [6,6]‐phenyl‐C61‐butyric acid methyl ester (PCBM) and PNDI(2OD)T2 via automated ultrasonic spray‐coating technique is demonstrated in air for planar inverted p–i–n solution‐processed perovskite solar cells. Films fabricated via laboratory‐sale spin‐coating and industrially compatible spray‐coating process, respectively, are compared with each other to optimize both the film‐coating quality and corresponding device performance. This is validated by the photovoltaic performance of prototype devices with three spray‐coated layers with the active area of 1 × 1 cm2. The champion cells achieve a power conversion efficiency of 10.09%, which is one of the highest efficiencies obtained from fully spray‐processed large‐area perovskite solar cells thus far. Furthermore, these results reinforce the feasibility of the spray‐coating methodology for the fabrication of multilayers within perovskite solar cells stack and low‐cost route toward upscaling the manufacturing alternatives to spin coating. [ABSTRACT FROM AUTHOR]

Perovskite solar cells (PSCs) have received great attention due to their outstanding performance and their low processing costs. To boost their performance, one approach is to reinforce the built‐in electric field (BEF) to promote oriented carrier transport. The BEF is maximized by reinforcing the work function difference between cathode and anode (Δμ1) and increasing the work function difference between lower and upper surfaces of perovskite film (Δμ2) via introduction of electric dipole molecules, denoted as PTFCN and CF3BACl. The synergistic reinforcement of BEF improves charge transport and collection, and realizes markedly high photovoltaic performances with the best power conversion efficiency (PCE) up to 21.5%, a growth of 15.6% as compared to the control device, which is higher than the superposition of improvements achieved by either raising Δμ1 or Δμ2. Importantly, dual‐functional CF3BACl not only supplies dipole effect for tuning the surface potential of perovskite but offers hydrophobic trifluoride group toward the long‐term stable unencapsulated PSCs retaining more than 95% PCE after storing 2000 h under ambient conditions. This work demonstrates the synergistic effect of Δμ1 and Δμ2, providing an effective strategy for the further development of PSC in terms of photovoltaic conversion and stability. [ABSTRACT FROM AUTHOR]

A series of small‐molecule‐based hole‐transporting materials (HTMs) featuring a 4H‐cyclopenta[2,1‐b : 3,4‐b′]dithiophene as the central core with triphenylamine‐ and carbazole‐based side groups was synthesized and evaluated for perovskite solar cells. The correlations of the chemical structure of the HTMs on the photovoltaic performance were explored through different combinations of the central π‐bridge moieties. The optical and electrochemical properties, energy levels, and hole mobility were systematically investigated, revealing the significant influence of the central core planarity and packing structure on their photovoltaic performance. The optimized device based on CT1 exhibited a PCE (power conversion efficiency) of 17.71 % with a device architecture of FTO/TiO2 compact layer/TiO2 mesoporous/CH3NH3PbI3/HTM/MoO3/Ag, which was found to be on par with that of a cell fabricated based on state‐of‐the‐art spiro‐OMeTAD (16.97 %) as HTM. Moreover, stability assessment showed an improved stability for CPDT‐based HTMs in comparison with spiro‐OMeTAD over 1300 h. Four HTMs based on cyclopenta[2,1‐b;3,4‐b′]dithiophene core are designed and applied for lead perovskite (MAPbI3) solar cells. PSCs based on CT1 as HTM afford an impressive power conversion efficiency of 17.71 %. The devices based on the CT1 presented significantly higher stability than the device based on spiro‐OMeTAD. [ABSTRACT FROM AUTHOR]

Four heterocyclic spiro-type hole transporting materials (HTMs) carrying a spiro[fluorene-9,9′-xanthene] (SFX) (SFX-TPAM and SFX-TPA) or spiro[fluorene-9,9′-thioxanthene] (SFT) unit (SFT-TPAM and SFT-TPA) were synthesized through a low-cost facile route with high yields for perovskite solar cell (PSC) applications. In terms of absorption, these four compounds in the film state are all transparent at wavelengths longer than 430 nm, which is beneficial for allowing visible light to reach the perovskite active layer without being absorbed by the hole transporting layer (HTL). The photovoltaic performance of the inverted PSCs based on these small molecular HTMs with the device architecture of glass/ITO/HTL/CH3NH3PbI3/C60/BCP/Ag was tested. Only SFX-TPAM had its highest occupied molecular orbital (HOMO) level matched with the valence band of CH3NH3PbI3. The inverted PSC based on a dopant-free SFX-TPAM HTL achieves a power conversion efficiency of 10.23% under the illumination of standard one sun lighting, which is better than that (8.17%) of the cell based on dopant-free spiro-OMeTAD. The better photovoltaic performance of SFX-TPAM compared to spiro-OMeTAD may be due to the MAPbI3 film deposited on it having better quality. These results indicate that the facilely synthesized, low-cost SFX based small molecules can be used as the HTMs for PSCs. [ABSTRACT FROM AUTHOR]

The power conversion efficiency (PCE) of the perovskite solar cell is high enough to be commercially viable. The next important issue is the stability of the device. This article discusses the effect of the perovskite grain-size on the long-term stability of inverted perovskite solar cells. Perovskite films composed of various sizes of grains were prepared by controlling the solvent annealing time. The grain-size related stability of the inverted cells was investigated both in ambient atmosphere at relative humidity of approximately 30-40 % and in a nitrogen filled glove box (H2O<0.1 ppm, O2<10 ppm). The PCE of the solar cell based on a perovskite film having the grain size larger than 1 μm ( D-10) decreases less than 10 % with storage in a glove box and less than 15 % when it was stored under an ambient atmosphere for 30 days. However, the cell using the perovskite film composed of small (∼100 nm) perovskite grains (D-0) exhibits complete loss of PCE after storage under the ambient atmosphere for only 15 days and a PCE loss of up to 70 % with storage in the glove box for 30 days. These results suggest that, even under H2O-free conditions, the chemical- and thermal-induced production of pin holes at the grain boundaries of the perovskite film could be the reason for long-term instability of inverted perovskite solar cells. [ABSTRACT FROM AUTHOR]

A new class of hole-transport materials (HTMs) based on the bimesitylene core designed for mesoporous perovskite solar cells is introduced. Devices fabricated using two of these derivatives yield higher open-circuit voltage values than the commonly used spiro-OMeTAD. Power conversion efficiency (PCE) values of up to 12.11 % are obtained in perovskite-based devices using these new HTMs. The stability of the device made using the highest performing HTM ( P1) is improved compared with spiro-OMeTAD as evidenced through long-term stability tests over 1000 h. [ABSTRACT FROM AUTHOR]

This work presents a CHNHPbI/PCBM organic solar cell. Organic PCBM film and CHNHPbI perovskite film are deposited on the PEDOT:PSS/ITO glass substrate by the spin coating method. The performance of the organic solar cells was observed by changing the thickness of CHNHPbI perovskite. The thickness of a perovskite film can affect the carrier diffusion length in a device that strongly absorbs light in the red spectral region. The short-circuit current density and the power conversion efficiency were 21.9 mA/cm and 11.99 %, respectively, for the sample with 210-nm-thick CHNHPbI perovskite active layer. [ABSTRACT FROM AUTHOR]

Perovskite solar cells (PSCs) are one of the highly promising new‐generation photovoltaic technologies. One of the remaining challenges for commercializing PSCs is to prepare high‐quality, large‐area perovskite films in an ambient atmosphere reproducibly using less toxic materials. Herein, a nonvolatile, less toxic substance, 2‐pyrrolidinone (2P), is used as a complexant solvent for the perovskite precursor solution. Combining this with a newly developed spin‐assisted solvent extraction (SASE) crystallization method, a high‐quality perovskite film is prepared in air reproducibly. The nonvolatile nature of 2P and the formation of MAI–PbI2–2P adduct widen the time window for antisolvent engineering, and SASE enhances the solvent exchange rate of the precursor film to form a high‐quality perovskite film in air. An inverted cell (based on the postsolvent‐treated perovskite absorber) exhibits a power conversion efficiency of more than 18%. This film preparation method is feasible for depositing a high‐quality mixed‐cation or mixed‐cation, mixed‐halide perovskite film on both PEDOT:PSS and TiO2 surfaces to fabricate inverted and regular PSCs, respectively, to achieve efficiencies of more than 16%. More importantly, high‐quality, large‐area MAPbI3 film is prepared reproducibly in air for fabricating perovskite submodules to achieve an efficiency of 14% (verified at 13.04% after the cell is packed for efficiency evaluation). [ABSTRACT FROM AUTHOR]

From light to electricity: The inside cover picture illustrates the concept of designing hole transporting materials (HTMs) for perovskite solar cells. A subtle change of the central π‐bridge unit can lead to a significant improvement of device performance. In view of their excellent performance, the materials with two‐dimensional structural framework are promising HTMs for efficient and stable perovskite photovoltaic devices. More details can be found in the Full Paper by Yan‐Duo Lin et al. on page 307 in Issue 2, 2019 (10.1002/ente.201800939). [ABSTRACT FROM AUTHOR]

Sputtering made ZnO thin film was used as an electron-transport layer in a regular planar perovskite solar cell based on high quality CH3NH3PbI3 absorber prepared with a two-step spin-coating. An efficiency up to 15.9% under AM 1.5G irradiation is achieved for the cell based on ZnO film fabricated under Ar working gas. The atmosphere of the sputtering chamber can tune the surface electronic properties (band structure) of the resulting ZnO thin film and therefore the photovoltaic performance of the corresponding perovskite solar cell. Precise surface engineering of ZnO thin film was found to be one of the key steps to fabricate ZnO based regular planar perovskite solar cell with high power conversion efficiency. Sputtering method is proved to be one of the excellent techniques to prepare ZnO thin film with controllable properties. [ABSTRACT FROM AUTHOR]

An antisolvent (iodobenzene, IB) was used to assist the formation of closely packed CH 3 NH 3 PbI 3 (MAPbI 3 ) thin films during the one-step spin-coating process using different volumes of IB. The morphological, structural, optical and excitonic properties of MAPbI 3 thin films were analyzed using a contact-mode atomic-force microscope, X-ray diffractometer, broadband absorbance spectrometer and optical microscope-based time-resolved photoluminescence spectrometer. The properties of the resultant MAPbI 3 thin films can be manipulated by using different IB volumes, which dominates the device performance of MAPbI 3 based photovoltaic cells. The experimental results show that the grain size (or particle size) of MAPbI 3 thin films influences the collection of photoexcited carriers and the contact at the 6,6-Phenyl C 61 butyric acid methyl ester (PCBM)/MAPbI 3 interface, thereby resulting in a trade-off between the fill factor (FF) and short-circuit current density (J SC ). In addition, it is predicted that the power conversion efficiency (PCE) can be further improved by increasing the crystallinity of the MAPbI 3 thin film while keeping the small grain size. [ABSTRACT FROM AUTHOR]

A series of nonpolar antisolvents (chlorobenzene, bromobenzene, iodobenzene and toluene) were used to assist in the formation of smooth and crystalline CH 3 NH 3 PbI 3 thin films by a one-step spin-coating method. The structural, optical and excitonic characteristics of the resultant CH 3 NH 3 PI 3 thin films were analyzed using an atomic-force microscope, X-ray diffractometer, absorbance spectrum, photoluminescence (PL) spectrum, time-resolved PL and temperature-dependent PL. The properties of the CH 3 NH 3 PbI 3 thin films are dependent on the relative polarity and boiling point of the nonpolar antisolvents used in the washing treatment process. The interplay between nucleation (relative polarity) and crystal growth (boiling point) during the formation of CH 3 NH 3 PbI 3 thin films influences the short-circuit current density (J SC ) and power conversion efficiency (PCE) of the corresponding solar cells. The experimental results demonstrate that iodobenzene can be substituted for toluene as a more efficient antisolvent in the washing treatment process during the fabrication of CH 3 NH 3 PbI 3 thin films. In addition, it is predicted that the J SC and PCE can be further improved by increasing the crystallinity of the CH 3 NH 3 PbI 3 thin film. [ABSTRACT FROM AUTHOR]

Inverted-type perovskite solar cells offer the potential of fabrication by low-temperature solution processing as an alternative to conventional-type perovskite solar cells. PEDOT:PSS is commonly used as the hole transport layer (HTL), but its acidic nature may damage the reliability and stability of the photovoltaic device. In this study, we demonstrate the use of MoO x and WO x HTLs as an alternative to PEDOT:PSS for planar CH 3 NH 3 PbI 3 perovskite solar cells. Furthermore, the MoO x and WO x HTLs are treated using a UV-ozone treatment to improve the surface coverage of the perovskite layer. The resultant conversion efficiency (PCE) for the best cells at AM1.5G illumination with a shadow mask was 13.1%. [ABSTRACT FROM AUTHOR]

A phase-pure mixed-organic-cation perovskite absorber (MOC-PA) was fabricated by a one-step spin-coating process with a toluene washing treatment, and the structural, optical and excitonic properties of the resultant MOC-PAs were then characterized by scanning electron microscopy, X-ray diffractometry, absorbance spectrometer, and time-resolved photoluminescence. The averaged power conversion efficiency (PCE) of inverted phase-pure MOC-PA based photovoltaics could be improved from 12.21% to 13.28% by tailing the surface roughness of the poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) thin film from 1.43 nm to 1.84 nm. The improved PCE is mainly due to the increased short-circuit current density ( J SC ) which is attributed to the improvement of the exciton dissociation, as confirmed by photoluminescence experiments. In addition, the experimental results indicate that the PCE can be further improved by increasing the crystallinity of MOC-PAs. [ABSTRACT FROM AUTHOR]

This work studies annealing effects of the CH 3 NH 3 PbI 3 perovskite film for solar cell applications by time-resolved photoluminescence (TR-PL) spectra. The different thermal annealing temperatures process influences the quality and exciton lifetime of the CH 3 NH 3 PbI 3 perovskite film and importantly the device performance. The CH 3 NH 3 PbI 3 perovskite film of the optimal thermal annealing temperatures (100 °C) would significantly extended exciton lifetime and yield a higher open-circuit voltage, with short-circuit current density ( J SC ) = 21.58 mA/cm 2 , open-circuit voltage ( V OC ) = 0.84 V, fill factor (FF) = 61.4%, and η = 11.12%, respectively. [ABSTRACT FROM AUTHOR]

A comprehensive study was carried out to understand the formation of a crystalline tri-iodide perovskite absorber (TPA) on top of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS). Scanning electron microscopy, two-dimensional X-ray diffraction and nanosecond time-resolved photoluminescence were used to explore the correlation between the surface morphology and the exciton lifetime in TPA fabricated with and without the in-situ toluene washing treatment. The toluene washing treatment decreases the crystallinity (exciton lifetime) of TPA and improves the TPA coverage on the non-crystalline PEDOT:PSS surface. The high average power conversion efficiency (PCE) of 10.61% achieved can be explained as due to the efficient exciton dissociation at the interface between the TPA and the PEDOT:PSS. The experimental results show that the PCE can be further improved when the crystallinity of TPA and the TPA coverage on PEDOT:PSS are simultaneously optimized. [ABSTRACT FROM AUTHOR]

Comprehensive studies were carried out to understand the thickness effects of ZnO thin films for tri-iodide perovskite absorber (TPA) based photovoltaics, including the absorption spectrum, photoluminescence, nanosecond time-resolved photoluminescence (NTRPL), and photo-induced absorption (PIA) of TPA/ZnO/ITO/glass. These were carried out in order to explore the Urbach energy of TPA films and the exciton dissociation at the interface between TPA and ZnO. The results show that the thickness of the ZnO thin film significantly influences the photovoltaic performance in terms of open-circuit voltage ( V OC ), fill factor (FF), and short-circuit current density ( J SC ). In the case of the thicker ZnO film, the photovoltaics have the better FF and V oc , as a result of the smaller electron recombination. This means that a thicker ZnO film can block the electron recombination from the Fermi level of the ITO to the valance band of the TPA. On the other hand, the thicker ZnO film results in a higher J SC due to the better exciton dissociation at the interface between TPA and ZnO, which means that the electron mobility of the thicker ZnO is higher. Consequently, the photovoltaic performance can be expected to be improved by using a transparent cathode electrode with high conductivity and electron mobility. [ABSTRACT FROM AUTHOR]