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Despite organic/inorganic lead halide perovskite solar cells becoming one of the most promising next‐generation photovoltaic materials, instability under heat and light soaking remains unsolved. In this work, a highly hydrophobic cation, perfluorobenzylammonium iodide (5FBzAI), is designed and a 2D perovskite with reinforced intermolecular interactions is engineered, providing improved passivation at the interface that reduces charge recombination and enhances cell stability compared with benchmark 2D systems. Motivated by the strong halogen bond interaction, (5FBzAI)2PbI4 used as a capping layer aligns in in‐plane crystal orientation, inducing a reproducible increase of ≈60 mV in the Voc, a twofold improvement compared with its analogous monofluorinated phenylethylammonium iodide (PEAI) recently reported. This endows the system with high power conversion efficiency of 21.65% and extended operational stability after 1100 h of continuous illumination, outlining directions for future work. [ABSTRACT FROM AUTHOR]

Recently, perovskite solar cells (PSC) with high power‐conversion efficiency (PCE) and long‐term stability have been achieved by employing 2D perovskite layers on 3D perovskite light absorbers. However, in‐depth studies on the material and the interface between the two perovskite layers are still required to understand the role of the 2D perovskite in PSCs. Self‐crystallization of 2D perovskite is successfully induced by deposition of benzyl ammonium iodide (BnAI) on top of a 3D perovskite light absorber. The self‐crystallized 2D perovskite can perform a multifunctional role in facilitating hole transfer, owing to its random crystalline orientation and passivating traps in the 3D perovskite. The use of the multifunctional 2D perovskite (M2P) leads to improvement in PCE and long‐term stability of PSCs both with and without organic hole transporting material (HTM), 2,2′,7,7′‐tetrakis‐(N,N‐di‐p‐methoxyphenyl‐amine)‐9,9′‐spirobifluorene (spiro‐OMeTAD) compared to the devices without the M2P. [ABSTRACT FROM AUTHOR]

Nanoscale CH3NH3PbI3 perovskite sensitizers are grown by delivering each precursor successively onto the surface of mesoporous (meso) TiO2 electrodes. Using Pb(NO3)2 ions as a lead(II) source and CH3NH3I (MAI) for methylammonium and iodide sources, repetitive cycles of the two dipping steps are successful in growing few nanometer‐sized MAPbI3 gradually on the TiO2 surface inside the meso‐TiO2 film. However, some aggregates are observed on the top surface of the meso‐TiO2 film due to slight dissolution of PbI2 and its accumulation/reaction with MAI at the top surface of the meso‐TiO2 film. To solve this inhomogeneity of the deposition, a nondestructive multiple deposition route for nanoscale MAPbI3 is suggested as a successive precursor layer adsorption and reaction (SPLAR) process where, from the second cycle of deposition, PbI2 is delivered with the help of an ionic liquid compound dissolved in dichloromethane. With this new Pb precursor in less‐polar solvents, nanoscale MAPbI3 sensitizers are grown without dissolution of preformed perovskites or formation of some aggregates at the top surface. After the third cycle of SPLAR deposition, about 7.0 nm–sized MAPbI3 sensitizers are prepared and display enhanced photovoltaic performance (7.18 ± 0.31%) compared with devices obtained from only one cycle (5.74 ± 0.30%). [ABSTRACT FROM AUTHOR]

Engineering two-/three-dimensional (2D/3D) perovskite solar cells is nowadays a popular strategy for efficient and stable devices. However, the exact function of the 2D/3D interface in controlling the long-term device behavior is still obscure. Here, we reveal a dynamical structural mutation of the 2D/3D interface: the small cations in the 3D cage move towards the 2D layer, which acts as an ion scavenger. If structurally stable, the 2D layer physically blocks the ion movement at the interface boosting the device stability. Otherwise, the 2D layer embeds them, dynamically self-transforming into a quasi-2D structure. The judicious choice of the 2D constituent is decisive in controlling the 2D/3D kinetics and improving the device lifetime, opening a new avenue for perovskite interface design. [ABSTRACT FROM AUTHOR]

Abstract: The synthesis and characterization of two related families of star‐shaped thiophene‐containing hole‐transporting materials (HTMs) based on fused tetrathienoanthracene and nonfused tetrathienylbenzene cores are reported. All of them are endowed with four terminal (4,4′‐dimethoxy)diphenylamino groups that are either linked directly to the core or showed a different type of bridges (i.e., thiophene‐phenyl or phenyl rings). The novel HTMs are tested in mixed‐ion perovskite (Cs0.1FA0.74MA0.13PbI2.48Br0.39) solar cells, and power conversion efficiencies of up to 18.8% are measured under 1 sun irradiation, comparable with the efficiency obtained for the reference cell using 2,2′,7,7′‐tetrakis(N,N′‐di‐p‐methoxyphenylamine)‐9,9′‐spirobifluorene as an HTM. [ABSTRACT FROM AUTHOR]

Abstract: Planar perovskite solar cells using low‐temperature atomic layer deposition (ALD) of the SnO2 electron transporting layer (ETL), with excellent electron extraction and hole‐blocking ability, offer significant advantages compared with high‐temperature deposition methods. The optical, chemical, and electrical properties of the ALD SnO2 layer and its influence on the device performance are investigated. It is found that surface passivation of SnO2 is essential to reduce charge recombination at the perovskite and ETL interface and show that the fabricated planar perovskite solar cells exhibit high reproducibility, stability, and power conversion efficiency of 20%. [ABSTRACT FROM AUTHOR]

Tin oxide is an excellent candidate to replace mesoporous TiO2 electron transport layers (ETLs) in perovskite solar cells. Here, we introduced a SnO2 layer by a low-temperature solution process, and investigated its morphology, opto-physical and electrical properties affecting the device performance. We reveal that low-temperature processed SnO2 is self-passivating in nature, which leads to a high efficiency. To further enhance the blocking effect, we combined a compact TiO2 underlayer with the SnO2 contact layer, and found that the bi-layered ETL is superior compared to single layers. The best device shows photovoltaic values in a planar structure with a short-circuit current density (Jsc) of 22.58 mA cm−2, an open-circuit voltage (Voc) of 1.13 V, a fill factor (FF) of 0.78, and a power conversion efficiency (PCE) of 19.80% under 1 sunlight illumination. [ABSTRACT FROM AUTHOR]

Through judicious molecular engineering, novel dopant-free star-shaped D–π–A type hole transporting materials coded KR355, KR321, and KR353 were systematically designed, synthesized and characterized. KR321 has been revealed to form a particular face-on organization on perovskite films favoring vertical charge carrier transport and for the first time, we show that this particular molecular stacking feature resulted in a power conversion efficiency over 19% in combination with mixed-perovskite (FAPbI3)0.85(MAPbBr3)0.15. The obtained 19% efficiency using a pristine hole transporting layer without any chemical additives or doping is the highest, establishing that the molecular engineering of a planar donor core, π-spacer and periphery acceptor leads to high mobility, and the design provides useful insight into the synthesis of next-generation HTMs for perovskite solar cells and optoelectronic applications. [ABSTRACT FROM AUTHOR]

Dimethoxydiphenylamine-substituted dispiro-oxepine derivative 2,2′,7,7′-tetrakis-(N,N′-di-4-methoxyphenylamine)dispiro-[fluorene-9,4′-dithieno[3,2-c:2′,3′-e]oxepine-6′,9′′-fluorene] (DDOF) has been designed and synthesized using a facile synthetic route. The novel hole transporting material (HTM) was fully characterized and tested in perovskite solar cells exhibiting a remarkable power conversion efficiency of 19.4%. More importantly, compared with spiro-OMeTAD-based devices, DDOF shows significantly improved stability. The comparatively comprehensive solid structure study is attempted to disclose the common features of good performance HTMs. These achievements clearly demonstrated that the highly hindered DDOF can be an effective HTM for the fabrication of efficient perovskite solar cells and further enlightened the rule of new HTM's design. [ABSTRACT FROM AUTHOR]

In this work we systematically investigated the role of reduced graphene oxide (rGO) in hybrid perovskite solar cells (PSCs). By mixing rGO within the mesoporous TiO2 (m-TiO2) matrix, highly efficient solar cells with power conversion efficiency values up to 19.54 % were realized. In addition, the boosted beneficial role of rGO with and without Li-treated m-TiO2 is highlighted, improving transport and injection of photoexcited electrons. This combined system may pave the way for further development and optimization of electron transport and collection in high efficiency PSCs. [ABSTRACT FROM AUTHOR]

Although 2D|3D has shown potential for application in multifunctional devices, the principle of operation for multifunction devices (SOLAR Cell‐LED: SOLED) has not yet been revealed. However, most studies have reported that the devices have only one auspicious characteristic. Here in this study the SOLED devices are monitored and investigated in a 2D|3D heterostructure with a multidimensional perovskite. It is fond that a 2D|3D heterostructure with a multidimensional perovskite interface induces carrier transmission from the interface, increasing the density of electrons and holes, and increasing their recombination. An interface‐engineered perovskite 2D|3D‐heterojunction structure is employed to realize the multifunctional photonic device in on‐chip, exhibiting overall power conversion efficiencies of photovoltaics up to 21.02% under AM1.5, and external quantum efficiency of the light‐emitting diode up to 5.13%. This novel phenomenon is attributed to carrier transfer resulting in a high carrier density and enhanced carrier recombination at the 2D|3D interface. [ABSTRACT FROM AUTHOR]

Herein, the optoelectronic properties of interface‐engineered perovskite 2D|3D‐heterojunction structure solar cells are reported. The reciprocity theorem is applied to determine the maximum open‐circuit voltage (Voc) the device can deliver under solar illumination. A Voc of 1.295 V is found, analyzing the measured external quantum efficiency and assuming only radiative recombination. For comparison, the experimental open‐circuit voltage found for the studied 2D|3D heterojunctions is 1.15 V. The contribution of nonradiative recombination is explored by measuring the electroluminescence quantum yield. A quantum yield of 0.4% is found at current densities equivalent to 1 sun illumination. This translates into a Voc loss of ≈140 mV, which is in very good agreement with the experimental findings. In addition, the fundamental correlation between luminescence intensity and the chemical potential predicted by the generalized Planck law is confirmed for the photoluminescence measured at different light intensities when the device is operated under open‐circuit conditions and for the electroluminescence when operated under a forward bias. The investigations in this study suggest that further efficiency improvements can be achieved by reducing the nonradiative recombination in the studied solar cell. At the same time, a high‐performance near IR light emitting diode can be realized. [ABSTRACT FROM AUTHOR]

By two‐step sequential Pb2+ adsorption and reaction with methylammonium‐iodide (MAI) or ‐bromide (MABr) at a low concentration level of 0.06–0.10 m over mesoporous TiO2 or ZrO2 film, a well‐defined nanoscale CH3NH3PbI3 (MAPbI3) photosensitizer or CH3NH3PbBr3 (MAPbBr3) light emitter could be prepared in situ, respectively in a reproducible and atom‐economical way. The as‐prepared nanoscale perovskites are compared with their thin film counterparts in terms of light absorption/emission, crystallinity, surface morphology, and energy‐conversion efficiency. The nanoscale perovskite‐decorated films display more transparency than the bulky film due to the much lower amount deposited, while blueshifted and overwhelmingly brighter photoluminescence is observed in the "nano" relative to the "bulk" due to quantum size confinement. Transmission electron microscopy images also clearly show that a few nanometer‐sized perovskite dots are deposited homogeneously over the surface of TiO2‐ or ZrO2‐particulate film in the course of the current preparative route. When the nano‐MAPbI3 is tested as a photosensitizer in a solid‐state dye‐sensitized solar cell configuration with a very thin (≈650 nm) TiO2 mesoporous film, it has a promising initial power conversion efficiency of 6.23%, which outperformed the result of 2.28% from a typical organic molecular dye coded as MK‐2. A nanoscale MAPbI3 photosensitizer and MAPbBr3 light emitter are prepared in situ over mesoporous metal oxide films by two‐step sequential Pb2+ adsorption and reaction with methylammonium‐iodide or ‐bromide at a reasonably low concentration level of precursors. The as‐formed nanoscale perovskites are compared with their thin film counterparts. [ABSTRACT FROM AUTHOR]