Mahui

Publication date: Available online 2 November 2019

Source: Nano Energy

Author(s): Ying Yang, Tian Chen, Dequn Pan, Jing Gao, Congtan Zhu, Feiyu Lin, Conghua Zhou, Qidong Tai, Si Xiao, Yongbo Yuan, Qilin Dai, Yibo Han, Xie Haipeng, Xueyi Guo

Graphical abstract

MAPbI₃/agarose photoactive composite serves as the humid stable light absorber for unencapsultated perovskite solar cells in air. Environmental stability for almost 2000 h are achieved. ∼46% enhancement in the light-to-electric efficiency are accomplished due to the passivation of agarose on perovskite and that MAPbI₃/agarose photoactive composite has potential in improving the operational stability of perovskite solar cells in humid air without glove box.

Publication date: Available online 5 November 2019

Source: Nano Energy

Author(s): Nabonswende Aida Nadege Ouedraogo, Yichuan Chen, Yue Yue Xiao, Qi Meng, Chang Bao Han, Hui Yan, Yongzhe Zhang

Graphical abstract

Publication date: Available online 6 November 2019

Source: Nano Energy

Author(s): Ligang Xu, Mengyuan Qian, Chi Zhang, Wenzhen Lv, Jibiao Jin, Jinshi Zhang, Chao Zheng, Mingguang Li, Runfeng Chen, Wei Huang

Graphical abstract

Using fluorine‐substituted benzotriazole (BTA) as the core building block, two novel donor–accepter–donor (D–A–D) structured hole‐transporting materials, 2FBTA‐1 and 2FBTA‐2, are synthesized and applied into perovskite solar cells, achieving a high power conversion efficiency of 17.94%.

Two novel donor–accepter–donor structured hole‐transporting materials based on fluorine‐substituted benzotriazole (BTA) core building blocks (2FBTA‐1 and 2FBTA‐2) are designed and synthesized through molecular regulation. Applying these materials into perovskite solar cells, power conversion efficiencies of 7.55% and 17.94% are obtained for 2FBTA‐1 and 2FBTA‐2, respectively. The better photovoltaic performance of 2FBTA‐2 is attributed to its more suitable energy level, more planar molecular configurations, and higher hole mobility. Moreover, the devices with 2FBTA‐2 as hole transport material (HTM) show good stability in air. The results indicate that BTA is a promising building block for future HTM design.

Hole‐transport material based on dibenzo[b,d]thiophene (DBTMT) is synthesized with low costs. A champion power conversion efficiency of the optimized p–i–n planar perovskite solar cells based on dopant‐free DBTMT reaches 21.12% with a high fill factor of 83.25%, due to good hole‐transport properties and the passivation effect of DBTMT.

N ²,N ²,N ⁸,N ⁸‐tetrakis(4‐(methylthio)phenyl)dibenzo[b,d]thiophene‐2,8‐diamine (DBTMT) is synthesized from three commercial monomers for application as a promising dopant‐free hole‐transport material (HTM) in perovskite solar cells (pero‐SCs). The intrinsic properties (optical properties and electronic energy levels) of DBTMT are investigated, proving that DBTMT is a suitable HTM for the planar p–i–n pero‐SCs. The champion power conversion efficiency (PCE) of the optimized pero‐SCs (with structure as ITO/pristine DBTMT/MAPbI₃/C₆₀/BCP/Ag) reaches 21.12% with a fill factor (FF) of 83.25%, which is among the highest PCEs and FFs reported for planar p–i–n pero‐SCs based on dopant‐free HTMs. The Fourier‐transform infrared spectroscopy, X‐ray diffraction, and X‐ray photoelectron spectroscopy spectra of MAPbI₃ and DBTMT–MAPbI₃ films demonstrate that there is an interaction between DBTMT and MAPbI₃ at the interface through the sulfur atoms in DBTMT to passivate the defects, which is corresponding to the higher FF and PCE of the corresponding device.

Herein, three polyfluorene copolymers (TFB, PFB, and PFO) are investigated as hole‐transport materials (HTMs) for the construction of inverted perovskite solar cells. The photovoltaic performance of the device is found to be closely correlated with the electronic properties of HTMs. The TFB‐based device exhibits the highest efficiency of 18.48% due to its high mobility and favored energy‐level alignment.

Inverted perovskite solar cells (PSCs) that can be entirely processed at low temperatures have attracted growing attention due to their cost‐effective production. Hole‐transport materials (HTMs) play an essential role in achieving efficient inverted PSCs, as they determine the effectiveness of charge extraction and recombination at interfaces. Herein, three polyfluorene copolymers (TFB, PFB, and PFO) are investigated as HTMs for construction of inverted PSCs. It is found that the photovoltaic performance of the solar cells is closely correlated with the electronic properties of the HTMs. Due to its high mobility along with the favored energy‐level alignment with perovskite, TFB shows superior charge extraction and suppressed interfacial recombination than PFB‐ and PFO‐based devices, which delivers a high efficiency of 18.48% with an open‐circuit voltage (V _OC) of up to 1.1 V. In contrast, the presence of a large energy barrier in the PFO‐based devices results in substantial losses in both V _OC and photocurrent. These results demonstrate that TFB can serve as a superior HTM for inverted PSCs. Moreover, it is anticipated that the performance of the three HTMs identified here might guide the molecular design of novel HTMs for the manufacture of highly efficient inverted PSCs.

Gap states present a new approach to develop multi‐photon upconversion light emission in quasi‐2D perovskite films under continuous‐wave infrared excitation. Magneto‐photoluminescence (PL) and polarization‐dependent PL reveal that the gap states are essentially spatially extended states involved in orbit–orbit interaction toward generating multi‐photon excitation in quasi‐2D perovskite films.

Abstract

A new approach to generate a two‐photon up‐conversion photoluminescence (PL) by directly exciting the gap states with continuous‐wave (CW) infrared photoexcitation in solution‐processing quasi‐2D perovskite films [(PEA)₂(MA)₄Pb₅Br₁₆ with n = 5] is reported. Specifically, a visible PL peaked at 520 nm is observed with the quadratic power dependence by exciting the gap states with CW 980 nm laser excitation, indicating a two‐photon up‐conversion PL occurring in quasi‐2D perovskite films. Decreasing the gap states by reducing the n value leads to a dramatic decrease in the two‐photon up‐conversion PL signal. This confirms that the gap states are indeed responsible for generating the two‐photon up‐conversion PL in quasi‐2D perovskites. Furthermore, mechanical scratching indicates that the different‐n‐value nanoplates are essentially uniformly formed in the quasi‐2D perovskite films toward generating multi‐photon up‐conversion light emission. More importantly, the two‐photon up‐conversion PL is found to be sensitive to an external magnetic field, indicating that the gap states are essentially formed as spatially extended states ready for multi‐photon excitation. Polarization‐dependent up‐conversion PL studies reveal that the gap states experience the orbit–orbit interaction through Coulomb polarization to form spatially extended states toward developing multi‐photon up‐conversion light emission in quasi‐2D perovskites.

A new all‐inorganic perovskite material, CsPbI₃:Br:InI₃, is prepared through defect engineering of CsPbI₃. This new perovskite retains the same bandgap as CsPbI₃, but with intrinsic defect concentration largely suppressed. Moreover, it can be prepared in an extremely high humidity atmosphere. By completely eliminating the labile and expensive components in traditional perovskite solar cells (PSCs), these all‐inorganic PSCs exhibit high photovoltaic performances.

Abstract

The emergence of cesium lead iodide (CsPbI₃) perovskite solar cells (PSCs) has generated enormous interest in the photovoltaic research community. However, in general they exhibit low power conversion efficiencies (PCEs) because of the existence of defects. A new all‐inorganic perovskite material, CsPbI₃:Br:InI₃, is prepared by defect engineering of CsPbI₃. This new perovskite retains the same bandgap as CsPbI₃, while the intrinsic defect concentration is largely suppressed. Moreover, it can be prepared in an extremely high humidity atmosphere and thus a glovebox is not required. By completely eliminating the labile and expensive components in traditional PSCs, the all‐inorganic PSCs based on CsPbI₃:Br:InI₃ and carbon electrode exhibit PCE and open‐circuit voltage as high as 12.04% and 1.20 V, respectively. More importantly, they demonstrate excellent stability in air for more than two months, while those based on CsPbI₃ can survive only a few days in air. The progress reported represents a major leap for all‐inorganic PSCs and paves the way for their further exploration in order to achieve higher performance.

Ionic conduction in the perovskite oxide La_0.9Sr_0.1Ga_0.95Mg_0.05O_{3– δ} (LSGM) is found to be strongly correlated with crystal structure. A structural design with simultaneously large unit‐cell volume and octahedral rotations for fast ionic conduction is proposed and realized in LSGM superlattice thin films, where the ionic conductivity is tuned with structure alone by a factor of ≈2.5 at 600 °C.

Abstract

Solid‐oxide fuel/electrolyzer cells are limited by a dearth of electrolyte materials with low ohmic loss and an incomplete understanding of the structure–property relationships that would enable the rational design of better materials. Here, using epitaxial thin‐film growth, synchrotron radiation, impedance spectroscopy, and density‐functional theory, the impact of structural parameters (i.e., unit‐cell volume and octahedral rotations) on ionic conductivity is delineated in La_0.9Sr_0.1Ga_0.95Mg_0.05O_{3– δ} . As compared to the zero‐strain state, compressive strain reduces the unit‐cell volume while maintaining large octahedral rotations, resulting in a strong reduction of ionic conductivity, while tensile strain increases the unit‐cell volume while quenching octahedral rotations, resulting in a negligible effect on the ionic conductivity. Calculations reveal that larger unit‐cell volumes and octahedral rotations decrease migration barriers and create low‐energy migration pathways, respectively. The desired combination of large unit‐cell volume and octahedral rotations is normally contraindicated, but through the creation of superlattice structures both expanded unit‐cell volume and large octahedral rotations are experimentally realized, which result in an enhancement of the ionic conductivity. All told, the potential to tune ionic conductivity with structure alone by a factor of ≈2.5 at around 600 °C is observed, which sheds new light on the rational design of ion‐conducting perovskite electrolytes.

An ideal materials combination based on the electron donor BSFTR and acceptor Y6 is selected to construct small‐molecule solar cells (SMSCs). By morphology optimization, an extraordinary power conversion efficiency of 13.69% with a remarkably low energy loss of 0.48 eV is achieved, which is beneficial from the matched photoelectric properties, the favorable blend morphology, and is the best binary SMSC performance reported so far.

Abstract

Compared with the quick development of polymer solar cells, achieving high‐efficiency small‐molecule solar cells (SMSCs) remains highly challenging, as they are limited by the lack of matched materials and morphology control to a great extent. Herein, two small molecules, BSFTR and Y6, which possess broad as well as matched absorption and energy levels, are applied in SMSCs. Morphology optimization with sequential solvent vapor and thermal annealing makes their blend films show proper crystallinity, balanced and high mobilities, and favorable phase separation, which is conducive for exciton dissociation, charge transport, and extraction. These contribute to a remarkable power conversion efficiency up to 13.69% with an open‐circuit voltage of 0.85 V, a high short‐circuit current of 23.16 mA cm⁻² and a fill factor of 69.66%, which is the highest value among binary SMSCs ever reported. This result indicates that a combination of materials with matched photoelectric properties and subtle morphology control is the inevitable route to high‐performance SMSCs.

Via an energy‐transfer mechanism, ternary organic solar cells based on a wide‐bandgap donor (PBDB‐T‐2Cl), a middle‐bandgap acceptor (ITC‐2Cl), and an ultranarrow‐bandgap acceptor (IOIC‐2Cl) achieve a champion power conversion efficiency of 14.75% with a low energy loss of 0.48 eV, outcompeting PBDB‐T‐2Cl: ITC‐2Cl (13.66%) and PBDB‐T‐2Cl: IOIC‐2Cl (11.60%) binary devices.

An effective way to improve the power conversion efficiency of organic solar cells (OSCs) is to use the ternary architecture consisting of a donor, an acceptor, and a third component. Identifying the proper third component for successful ternary OSCs, however, is not an easy task. Herein, it is demonstrated that a middle‐bandgap acceptor, ITC‐2Cl, functions as a successful third component for several wide‐bandgap donor: ultranarrow bandgap acceptor binary systems (PBDB‐T‐2F: F8IC, PBDB‐T‐2F: IOIC‐2Cl, and PBDB‐T‐2Cl: IOIC‐2Cl). Photovoltaic parameters, including V _OC, J _SC, fill factor (FF), and power conversion efficiency (PCE), are effectively improved by incorporating ITC‐2Cl, which lies in the complementary absorption of ITC‐2Cl and host binary system, high‐lying LUMO level of ITC‐2Cl, and the inhibition of bimolecular recombination. The ternary device based on PBDB‐T‐2Cl: ITC‐2Cl: IOIC‐2Cl achieves a champion PCE of 14.75% (certified as 13.78%) with a very low energy loss of 0.48 eV. These results provide critical insight into the ternary strategy and encourage re‐evaluation and restudy of the photoactive materials previously reported with moderate performance.

A hybrid electron transport layer (ETL) of SnO₂ and carbon nanotubes (CNTs) is designed by simple thermal decomposition of a mixed solution of SnCl₄·5H₂O and pretreated CNTs. Based on the hybrid ETL, a high efficiency of 20.33% is achieved in the hysteresis‐free perovskite solar cell, which shows 13.58% enhancement compared with the conventional device (power conversion efficiency = 17.90%).

Tin oxide (SnO₂) has recently received increasing attention as an electron transport layer (ETL) in planar perovskite solar cells (PSCs) and is considered a possible alternative to titanium oxide (TiO₂). However, planar devices based on pure solution‐processed SnO₂ ETL still have hysteresis, which greatly limits the application of SnO₂ in high‐efficiency solar cells. Herein, to address this issue, a hybrid ETL of SnO₂ and carbon nanotubes (CNTs) is fabricated by a simple thermal decomposing of a mixed solution of SnCl₄·5H₂O and pretreated CNTs (termed SnO₂–CNT). The addition of CNTs can significantly improve the conductivity of SnO₂ films and reduce the trap‐state density of SnO₂ films, which benefit carrier transfer from the perovskite layer to the cathode. As a result, a high efficiency of 20.33% is achieved in the hysteresis‐free PSCs based on SnO₂–CNT ETL, which shows 13.58% enhancement compared with the conventional device (power conversion efficiency = 17.90%).

A method of combined electron transporting bilayer is reported to reduce energy loss and inhibit defects in the perovskite solar cells (PSCs) by combining the commercially accessible SnO₂ and home‐made TiO₂ nanoparticles. Consequently, the PSCs devices acquire a high efficiency of 20.50%, which is superior to that based on SnO₂ layers with a efficiency of 18.09%.

Herein, commercially accessible SnO₂ and home‐made TiO₂ nanoparticles as a combined electron transporting bilayer (ETBL) are applied to achieve highly efficient planar perovskite solar cells (PSCs). With the formed cascade‐aligned energy levels from the proper stacking of SnO₂ and TiO₂ layers and the excellent defect‐passivation ability of TiO₂, SnO₂/TiO₂ ETBLs effectively reduce energy loss and inhibit defects formation both at the electron transporting layers (ETL)/perovskite interfaces and within the bulk of perovskite layer as revealed by a comprehensive analysis of photoelectric characteristic analysis, including ultraviolet photoelectron spectroscopy, photoluminescence, and electrochemical impedance spectroscopy. Consequently, the PSC devices acquired a power conversion efficiency (PCE) of 20.50% with a V _oc of 1.10 V, a J _sc of 24.2 mA cm⁻² and an fill factor of 77%, which are superior to the values of the control device based on single SnO₂ layer with a PCE of 18.09% (a 13.3% boosting on PCE). Moreover, there was no degradation after 49 days, indicating the great stability after adding TiO₂ layer. Herein, it is demonstrated that the cascaded alignment of energy levels between the electrode and perovskite layer by ETBLs could be an effective approach to improve the photovoltaic performance of the PSCs with excellent long‐term stability.

A two‐step annealing method is developed for studying the water effect on different kinds of perovskites. It is demonstrated that 60 °C is favorable to the formation of hydrate phase which leads to a reconstruction process in the second annealing stage. The corresponding water effects highly depend on the cations of the perovskite itself.

Water effect on perovskite solar cells has received growing interest in recent years. A widely accepted view is that moderate water content induces the formation of hydrate phase which enhances the recrystallization of the perovskite. However, the underlying factors which influence the formation of hydrate phase are yet to be investigated. Herein, by controlling the annealing temperature, it is demonstrated that 60 °C is the most suitable temperature for the formation of hydrated perovskite. After further annealing at 120 °C, the resulting perovskite film reveals enhanced crystallinity with a more uniform morphology, contributing to device efficiency above 20%. In addition, the water effect on different types of perovskites is studied and it is concluded that the formation of hydrated perovskite is mainly determined by the cations of the perovskite itself. The findings in this work elucidate the conditions for the formation of hydrated perovskite, contributing to the fabrication of highly efficient perovskite solar cells.

Perovskite solar cells have reached certified efficiencies of 25.2% within just ten years due to their excellent optoelectronic properties. Nonradiative recombination at the interface between the perovskite absorber and charge‐transporting layers is identified as the major source of open‐circuit‐voltage losses in state‐of‐the‐art devices, requiring advanced strategies to study and to control efficiency‐limiting interfacial processes.

Abstract

Perovskite solar cells combine high carrier mobilities with long carrier lifetimes and high radiative efficiencies. Despite this, full devices suffer from significant nonradiative recombination losses, limiting their V _OC to values well below the Shockley–Queisser limit. Here, recent advances in understanding nonradiative recombination in perovskite solar cells from picoseconds to steady state are presented, with an emphasis on the interfaces between the perovskite absorber and the charge transport layers. Quantification of the quasi‐Fermi level splitting in perovskite films with and without attached transport layers allows to identify the origin of nonradiative recombination, and to explain the V _OC of operational devices. These measurements prove that in state‐of‐the‐art solar cells, nonradiative recombination at the interfaces between the perovskite and the transport layers is more important than processes in the bulk or at grain boundaries. Optical pump‐probe techniques give complementary access to the interfacial recombination pathways and provide quantitative information on transfer rates and recombination velocities. Promising optimization strategies are also highlighted, in particular in view of the role of energy level alignment and the importance of surface passivation. Recent record perovskite solar cells with low nonradiative losses are presented where interfacial recombination is effectively overcome—paving the way to the thermodynamic efficiency limit.

The power conversion efficiency of inorganic perovskite solar cells (PSCs) is still low compared with hybrid PSCs. The use of lithium fluoride on SnO₂ and PbCl₂ additive in perovskite is reported for reducing the charge recombination; 18.64% efficiency of CsPbI_3–x Br _x solar cells is demonstrated; and the devices show over than 1000 h light soaking stability.

Abstract

Cesium‐based inorganic perovskite solar cells (PSCs) are promising due to their potential for improving device stability. However, the power conversion efficiency of the inorganic PSCs is still low compared with the hybrid PSCs due to the large open‐circuit voltage (V _OC) loss possibly caused by charge recombination. The use of an insulated shunt‐blocking layer lithium fluoride on electron transport layer SnO₂ for better energy level alignment with the conduction band minimum of the CsPbI_{3‐ x} Br _x and also for interface defect passivation is reported. In addition, by incorporating lead chloride in CsPbI_{3‐ x} Br _x precursor, the perovskite film crystallinity is significantly enhanced and the charge recombination in perovksite is suppressed. As a result, optimized CsPbI_{3‐ x} Br _x PSCs with a band gap of 1.77 eV exhibit excellent performance with the best V _OC as high as 1.25 V and an efficiency of 18.64%. Meanwhile, a high photostability with a less than 6% efficiency drop is achieved for CsPbI_{3‐ x} Br _x PSCs under continuous 1 sun equivalent illumination over 1000 h.

Stability and toxicity are bottlenecks for halide perovskite solar cells despite their remarkable efficiency. Double halide perovskites with heterovalent metal cations pave a way for lead‐free‐based devices for enhanced stability. This Review summarizes the theoretical and experimental progress of lead‐free double perovskite. The issues, challenges, applications, and future prospects are integrated to provide a full picture.

Perovskite solar cells (PSCs) have achieved a high power conversion efficiency (PCE) with a credible certified value over 25%. More efforts have been devoted to the development of stable and ecofriendly perovskite materials. Lead‐free double perovskites (LFDPs) are a noteworthy choice as a photoactive layer because of their favorable photovoltaic (PV) properties, intrinsic chemical stability, and environmental friendliness. This Review presents various LFDP materials whose structural stability and optoelectronic properties are predicted by theoretical calculations. The synthesis and experimental properties of LFDPs and their applications in PSCs and optoelectronics in pursuing high performance, low toxicity, and functional stability are also reviewed. Perovskites active layers are critical for PSCs, and their appropriate properties are responsible for achieving a high PCE. On the other side, the stability of PSCs under working conditions is a critical requirement for their practical applications. Defect‐ordered perovskites are also presented to provide another outlook on lead‐free perovskite‐based PVs. The introduction and interest toward LFDP in PSCs can represent a viable solution to the toxicity issue, stimulate further research, and bring a real impact to future PV technologies.

A novel method is developed for fabricating high‐quality Ruddlesden–Popper perovskite films by directly using commercially available organic amines, avoiding extra chemical synthesis processing of organic ammonium halides. This new approach results in similar (and even better) device performance for both solar cells and light‐emitting diodes when compared with control devices fabricated from organic ammonium halides.

Abstract

Ruddlesden–Popper perovskites (RPPs), consisting of alternating organic spacer layers and inorganic layers, have emerged as a promising alternative to 3D perovskites for both photovoltaic and light‐emitting applications. The organic spacer layers provide a wide range of new possibilities to tune the properties and even provide new functionalities for RPPs. However, the preparation of state‐of‐the‐art RPPs requires organic ammonium halides as the starting materials, which need to be ex situ synthesized. A novel approach to prepare high‐quality RPP films through in situ formation of organic spacer cations from amines is presented. Compared with control devices fabricated from organic ammonium halides, this new approach results in similar (and even better) device performance for both solar cells and light‐emitting diodes. High‐quality RPP films are fabricated based on different types of amines, demonstrating the universality of the approach. This approach not only represents a new pathway to fabricate efficient devices based on RPPs, but also provides an effective method to screen new organic spacers with further improved performance.

The spintronic properties of different hybrid organic–inorganic perovskites (HOIPs) are studied in spin valve devices, including spin diffusion length and spin lifetime, as well as the impact of the chemical components on these properties. This study aims at demonstrating promising spintronic applications of HOIPs, and providing a clear path for engineering spintronic devices based on HOIPs.

Abstract

The hybrid organic–inorganic perovskites (HOIPs) form a new class of semiconductors which show promising optoelectronic device applications. Remarkably, the optoelectronic properties of HOIP are tunable by changing the chemical components of their building blocks. Recently, the HOIP spintronic properties and their applications in spintronic devices have attracted substantial interest. Here the impact of the chemical component diversity in HOIPs on their spintronic properties is studied. Spin valve devices based on HOIPs with different organic cations and halogen atoms are fabricated. The spin diffusion length is obtained in the various HOIPs by measuring the giant magnetoresistance (GMR) response in spin valve devices with different perovskite interlayer thicknesses. In addition spin lifetime is also measured from the Hanle response. It is found that the spintronic properties of HOIPs are mainly determined by the halogen atoms, rather than the organic cations. The study provides a clear avenue for engineering spintronic devices based on HOIPs.

A high power conversion efficiency of 11.76%, the best efficiency for all‐polymer solar cells, is achieved by printing fabrication based on PTzBI‐Si:N2200 processing with 2‐methyltetrahydrofuran. A Multi‐length‐scaled morphology is found in the bulk heterojunctions, which ensures fast transfer of carriers and facilitates exciton separation, and boosts carrier mobility and current density, thus improving the device performance.

Abstract

All‐polymer solar cells (all‐PSCs) exhibit excellent stability and readily tunable ink viscosity, and are therefore especially suitable for printing preparation of large‐scale devices. At present, the efficiency of state‐of‐the‐art all‐PSCs fabricated by the spin‐coating method has exceeded 11%, laying the foundation for the preparation and practical utilization of printed devices. A high power conversion efficiency (PCE) of 11.76% is achieved based on PTzBI‐Si:N2200 all‐PSCs processing with 2‐methyltetrahydrofuran (MTHF, an environmentally friendly solvent) and preparation of active layers by slot die printing, which is the top efficient for all‐PSCs. Conversely, the PCE of devices processed by high‐boiling point chlorobenzene is less than 2%. Through the study of film formation kinetics, volatile solvents can freeze the morphology in a short time, and a more rigid conformation with strong intermolecular interaction combined with the solubility limit of PTzBI‐Si and N2200 in MTHF results in the formation of a fibril network in the bulk heterojunction. The multilength scaled morphology ensures fast transfer of carriers and facilitates exciton separation, which boosts carrier mobility and current density, thus improving the device performance. These results are of great significance for large‐scale printing fabrication of high‐efficiency all‐PSCs in the future.

The variation of A‐site cations is promising to achieve enhanced properties; however, it is limited to a few available choices of methylamine, formamidine, and cesium. Halogenated methylammoniums are reported as novel A cations to broaden the family of hybrid perovskites, which breaks through the limitation of A cations.

Abstract

3D perovskites with typical structure of ABX₃ are emerging as key materials to achieve high‐performance optoelectronic devices. The variation of A‐site cation is promising to achieve enhanced properties; however, is limited to a few available choices of methylamine, formamidine, and cesium. In this work, halogenated‐methylammoniums are developed as A cation to broaden the family of hybrid perovskites. Single crystals and colloidal nanocrystals of halogenated‐methylammoniums based perovskites are successfully synthesized, showing bright future as alternatives for device exploration. In particular, the improved thermal stability and low exciton binding energy from single crystals measurements are demonstrated and bright tunable emission from blue to green for colloidal nanocrystals is achieved.

Application of the proposed slow post‐annealing for layered 2D perovskite solar cells based on BA₂MA₃Pb₄I₁₃ photo‐absorber leads to a favorable alignment on the multi‐perovskite phases and resultant champion power conversion efficiency to 17.26%, showing simultaneously enhanced open‐circuit voltage and short‐circuit current.

Abstract

Layered Ruddlesden–Popper (RP) phase (2D) halide perovskites have attracted tremendous attention due to the wide tunability on their optoelectronic properties and excellent robustness in photovoltaic devices. However, charge extraction/transport and ultimate power conversion efficiency (PCE) in 2D perovskite solar cells (PSCs) are still limited by the non‐eliminable quantum well effect. Here, a slow post‐annealing (SPA) process is proposed for BA₂MA₃Pb₄I₁₃ (n = 4) 2D PSCs by which a champion PCE of 17.26% is achieved with simultaneously enhanced open‐circuit voltage, short‐circuit current, and fill factor. Investigation with optical spectroscopy coupled with structural analyses indicates that enhanced crystal orientation and favorable alignment on the multiple perovskite phases (from the 2D phase near bottom to quasi‐3D phase near top regions) is obtained with SPA treatment, which promotes carrier transport/extraction and suppresses Shockley–Read–Hall charge recombination in the solar cell. As far as it is known, the reported PCE is so far the highest efficiency in RP phase 2D PSCs based on butylamine (BA) spacers (n = 4). The SPA‐processed devices exhibit a satisfactory stability with <4.5% degradation after 2000 h under N₂ environment without encapsulation. The demonstrated process strategy offers a promising route to push forward the performance in 2D PSCs toward realistic photovoltaic applications.

Organic photovoltaic (OPV) cells promise to have a good photovoltaic performance under the indoor light environment. Via optimizing the active layers, 1 cm² OPV cells are fabricated and a top power conversion efficiency of 22% under 1000 lux illumination is demonstrated.

Abstract

Organic photovoltaic (OPV) technologies have the advantages of fabricating larger‐area and light‐weight solar panels on flexible substrates by low‐cost roll‐to‐toll production. Recently, OPV cells have achieved many significant advances with power conversion efficiency (PCE) increasing rapidly. However, large‐scale solar farms using OPV modules still face great challenges, such as device stability. Herein, the applications of OPV cells in indoor light environments are studied. Via optimizing the active layers to have a good match with the indoor light source, 1 cm² OPV cells are fabricated and a top PCE of 22% under 1000 lux light‐emitting diode (2700 K) illumination is demonstrated. In this work, the light intensities are measured carefully. Incorporated with the external quantum efficiency and photon flux spectrum, the integral current densities of the cells are calculated to confirm the reliability of the photovoltaic measurement. In addition, the devices show much better stability under continuous indoor light illumination. The results suggest that designing wide‐bandgap active materials to meet the requirements for the indoor OPV cells has a great potential in achieving higher photovoltaic performance.

The changes in photophysical properties of mixed‐halide perovskite films under solar‐equivalent illumination are studied. The illumination generates localized low‐bandgap surface domains, onto which photoexcited charge carriers transfer and recombine with high radiative efficiency. The fraction of radiative and nonradiative (Auger) recombination bandgap can be balanced to achieve extremely high photoluminescence quantum yields at low excitation densities.

Abstract

Mixed‐halide lead perovskites have attracted significant attention in the field of photovoltaics and other optoelectronic applications due to their promising bandgap tunability and device performance. Here, the changes in photoluminescence and photoconductance of solution‐processed triple‐cation mixed‐halide (Cs_0.06MA_0.15FA_0.79)Pb(Br_0.4I_0.6)₃ perovskite films (MA: methylammonium, FA: formamidinium) are studied under solar‐equivalent illumination. It is found that the illumination leads to localized surface sites of iodide‐rich perovskite intermixed with passivating PbI₂ material. Time‐ and spectrally resolved photoluminescence measurements reveal that photoexcited charges efficiently transfer to the passivated iodide‐rich perovskite surface layer, leading to high local carrier densities on these sites. The carriers on this surface layer therefore recombine with a high radiative efficiency, with the photoluminescence quantum efficiency of the film under solar excitation densities increasing from 3% to over 45%. At higher excitation densities, nonradiative Auger recombination starts to dominate due to the extremely high concentration of charges on the surface layer. This work reveals new insight into phase segregation of mixed‐halide mixed‐cation perovskites, as well as routes to highly luminescent films by controlling charge density and transfer in novel device structures.

The OH…I⁻ hydrogen bonding interactions between poly(vinyl alcohol) (PVA) and FASnI₃ have the effects of introducing nucleation sites, slowing down crystal growth, directing the crystal orientation, reducing the trap states, and suppressing the migration of the ions. By adding PVA, the FASnI₃–PVA perovskite solar cells attain improved power conversion efficiency and stability.

Abstract

Tin‐based perovskites with narrow bandgaps and high charge‐carrier mobilities are promising candidates for the preparation of efficient lead‐free perovskite solar cells (PSCs). However, the crystalline rate of tin‐based perovskites is much faster, leading to abundant trap states and much lower open‐circuit voltage (V _oc). Here, hydrogen bonding is introduced to retard the crystalline rate of the FASnI₃ perovskite. By adding poly(vinyl alcohol) (PVA), the OH…I⁻ hydrogen bonding interactions between PVA and FASnI₃ have the effects of introducing nucleation sites, slowing down the crystal growth, directing the crystal orientation, reducing the trap states, and suppressing the migration of the iodide ions. In the presence of the PVA additive, the FASnI₃–PVA PSCs attain higher power conversion efficiency of 8.9% under a reverse scan with significantly improved V _oc from 0.55 to 0.63 V, which is one of the highest V _oc values for FASnI₃‐based PSCs. More importantly, the FASnI₃–PVA PSCs exhibit striking long‐term stability, with no decay in efficiency after 400 h of operation at the maximum power point. This approach, which makes use of the OH…I⁻ hydrogen bonding interactions between PVA and FASnI₃, is generally applicable for improving the efficiency and stability of the FASnI₃‐based PSCs.

A novel red thermally activated delayed fluorescence (TADF) emitter, TPA–PZCN, is designed and synthesized. It simultaneously possesses a high Φ _PL of 97% and a small ΔE _ST of 0.13 eV. Red, deep‐red, and near‐infrared organic light‐emitting diodes (LEDs) based on it achieve record external quantum efficiencies of 27.4%, 28.1%, and 5.3%, respectively, which are the best performances in comparison with LEDs having a similar device structure.

Abstract

Researchers have spared no effort to design new thermally activated delayed fluorescence (TADF) emitters for high‐efficiency organic light‐emitting diodes (OLEDs). However, efficient long‐wavelength TADF emitters are rarely reported. Herein, a red TADF emitter, TPA–PZCN, is reported, which possesses a high photoluminescence quantum yield (Φ _PL) of 97% and a small singlet–triplet splitting (ΔE _ST) of 0.13 eV. Based on the superior properties of TPA–PZCN, red, deep‐red, and near‐infrared (NIR) OLEDs are fabricated by utilizing different device structure strategies. The red devices obtain a remarkable maximum external quantum efficiency (EQE) of 27.4% and an electroluminescence (EL) peak at 628 nm with Commission Internationale de L'Eclairage (CIE) coordinates of (0.65, 0.35), which represents the best result with a peak wavelength longer than 600 nm among those of the reported red TADF devices. Furthermore, an exciplex‐forming cohost strategy is adopted. The devices achieve a record EQE of 28.1% and a deep‐red EL peak at 648 nm with the CIE coordinates of (0.66, 0.34). Last, nondoped devices exhibit 5.3% EQE and an NIR EL peak at 680 nm with the CIE coordinates of (0.69, 0.30).

A cosensitization strategy with use of dual heavy‐metal‐free NIR absorption Zn–Cu–In–Se and Zn–Cu–In–S quantum dots (QDs) as cosensitizers is applied to control the light‐absorption, electron‐injection, and charge‐recombination processes simultaneously in QD‐sensitized solar cells (QDSCs). An average power conversion efficiency of 13.18% and a new certified efficiency record of 12.98% are obtained for environmentally friendly QDSCs under AM 1.5G 1 sun irradiation.

Abstract

Generally, high light‐harvesting efficiency, electron‐injection efficiency, and charge‐collection efficiency are the prerequisites for high‐efficiency quantum‐dot‐sensitized solar cells (QDSCs). However, it is fairly difficult for a single QD sensitizer to meet these three requirements simultaneously. It is demonstrated that these parameters can be felicitously balanced by a cosensitization strategy through the adoption of environmental‐friendly Zn–Cu–In–Se and Zn–Cu–In–S dual QD sensitizers with cascade energy structure. Experimental results indicate that: i) the combination of the dual QDs can improve the light‐harvesting capability of the cells, especially in the visible light window; ii) the cosensitization approach can facilitate electron injection, benefitting from the cascade energy structure of the two QD sensitizers employed; iii) the charge‐collection efficiency can be remarkably enhanced by the suppressed charge‐recombination process due to the improved QD coverage on TiO₂. Consequently, this cosensitization strategy delivers a new certified efficiency record of 12.98% for liquid‐junction QDSCs under AM 1.5G 1 sun irradiation. Moreover, the constructed cells exhibit good stability in a high‐humidity environment.