Search

The perovskite/silicon tandem solar cell represents one of the most promising avenues for exceeding the Shockley-Queisser limit for single-junction solar cells at a reasonable cost. Remarkably, its efficiency has rapidly increased from 13.7% in 2015 to 34.6% in 2024. Despite the significant research efforts dedicated to this topic, the "secret" to achieving high-performance perovskite/silicon tandem solar cells seems to be confined to a few research groups. Additionally, the discrepancies in preparation and characterization between single-junction and tandem solar cells continue to impede the transition from efficient single-junction to efficient tandem solar cells. This review first revisits the key milestones in the development of monolithic perovskite/silicon tandem solar cells over the past decade. Then, a comprehensive analysis of the background, advancements, and challenges in perovskite/silicon tandem solar cells is provided, following the sequence of the tandem fabrication process. The progress and limitations of the prevalent stability measurements for tandem devices are also discussed. Finally, a roadmap for designing efficient, scalable, and stable perovskite/silicon tandem solar cells is outlined. This review takes the growth history into consideration while charting the future course of perovskite/silicon tandem research., (© 2024 Wiley‐VCH GmbH.)

Tunnel oxide passivating contact (TOPCon) solar cells (SCs) as one of the most competitive crystalline silicon (c-Si) technologies for the TW-scaled photovoltaic (PV) market require higher passivation performance to further improve their device efficiencies. Here, the successful construction of a double-layered polycrystalline silicon (poly-Si) TOPCon structure is reported using an in situ nitrogen (N)-doped poly-Si covered by a normal poly-Si, which achieves excellent passivation and contact properties simultaneously. The new design exhibits the highest implied open-circuit voltage of 755 mV and the lowest single-sided recombination current density (J 0 ) of ≈0.7 fA cm⁻ 2 for a TOPCon structure and a low contact resistivity of less than 5 mΩ·cm 2 , resulting in a high selectivity factor of ≈16. The mechanisms of passivation improvement are disclosed, which suggest that the introduction of N atoms into poly-Si restrains H overflow by forming stronger Si-N and N-H bonds, reduces interfacial defects, and induces favorable energy bending. Proof-of-concept TOPCon SCs with such a design receive a remarkable certified efficiency of 25.53%., (© 2023 Wiley-VCH GmbH.)

Metal halide perovskite solar cells (PSCs) have emerged as one of the most promising candidates for next-generation photovoltaic technologies. However, perovskite films deposited by blade-coating usually exhibit inferior film morphology compared to those fabricated by spin-coating, which hinders the power conversion efficiency (PCE) and stability of the scalable perovskite solar modules (PSMs). Herein, ellipsoidal colloids are tailored in the perovskite precursor solution by incorporating perovskite colloids and polymer additives. Compared to unregulated spherical colloids, the ellipsoidal colloids demonstrate more oriented packing during the blade-coating process, which is due to the anisotropic driven force from the fluidic flow in the meniscus. As a result of the improved film morphology, the regulated PSCs and PSMs achieve superior PCE of 24.31% and 21.67% (21.37% certified), respectively, for aperture areas of 0.09 and 13.94 cm 2 , and 89% initial PCE after 600 h continuous operation., (© 2025 Wiley‐VCH GmbH.)

Over the past decade, semiconducting halide perovskite lasers have emerged as a transformative platform in optoelectronics, owing to unique properties such as high photoluminescence quantum yields, tunable bandgaps, and low-cost fabrication processes. This review systematically examines the advancements in halide perovskite lasers, covering diverse laser architectures, such as whispering gallery mode, Fabry-Pérot, plasmonic, bound states in the continuum (BIC), quantum dot, and polariton lasers. The mechanisms of optical gain, the role of material engineering in optimizing lasing performance, and the challenges associated with continuous-wave (CW) pumping and electrically driven lasing are discussed. Furthermore, recent progress in improving the stability and scalability of perovskite lasers, essential for their integration into practical applications in displays, optical communications, sensing, and integrated photonics is highlighted. Finally, future research directions are discussed, emphasizing the potential of perovskite lasers to revolutionize various technological domains by enabling the development of next-generation photonic devices., (© 2025 Wiley‐VCH GmbH.)

Tin-based halide perovskites (ASnX 3 ) have garnered substantial interest due to their unique photoelectric properties and environmentally friendly features. The A-site ions tuning strategy has been proven to promote material performance. However, there is a lack of systematic research on the optical properties, lattice structure variation, and band structure evolution in tin-based perovskites when the A-site ions tune from organic to inorganic. Herein, MA 1-x Cs x SnBr 3 and MA 1-x Cs x SnI 3 (0≤x≤1) flakes are synthesized through a one-pot reaction method. By controlling the Cs ratio, a tunable photoluminescence (PL) emission covering a wide range of 560-685 nm can be observed in MA 1-x Cs x SnBr 3 , with bandgap tuned from 1.8 to 2.15 eV, while the PL ranges from 900 to 950 nm with the bandgap 1.2-1.3 eV for MA 1-x Cs x SnI 3 . Besides, the PL intensity of MA 1-x Cs x SnBr 3 significantly enhances with the increasing Cs ratio. First-principles calculations reveal that the octahedron shrinks gradually as the Cs ratio increases. It increases the orbital overlap between Sn and Br and causes a symmetry variation, thus decreasing the bandgap and increasing emission intensity. This work reveals the photophysical mechanism of improved optical properties and bandgap variation in tin-based perovskites, paving the way for their future applications., (© 2025 Wiley‐VCH GmbH.)

The development of efficient electron-collecting monolayer materials is desired to lower manufacturing costs and improve the performance of regular (negative-intrinsic-positive, n-i-p) type perovskite solar cells (PSCs). Here, we designed and synthesized four electron-collecting monolayer materials based on thiazolidinone skeletons, with different lowest-unoccupied molecular orbital (LUMO) levels (rhodanine or thiazolidinedione) and different anchoring groups to the transparent electrode (phosphonic acid or carboxylic acid). These molecules, when adsorbed on indium tin oxide (ITO) substrates, lower the work function of ITO, decreasing the energy barrier for electron extraction at the ITO/perovskite interface and improving the device performance. The shift of work function, rather than the LUMO levels of the molecules themselves, was found to be correlated with the performance of the perovskite solar cells., (© 2025 Wiley-VCH GmbH.)

Hole-transport layers (HTL) in perovskite solar cells (PSCs) with an n-i-p structure are commonly doped by bis(trifluoromethane)sulfonimide (TFSI) salts to enhance hole conduction. While lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) dopant is a widely used and effective dopant, it has significant limitations, including the need for additional solvents and additives, environmental sensitivity, unintended oxidation, and dopant migration, which can lead to lower stability of PSCs. A novel ionic liquid, 1-(2-methoxyethyl)-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)amide (MMPyTFSI), is explored as an alternative dopant for 2,2',7,7'-tetrakis(N,N-di-p-methoxyphenylamino)-9,9'-spirobifluorene (spiro-OMeTAD). MMPy ions act as a surface passivator, reducing defects on the perovskite surface, while TFSI ions facilitate p-type doping. MMPyTFSI functions as an efficient dopant, maintaining excellent performance even when tetrahydrofuran (THF) is utilized as a solvent in place of chlorobenzene (CB), while significantly reducing the environmental impact of the process. The optimized PSC achieves a power conversion efficiency (PCE) of 23.10% and demonstrates enhanced long-term stability in all aging tests for over 1000 h in a humid atmosphere, at high temperature, and under simulated sunlight illumination. These results demonstrate that MMPyTFSI is an effective and environmentally friendly dopant for producing stable and efficient PSCs., (© 2025 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Halide-perovskite semiconductors have a high potential for use in single-junction and tandem solar cells. Despite their unprecedented rise in power conversion efficiencies (PCEs) for photovoltaic (PV) applications, it remains unclear whether perovskite solar modules can reach a sufficient operational lifetime. In order to make perovskite solar cells (PSCs) commercially viable, a fundamental understanding of the relationship between their nanostructure, optoelectronic properties, device efficiency, and long-term operational stability/reliability needs to be established. In this review, the phase instabilities in state-of-the-art formamidinium (FA)-rich perovskite absorbers is discussed. Furhermore, the concerted efforts are summarized in this prospect, covering aspects from fundamental research to device engineering. Subsequently, a critical analysis of the dictating impact of the nanoscale landscape of perovskite materials on their resulting intrinsic stability is provided '. Finally, the remaining challenges in the field are assessed and future research directions are proposed for improving the operational lifetimes of perovskite devices. It is believed that these approaches, which bridge nanoscale structural properties to working solar cell devices, will be critical to assessing the realization of a bankable PSC product., (© 2024 Wiley‐VCH GmbH.)

Developing high-quality wide bandgap (WBG) perovskites with ≈1.7 eV bandgap (E g ) is critical to couple with silicon and create efficient silicon/perovskite tandem devices. The sufferings of large open-circuit voltage (V OC ) loss and unstable power output under operation continuously highlight the criticality to fully develop high-quality WBG perovskite films. In this study, rubidium and thiocyanate as additive regulators in WBG perovskites are incorporated, significantly reducing non-radiative recombination, ion-migration, and phase segregation. The optimized 1.66 eV E g perovskite solar cells achieved state-of-art 1.3 V V OC (0.36 V deficit), and delivered a stabilized power conversion efficiency of 24.3%, along with good device stability (20% degradation (T 80 ) after over 994 h of operation under 1 sun at ≈65°C). When integrated with a flat front side silicon cell, silicon/perovskite two-terminal tandem device (30% efficient) is obtained with a 1.97 V V OC , and T 90 operational lifetime of more than 600 h at room temperature., (© 2024 Wiley‐VCH GmbH.)

The rapid emergence of organic-inorganic lead halide perovskites for low-cost and high-efficiency photovoltaics promises to impact new photovoltaic concepts. Their high power conversion efficiencies, ability to coat perovskite layers on glass via various scalable deposition techniques, excellent optoelectronic properties, and synthetic versatility for modulating transparency and color allow perovskite solar cells (PSCs) to be an ideal solution for building-integrated photovoltaics (BIPVs), which transforms windows or façades into electric power generators. In this review, the unique features and properties of PSCs for BIPV application are accessed. Device engineering and optical management strategies of active layers, interlayers, and electrodes for semitransparent, bifacial, and colorful PSCs are also discussed. The performance of PSCs under conditions that are relevant for BIPV such as different operational temperature, light intensity, and light incident angle are also reviewed. Recent outdoor stability testing of PSCs in different countries and other demonstration of scalability and deployment of PSCs are also spotlighted. Finally, the current challenges and future opportunities for realizing perovskite-based BIPV are discussed., (© 2022 Wiley-VCH GmbH.)

Modifying perovskites with functional additives has proven effective in refining the crystallization process and passivating the defects of perovskite films, thereby ensuring high photovoltaic efficiencies. However, conventional methods that involve pre-mixing additives into the precursor solution often face challenges due to discrepancies in the spatial distribution of slow-diffused additives relative to dynamically formed defect sites, resulting in limited passivation effectiveness. To address this issue, this study innovatively proposes a dynamic passivation strategy that utilizes a pre-passivator to gradually release active additives during the thermal crystallization process of perovskite films. By leveraging the principle of energy minimization, these timely-released additives can interact precisely and selectively with the high-energy defect sites generated during crystallization, thus facilitating efficient additive utilization and in situ real-time defect passivation. Through analysis of crystallization kinetics and carrier dynamic, it is demonstrated that this dynamic passivation approach significantly improves film quality and prolongs carrier lifetime, outperforming traditional pre-mixing tactics. Consequently, the final perovskite solar cell achieves an impressive solar conversion efficiency of 25.33 %, along with exceptional stability. This work provides strong support of tailored additive strategies aimed at further enhancing the efficiency of perovskite solar cells and their subsequent commercial applications., (© 2024 Wiley-VCH GmbH.)

Perovskite solar cells (PSCs) have attracted widespread research and commercialization attention because of their high power conversion efficiency (PCE) and low fabrication cost. The long-term stability of PSCs should satisfy industrial requirements for photovoltaic devices. Inverted PSCs with a p-i-n architecture exhibit considerable advantages because of their excellent stability and competitive efficiency. The continuously broken-through PCE of inverted PSCs shows huge application potential. This review summarizes the developments and outlines the characteristics of inverted PSCs including charge transport layers (CTLs), perovskite compositions, and interfacial regulation strategies. The latest effective CTLs, interfacial modification, and stability promotion strategies especially under light, thermal, and bias conditions are emphatically analyzed. Furthermore, the applications of the inverted structure in high-efficiency and stable tandem, flexible photovoltaic devices, and modules and their main obstacles are systematically introduced. Finally, the remaining challenges faced by inverted devices are discussed, and several directions for advancing inverted PSCs are proposed according to their development status and industrialization requirements., (© 2024 Wiley‐VCH GmbH.)

The organic-inorganic lead halide per materials have emerged as highly promising contenders in the field of photovoltaic technology, offering exceptional efficiency and cost-effectiveness. The commercialization of perovskite photovoltaics hinges on successfully transitioning from lab-scale perovskite solar cells to large-scale perovskite solar modules (PSMs). However, the efficiency of PSMs significantly diminishes with increasing device area, impeding commercial viability. Central to achieving high-efficiency PSMs is fabricating uniform functional films and optimizing interfaces to minimize energy loss. This review sheds light on the path toward large-scale PSMs, emphasizing the pivotal role of integrating cutting-edge scientific research with industrial technology. By exploring scalable deposition techniques and optimization strategies, the advancements and challenges in fabricating large-area perovskite films are revealed. Subsequently, the architecture and contact materials of PSMs are delved while addressing pertinent interface issues. Crucially, efficiency loss during scale-up and stability risks encountered by PSMs is analyzed. Furthermore, the advancements in industrial efforts toward perovskite commercialization are highlighted, emphasizing the perspective of PSMs in revolutionizing renewable energy. By highlighting the scientific and technical challenges in developing PSMs, the importance of combining science and industry to drive their industrialization and pave the way for future advancements is stressed., (© 2024 Wiley‐VCH GmbH.)

The integration of optoelectronic devices, such as transistors and photodetectors (PDs), into wearables and textiles is of great interest for applications such as healthcare and physiological monitoring. These require flexible/wearable systems adaptable to body motions, thus materials conformable to non-planar surfaces, and able to maintain performance under mechanical distortions. Here, fibre PDs are prepared by combining rolled graphene layers and photoactive perovskites. Conductive fibres (~500 Ωcm -1 ) are made by rolling single-layer graphene (SLG) around silica fibres, followed by deposition of a dielectric layer (Al 2 O 3 and parylene C), another rolled SLG as a channel, and perovskite as photoactive component. The resulting gate-tunable PD has a response time~9ms, with an external responsivity~22kAW -1 at 488nm for a 1V bias. The external responsivity is two orders of magnitude higher, and the response time one order of magnitude faster, than state-of-the-art wearable fibre-based PDs. Under bending at 4mm radius, up to~80% photocurrent is maintained. Washability tests show~72% of initial photocurrent after 30 cycles, promising for wearable applications., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Two-terminal (2T) perovskite-based tandem solar cells (TSCs) arouse burgeoning interest in breaking the Shockley-Queisser (S-Q) limit of single-junction solar cells by combining two subcells with different bandgaps. However, the highest certified efficiency of 2T perovskite-based TSCs (33.9%) lags behind the theoretical limit (42-43%). A vital challenge limiting the development of 2T perovskite-based TSCs is the transparent recombination layers/interconnecting layers (RLs) design between two subcells. To improve the performance of 2T perovskite-based TSCs, RLs simultaneously fulfill the optical loss, contact resistance, carrier mobility, stress management, and conformal coverage requirements. In this review, the definition, functions, and requirements of RLs in 2T perovskite-based TSCs are presented. The insightful characterization methods applicable to RLs, which are inspiring for further research on the RLs both in 2T perovskite-based two-junction and multi-junction TSCs, are also highlighted. Finally, the key factors that currently limit the performance enhancement of RLs and the future directions that should be continuously focused on are summarized., (© 2024 Wiley‐VCH GmbH.)

The demand for accurate perception of the physical world leads to a dramatic increase in sensory nodes. However, the transmission of massive and unstructured sensory data from sensors to computing units poses great challenges in terms of power-efficiency, transmission bandwidth, data storage, time latency, and security. To efficiently process massive sensory data, it is crucial to achieve data compression and structuring at the sensory terminals. In-sensor computing integrates perception, memory, and processing functions within sensors, enabling sensory terminals to perform data compression and data structuring. Here, vision sensors are adopted as an example and discuss the functions of electronic, optical, and optoelectronic hardware for visual processing. Particularly, hardware implementations of optoelectronic devices for in-sensor visual processing that can compress and structure multidimensional vision information are examined. The underlying resistive switching mechanisms of volatile/nonvolatile optoelectronic devices and their processing operations are explored. Finally, a perspective on the future development of optoelectronic devices for in-sensor computing is provided., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Efficient and robust n-i-p perovskite solar cells necessitate superior organic hole-transport materials with both mechanical and electronic prowess. Deciphering the structure-property relationship of these materials is crucial for practical perovskite solar cell applications. Through direct arylation, two high glass transition temperature molecular semiconductors, DBC-ETPA (202 °C) and TPE-ETPA (180 °C) are synthesized, using dibenzo[g,p]chrysene (DBC) and 1,1,2,2-tetraphenylethene (TPE) tetrabromides with triphenylene-ethylenedioxythiophene-dimethoxytriphenylamine (ETPA). In comparison to spiro-OMeTAD, both semiconductors exhibit shallower HOMO energy levels, resulting in increased hole densities (generated by air oxidation doping) and accelerated hole extraction from photoexcited perovskite. Experimental and theoretical studies highlight the more rigid DBC core, enhancing hole mobility due to reduced reorganization energy and lower energy disorder. Importantly, DBC-ETPA possesses a higher cohesive energy density, leading to lower ion diffusion coefficients and higher Young's moduli. Leveraging these attributes, DBC-ETPA is employed as the primary hole-transport layer component, yielding perovskite solar cells with an average efficiency of 24.5%, surpassing spiro-OMeTAD reference cells (24.0%). Furthermore, DBC-ETPA-based cells exhibit superior operational stability and 85 °C thermal storage stability., (© 2024 Wiley‐VCH GmbH.)

Challenges such as shuttle effect have hindered the commercialization of lithium-sulfur batteries (LSBs), despite their potential as high-energy-density storage devices. To address these issues, we explore the integration of solar energy into LSBs, creating a photo-assisted lithium-sulfur battery (PA-LSB). The PA-LSB provides a novel and sustainable solution by coupling the photocatalytic effect to accelerate sulfur redox reactions. Herein, a perovskite quantum dot-loaded MOF material serves as a cathode for the PA-LSB, creating built-in electric fields at the micro-interface to extend the lifetime of photo-generated charge carriers. The band structure of the composite material aligns well with the electrochemical reaction potential of lithium-sulfur, enabling precise regulation of polysulfides in the cathode of the PA-LSB system. This is attributed to the selective catalysis of the liquid-solid reaction stage in the lithium-sulfur electrochemical process by photocatalysis. These contribute to the outstanding performance of PA-LSBs, particularly demonstrating a remarkably high reversible capacity of 679 mAh g -1 at 5 C, maintaining stable cycling for 1500 cycles with the capacity decay rate of 0.022 % per cycle. Additionally, the photo-charging capability of the PA-LSB holds the potential to compensate for non-electric energy losses during the energy storage process, contributing to the development of lossless energy storage devices., (© 2024 Wiley-VCH GmbH.)

Carrier-selective passivating contacts using transition metal oxides (TMOs) have attracted great attention for crystalline silicon (c-Si) heterojunction solar cells recently. Among them, tantalum oxide (Ta 2 O 5 ) exhibits outstanding advantages, such as a wide bandgap, good surface passivation, and a small conduction band offset with c-Si, which is typically used as an electron-selective contact layer. Interestingly, it is first demonstrated that solution-processed Ta 2 O 5 films exhibit a high hole selectivity, which blocks electrons and promotes hole transport simultaneously. Through the ozone pre-treatment of Ta 2 O 5 /p-Si interface and optimization of the film thickness (≈9 nm), the interfacial recombination is suppressed and the contact resistivity is reduced from 178.0 to 29.3 mΩ cm 2 . Moreover, the Sn 4+ doping increases both the work function and oxygen vacancies of the film, contributing to the improved hole-selective contact performance. As a result, the photoelectric conversion efficiencies of Ta 2 O 5 /p-Si heterojunction solar cells are significantly improved from 14.84% to 18.47%, with a high thermal stability up to 300 °C. The work has provided a feasible strategy to explore new features of TMOs for carrier-selective contact applications, that is, bipolar carrier transport properties., (© 2023 Wiley‐VCH GmbH.)

The reversal of halide ions is studied under various conditions. However, the underlying mechanism of heat-induced reversal remains unclear. This work finds that dynamic disorder-induced localization of self-trapped polarons and thermal disorder-induced strain (TDIS) can be co-acting drivers of reverse segregation. Localization of polarons results in an order of magnitude decrease in excess carrier density (polaron population), causing a reduced impact of the light-induced strain (LIS - responsible for segregation) on the perovskite framework. Meanwhile, exposing the lattice to TDIS exceeding the LIS can eliminate the photoexcitation-induced strain gradient, as thermal fluctuations of the lattice can mask the LIS strain. Under continuous 0.1 W cm⁻ 2 illumination (upon segregation), the strain disorder is estimated to be 0.14%, while at 80 °C under dark conditions, the strain is 0.23%. However, in situ heating of the segregated film to 80 °C under continuous illumination (upon reversal) increases the total strain disorder to 0.25%, where TDIS is likely to have a dominant contribution. Therefore, the contribution of entropy to the system's free energy is likely to dominate, respectively. Various temperature-dependent in situ measurements and simulations further support the results. These findings highlight the importance of strain homogenization for designing stable perovskites under real-world operating conditions., (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Recently, multijunction tandem solar cells (TSCs) have presented high power conversion efficiency and revealed their immense potential in photovoltaic evolution. It is demonstrated that multiple light absorbers with various bandgap energies overcome the Shockley-Queisser limit of single-junction solar cells by absorbing the wide-range wavelength photons. Here, the main key challenges are reviewed, especially the charge carrier dynamics in perovskite-based 2-terminal (2-T) TSCs in terms of current matching, and how to manage these issues from a vantage point of characterization. To do this, the effect of recombination layers, optical and fabrication hurdles, and the impact of wide bandgap perovskite solar cells are discussed extensively. Afterward, this review focuses on various optoelectronics, spectroscopic, and theoretical (optical simulation) characterizations to figure out those issues, especially current-matching issues faced by the photovoltaic society. This review comprehensively provides deep insights into the relationship between the current-matching problems and the photovoltaic performance of TSCs through a variety of perspectives. Consequently, it is believed that this review is essential to address the main problems of 2-T TSCs, and the suggestions to elucidate the charge carrier dynamics and its characterization may pave the way to overcome such obstacles to further improve the development of 2-T TSCs in relation to the current-matching problems., (© 2023 Wiley-VCH GmbH.)

Tandem solar cells are rationally designed and fabricated by stacking multiple subcells to achieve power conversion efficiency well above the Shockley-Queisser (SQ) limit. There is a large selection pool for the subcell candidates, such as Si, III-V, Kesterite, Perovskite, and organic solar cells. A series of different combinations of these subcells have been successfully demonstrated in practical tandem solar cell devices. However, there has not been a systematic summary of how to connect subcells in a tandem solar cell using a practical, cost-effective, and efficiency-beneficial fashion. In this work, the connection manners of subcells within a tandem cell are classified into three main categories, performing sequential growth, using the physical connection, and applying an intermediate layer, focusing on systematical description of intermediate layers using different materials. The advantages and disadvantages of these connection methods and their applicability to tandem cell types are further elaborated using two typical example models, III-V/Si and Perovskite inclusive tandem cell devices. Eventually, this work can provide useful guidance on how to carry out a suitable intermediate connection in the design of tandem solar cells depending on the selected subcells and device structure., (© 2023 The Authors. Small Methods published by Wiley-VCH GmbH.)

Minimizing interfacial charged traps in perovskite films is crucial for reducing the non-radiative recombination and improving device performance. In this study, succinic acid (SA) derivatives varying active sites and spatial configurations are designed to modulate defects and crystallization in perovskite film. The SA derivative with two symmetric Br atoms, dibromosuccinic acid (DBSA), exhibits the optimal spatial arrangement for defect passivation. Experimental and theoretical results indicate that the carboxyl group and atomic Br in DBSA synergistically interact with the under-coordinated Pb 2+ . Moreover, the strong electronegativity of Br efficiently stabilizes the formamidinium cation via electrostatic interaction. Consequently, film quality is significantly improved and non-radiative recombination is markedly depressed, resulting in a photoluminesence lifetime of exceeding 4 µs of and a carrier diffusion length of 3 µm. An exceptional efficiency of 25.41% (certified at 25.00%) along with a high fill factor of 84.39% and excellent long-term operational stability have been achieved finally., (© 2023 Wiley-VCH GmbH.)

With excellent homogeneity, compactness and controllable thickness, atomic layer deposition (ALD) technology is widely used in perovskite solar cells (PSCs). However, residual organic sources and undesired reactions pose serious challenges to device performance as well as stability. Here, ester groups of poly(ethylene-co-vinyl acetate) are introduced as a reaction medium to promote the nucleation and complete conversion of tetrakis(dimethylamino)tin(IV) (TDMA-Sn). Through simulations and experiments, it is verified that ester groups as Lewis bases can coordinate with TDMA-Sn to facilitate homogeneous deposition of ALD-SnO x , which acts as self-encapsulated interface with blocking properties against external moisture as well as internal ion migration. Meanwhile, a comprehensive evaluation of the self-encapsulated interface reveals that the energy level alignment is optimized to improve the carrier transport. Finally, the self-encapsulated device obtains a champion photovoltaic conversion efficiency (PCE) of 22.06% and retains 85% of the initial PCE after being stored at 85 °C with relative humidity of 85% for more than 800 h., (© 2023 Wiley-VCH GmbH.)

The ever-growing need to inspect matter with hyperfine structures requires a revolution in current scintillation detectors, and the innovation of scintillators is revived with luminescent metal halides entering the scene. Notably, for any scintillator, two fundamental issues arise: Which kind of material is suitable and in what form should the material exist? The answer to the former question involves the sequence of certain atoms into specific crystal structures that facilitate the conversion of X-ray into light, whereas the answer to the latter involves assembling these crystallites into particular material forms that can guide light propagation toward its corresponding pixel detector. Despite their equal importance, efforts are overwhelmingly devoted to improving the X-ray-to-light conversion, while the material-form-associated light propagation, which determines the optical signal collected for X-ray imaging, is largely overlooked. This perspective critically correlates the reported spatial resolution with the light-propagation behavior in each form of metal halides, combing the designing rules for their future development., (© 2023 Wiley-VCH GmbH.)

In recent years, there has been an impressively fast technological progress in the development of highly efficient lead halide perovskite solar cells. Nonetheless, the stability of perovskite films and associated solar cells remains a source of uncertainty and necessitates sophisticated characterization techniques. Here, we report low- to mid-frequency resonant Raman spectra of formamidinium-based lead mixed-halide perovskites. The assignment of the different Raman lines in the measured spectra is assisted by DFT simulations of the Raman spectra of suitable periodic model systems. An important result of this work is that both experiment and theory point to an increase of the stability of the perovskite structure with increasing chloride doping concentration. In the Raman spectra, this is reflected by the appearance of new lines due to the formation of hydrogen bonds. Thus, higher chloride doping results in less torsional motion and lower asymmetric bending contributing to higher stability. This study yields a solid basis for the interpretation of the Raman spectra of formamidinium-based mixed-halide perovskites, furthering the understanding of the properties of these materials, which is essential for their full exploitation in solar cells., (© 2023 The Authors. ChemPhysChem published by Wiley-VCH GmbH.)

The application of halide perovskites in the photoelectrochemical generation of solar fuels and feedstocks is hindered by the instability of perovskites in aqueous electrolytes and the use of expensive electrode and catalyst materials, particularly in photoanodes driving kinetically slow water oxidation. Here, solely earth-abundant materials are incorporated to fabricate a CsPbBr 3 -based photoanode that reaches a low onset potential of +0.4 V RHE and 8 mA cm -2 photocurrent density at +1.23 V RHE for water oxidation, close to the radiative efficiency limit of CsPbBr 3 . This photoanode retains 100% of its stabilized photocurrent density for more than 100 h of operation by replacing once the inexpensive graphite sheet upon signs of deterioration. The improved performance is due to an efficiently electrodeposited NiFeOOH catalyst on a protective self-adhesive graphite sheet, and enhanced charge transfer achieved by phase engineering of CsPbBr 3 . Devices with >1 cm 2 area, and low-temperature processing demonstrate the potential for low capital cost, stable, and scalable perovskite photoanodes., (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Many devices heavily rely on combinatorial material optimization. However, new material alloys are classically developed by studying only a fraction of giant chemical space, while many intermediate compositions remain unmade in light of the lack of methods to synthesize gapless material libraries. Here report a high-throughput all-in-one material platform to obtain and study compositionally-tunable alloys from solution is reported. This strategy is applied to make all Cs x MA y FA z PbI 3 perovskite alloys (MA and FA stand for methylammonium and formamidinium, respectively), in less than 10 min, on a single film, on which 520 unique alloys are then studied. Through stability mapping of all these alloys in air supersaturated with moisture, a range of targeted perovskites are found, which are then chosen to make efficient and stable solar cells in relaxed fabrication conditions, in ambient air. This all-in-one platform provides access to an unprecedented library of compositional space with no unmade alloys, and hence aids in a comprehensive accelerated discovery of efficient energy materials., (© 2023 The Authors. Small published by Wiley-VCH GmbH.)

Exploring strategies to control the crystallization and modulate interfacial properties for high-quality perovskite film on industry-relevant textured crystalline silicon solar cells is highly valued in the perovskite/silicon tandem photovoltaics community. The formation of a 2D/3D perovskite heterojunction is widely employed to passivate defects and suppress ion migration in the film surface of perovskite solar cells. However, realizing solution-processed heterostructures at the buried interface faces solvent incompatibilities with the challenge of underlying-layer disruption, and texture incompatibilities with the challenge of uneven coverage. Here, a hybrid two-step deposition method is used to prepare robust 2D perovskites with cross-linkable ligands underneath the 3D perovskite. This structurally coherent interlayer benefits by way of preferred crystal growth of strain-free and uniform upper perovskite, inhibits interfacial defect-induced instability and recombination, and promotes charge-carrier extraction with ideal energy-level alignment. The broad applicability of the bottom-contact heterostructure for different textured substrates with conformal coverage and various precursor solutions with intact properties free of erosion are demonstrated. With this buried interface engineering strategy, the resulting perovskite/silicon tandem cells, based on industrially textured Czochralski (CZ) silicon, achieve a certified efficiency of 28.4% (1.0 cm 2 ), while retaining 89% of the initial PCE after over 1000 h operation., (© 2023 Wiley-VCH GmbH.)

Metal halide perovskite based materials have emerged over the past few decades as remarkable solution-processable optoelectronic materials with many intriguing properties and potential applications. These emerging materials have recently been considered for their promise in low-energy memory and information processing applications. In particular, their large optical cross-sections, high photoconductance contrast, large carrier-diffusion lengths, and mixed electronic/ionic transport mechanisms are attractive for enabling memory elements and neuromorphic devices that are written and/or read in the optical domain. Here, recent progress toward memory and neuromorphic functionality in metal halide perovskite materials and devices where photons are used as a critical degree of freedom for switching, memory, and neuromorphic functionality is reviewed., (© 2023 Wiley-VCH GmbH.)

The unprecedented development of perovskite solar cells (PSCs) makes them one of the most promising candidates for terawatt-scale green energy production with low cost. However, the high boiling point solvents during the solution-processed film deposition cause anisotropic crystal growth and toxic solvent vapor during high-throughput manufacturing. Here, a dual-component green solvent consisting of isopropyl acetate and acetonitrile is proposed to form a volatile perovskite precursor, which can realize the high-quality perovskite thin film deposition by intermediate phase regulation. A room-temperature stable perovskite intermediate phase is constructed with the engagement of isopropyl acetate as co-solvent, which suppresses the exploding nucleation rate in volatile perovskite precursor, providing a fine grain growth rate and wide processing window in scalable film deposition. The corresponding PSCs fabricated by blade coating without anti-solvents or gas quenching achieve power conversion efficiency (PCE) of 16.37 % and 15.29 % for the areas of 14.08 cm 2 and 37.83 cm 2 , respectively., (© 2023 Wiley-VCH GmbH.)

Given that it is closely related to perovskite crystallization and interfacial trap densities, buried interfacial engineering is crucial for creating effective and stable perovskite solar cells. Compared with the in-depth studies on the defect at the top perovskite interface, exploring the defect of the buried side of perovskite film is relatively complicated and scanty owing to the non-exposed feature. Herein, the degradation process is probed from the buried side of perovskite films with continuous illumination and its effects on morphology and photoelectronic characteristics with a facile lift-off method. Additionally, a buffer layer of Piperazine Dihydriodide (PDI 2 ) is inserted into the imbedded bottom interface. The PDI 2 buffer layer is able to lubricate the mismatched thermal expansion between perovskite and substrate, resulting in the release of lattice strain and thus a void-free buried interface. With the PDI 2 buffer layer, the degradation originates from the growing voids and increasing non-radiative recombination at the imbedded bottom interfaces are suppressed effectively, leading to prolonged operation lifetime of the perovskite solar cells. As a result, the power conversion efficiency of an optimized p-i-n inverted photovoltaic device reaches 23.47% (with certified 23.42%) and the unencapsulated devices maintain 90.27% of initial efficiency after 800 h continuous light soaking., (© 2023 Wiley-VCH GmbH.)

Despite great progress in perovskite photovoltaics, it should be noted that the intrinsic disorder dipolar cations in organic-inorganic hybrid perovskites exert negative effects on the energy band structure as well as the carrier separation and transfer dynamics. However, oriented polarization achieved by applying an external electric field may cause irreversible damage to perovskites. Herein, a unique and efficient strategy is developed to modulate the intrinsic dipole arrangement in perovskite films for high-performance and stable perovskite solar cells (PSCs). The spontaneous reorientation of dipolar cation methylamine is triggered by a polar molecule, constructing a vertical polarization during crystallization regulation. The oriented dipole determines a gradient energy-level arrangement in PSCs and more favorable energetics at interfaces, effectively enhancing the built-in electric field and suppressing the nonradiative recombination. Besides, the dipole reorientation induces a local dielectric environment to remarkably reduce exciton binding energy, leading to an ultralong carrier diffusion length of up to 1708 nm. Accordingly, the n-i-p PSCs achieve a significant increase in power conversion efficiency, reaching 24.63% with negligible hysteresis and exhibiting outstanding stabilities. This strategy also provides a facile route to eliminate the mismatched energetics and enhance carrier dynamics for other novel photovoltaic devices., (© 2023 Wiley-VCH GmbH.)

Methylammonium (MA)-free formamidinium (FA)-dominated Cs x FA 1-x PbI 3 is rising as the most promising candidate for highly efficient and stable perovskite solar cells. However, the growth of high-quality Cs x FA 1-x PbI 3 black-phase perovskite structure without ion doping in the lattice remains a challenge. Herein, propeller-shaped halogenated tertiary ammonium is synthesized, showing high binding energy on the perovskite surface and large steric hindrance. This molecule can significantly reduce the barrier of high surface energy that suppresses the growth of the α-phase Cs x FA 1-x PbI 3 structure. As a result, the α-phase structure can be formed at room temperature, which can further act as a seed for the growth of high-quality film. Solar cells based on the film show a record efficiency up to 23.6% for MA free Cs x FA 1- x PbI 3 solar cells with inverted structure and excellent stability at 85 °C over 200 h., (© 2023 Wiley-VCH GmbH.)

Organic-inorganic halide perovskites (OIHPs) obtained tremendous attention due to their low cost and excellent properties. However, the stability and toxicity of Pb-based OIHPs (POIHPs), as well as the weakness of efficiency and stability in Sn-based OIHPs (SOIHPs), are still serious issues for commercial application. Notably, composition engineering is an effective and direct strategy for improving these issues along with the control and modification of properties. Recently, the doping strategies for POIHPs and SOIHPs are booming. Based on the relationship between properties and composition, the doping strategies for POIHPs and SOIHPs, aiming to provide a comprehensive review and guidance for the research are systematically summarized. Moreover, the doping strategies for Pb-Sn mixed OIHPs are also discussed. Finally, a brief perspective and conclusion toward future possible doping schemes and properties designment of POIHPs and SOIHPs are offered., (© 2023 Wiley-VCH GmbH.)

Monolithic perovskite/silicon tandem solar cells promise power-conversion efficiencies (PCEs) exceeding the Shockley-Queisser limit of single-junction solar cells. The conformal deposition of perovskites on industrially feasible textured silicon solar cells allows for both lowered manufacturing costs and a higher matched photocurrent density, compared to state-of-the-art tandems using front-side flat or mildly textured silicon. However, the inferior crystal quality of perovskite films grown on fully-textured silicon compromises the photovoltaic performance. Here, an anion-engineered additive strategy is developed to control the crystallization process of wide-bandgap perovskite films, which enables improved film crystallinity, reduced trap density, and conformal deposition on industrially textured silicon. This strategy allows the fabrication of 28.6%-efficient perovskite/silicon heterojunction tandem solar cells (certified 27.9%, 1 cm 2 ). This approach is compatible with the scalable fabrication of tandems on industrially textured silicon, demonstrating an efficiency of 25.1% for an aperture area of 16 cm 2 . The anion-engineered additive significantly improves the operating stability of wide-bandgap perovskite solar cells, and the encapsulated tandem solar cells retain over 80% of their initial performance following 2000 h of operation under full 1-sun illumination in ambient conditions., (© 2023 Wiley-VCH GmbH.)

All-polymer organic photovoltaic (OPV) cells possessing high photovoltaic performance and mechanical robustness are promising candidates for flexible wearable devices. However, developing photoactive materials with good mechanical properties and photovoltaic performance so far remains challenging. In this work, a polymer donor PBDB-TF with a high weight-average molecular weight (M w ) is introduced to enable highly efficient all-polymer OPV cells featuring excellent mechanical reliability. By incorporating the high-M w PBDB-TF as a third component into the PBQx-TF:PY-IT blend, the bulk heterojunction morphology is finely tuned with a more compact π-π stacking distance, affording efficient pathways for charge transport as well as mechanical stress dissipation. Hence, all-polymer OPV cells based on the ternary blend film demonstrate a maximum power conversion efficiency (PCE) of 18.2% with an outstanding fill factor of 0.796. The flexible OPV cell delivers a decent PCE of 16.5% with high mechanical stability. These results present a promising strategy to address the mechanical properties and boost the photovoltaic performance of all-polymer OPV cells., (© 2022 Wiley-VCH GmbH.)

An unusual spectrally reproducible near-IR random lasing (RL) with no fluctuation of lasing peak wavelength is disclosed in polycrystalline films of formamidinium tin triiodide perovskite, which have been chemically stabilized against Sn 2+ to Sn 4+ oxidation. Remarkably, a quality Q-factor as high as ≈10 4 with an amplified spontaneous emission (ASE) threshold as low as 2 µJ cm -2 (both at 20 K) are achieved. The observed spectral reproducibility is unprecedented for semiconductor thin film RL systems and cannot be explained by the strong spatial localization of lasing modes. Instead, it is suggested that the spectral stability is a result of such an unique property of Sn-based perovskites as a large inhomogeneous broadening of the emitting centers, which is a consequence of an intrinsic structural inhomogeneity of the material. Due to this, lasing can occur simultaneously in modes that are spatially strongly overlapped, as long as the spectral separation between the modes is larger than the homogeneous linewidth of the emitting centers. The discovered mechanism of RL spectral stability in semiconductor materials, possessing inhomogeneous broadening, opens up prospects for their practical use as cheap sources of narrow laser lines., (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Single-crystal halide perovskites exhibit photogenerated-carriers of high mobility and long lifetime, making them excellent candidates for applications demanding thick semiconductors, such as ionizing radiation detectors, nuclear batteries, and concentrated photovoltaics. However, charge collection depreciates with increasing thickness; therefore, tens to hundreds of volts of external bias is required to extract charges from a thick perovskite layer, leading to a considerable amount of dark current and fast degradation of perovskite absorbers. However, extending the carrier-diffusion length can mitigate many of the anticipated issues preventing the practical utilization of perovskites in the abovementioned applications. Here, single-crystal perovskite solar cells that are up to 400 times thicker than state-of-the-art perovskite polycrystalline films are fabricated, yet retain high charge-collection efficiency in the absence of an external bias. Cells with thicknesses of 110, 214, and 290 µm display power conversion efficiencies (PCEs) of 20.0, 18.4, and 14.7%, respectively. The remarkable persistence of high PCEs, despite the increase in thickness, is a result of a long electron-diffusion length in those cells, which was estimated, from the thickness-dependent short-circuit current, to be ≈0.45 mm under 1 sun illumination. These results pave the way for adapting perovskite devices to optoelectronic applications in which a thick active layer is essential., (© 2022 Wiley-VCH GmbH.)

In this report, a large-area laser beam induced current microscope that has been adapted to perform intensity modulated photocurrent spectroscopy (IMPS) in an imaging mode is described. Microscopy-based IMPS method provides a spatial resolution of the frequency domain response of the solar cell, allowing correlation of the optoelectronic response with a particular interface, bulk material, specific transport layer, or transport parameter. The system is applied to study degradation effects in back-contact perovskite cells where it is found to readily differentiate areas based on their markedly different frequency response. Using the diffusion-recombination model, the IMPS response is modeled for a sandwich structure and extended for the special case of lateral diffusion in a back-contact cell. In the low-frequency limit, the model is used to calculate spatial maps of the carrier ambipolar diffusion length. The observed frequency response of IMPS images is then discussed., (© 2022 The Authors. Small Methods published by Wiley-VCH GmbH.)

Advanced doped-silicon-layer-based passivating contacts have boosted the power conversion efficiency (PCE) of single-junction crystalline silicon (c-Si) solar cells to over 26%. However, the inevitable parasitic light absorption of the doped silicon layers impedes further PCE improvement. To this end, alternative passivating contacts based on wide-bandgap metal compounds (so-called dopant-free passivating contacts (DFPCs)) have attracted great attention, thanks to their potential merits in terms of parasitic absorption loss, ease-of-deposition, and cost. Intensive research activity has surrounded this topic with significant progress made in recent years. Various electron-selective and hole-selective contacts based on metal compounds have been successfully developed, and a champion PCE of 23.5% has been achieved for a c-Si solar cell with a MoO x -based hole-selective contact. In this work, the fundamentals and development status of DFPCs are reviewed and the challenges and potential solutions for enhancing the carrier selectivity of DFPCs are discussed. Based on comprehensive and in-depth analysis and simulations, the improvement strategies and future prospects for DFPCs design and device implementation are pointed out. By tuning the carrier concentration of the metal compound and the work function of the capping transparent electrode, high PCEs over 26% can be achieved for c-Si solar cells with DFPCs., (© 2022 Wiley-VCH GmbH.)

This review focuses on monolithic 2-terminal perovskite-silicon tandem solar cells and discusses key scientific and technological challenges to address in view of an industrial implementation of this technology. The authors start by examining the different crystalline silicon (c-Si) technologies suitable for pairing with perovskites, followed by reviewing recent developments in the field of monolithic 2-terminal perovskite-silicon tandems. Factors limiting the power conversion efficiency of these tandem devices are then evaluated, before discussing pathways to achieve an efficiency of >32%, a value that small-scale devices will likely need to achieve to make tandems competitive. Aspects related to the upscaling of these device active areas to industry-relevant ones are reviewed, followed by a short discussion on module integration aspects. The review then focuses on stability issues, likely the most challenging task that will eventually determine the economic viability of this technology. The final part of this review discusses alternative monolithic perovskite-silicon tandem designs. Finally, key areas of research that should be addressed to bring this technology from the lab to the fab are highlighted., (© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

While halide perovskites have excellent optoelectronic properties, their poor stability is a major obstacle toward commercialization. There is a strong interest to move away from organic A-site cations such as methylammonium and formamidinium toward Cs with the aim of improving thermal stability of the perovskite layers. While the optoelectronic properties and the device performance of Cs-based all-inorganic lead-halide perovskites are very good, they are still trailing behind those of perovskites that use organic cations. Here, the state-of-the-art of all-inorganic perovskites for photovoltaic applications is reviewed by performing detailed meta-analyses of key performance parameters on the cell and material level. Key material properties such as carrier mobilities, external photoluminescence quantum efficiency, and photoluminescence lifetime are discussed and what is known about defect tolerance in all-inorganic is compared relative to hybrid (organic-inorganic) perovskites. Subsequently, a unified approach is adopted for analyzing performance losses in perovskite solar cells based on breaking down the losses into several figures of merit representing recombination losses, resistive losses, and optical losses. Based on this detailed loss analysis, guidelines are eventually developed for future performance improvement of all-inorganic perovskite solar cells., (© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Herein, we demonstrate a vacuum-based evaporation approach to fabricate organic-inorganic perovskite thin films by using phase-formed halide perovskite nanoparticles (NPs) as a precursor/source. We are able to consistently obtain MAPbX 3 (MA=CH 3 NH 3 and X=Cl, Br or I) thin films at various substrates (e. g., glass, ITO, or plastic). The perovskite phase formation in thin film form is confirmed by x-ray diffraction (XRD) studies. Small micro-strain (tensile) values of 1.64×10 -3 , 1.42×10 -3 and 6.85×10 -4 obtained for MAPbCl 3 , MAPbBr 3 and MAPbI 3 films respectively from Williamson-Hall equation indicate low structural distortions in perovskite thin films. The absorption spectra of thin films show sharp band edge having direct band gap, which is followed by narrow full width at half maxima (FWHM ∼0.1 eV) of the emission peak. Thin films of MAPbCl 3 , MAPbBr 3 and MAPbI 3 show direct band gap of 3.1 eV, 2.4 eV and 1.6 eV, respectively. Small Urbach energy values of 33 meV, 44 meV and 66 meV for MAPbCl 3 , MAPbBr 3 and MAPbI 3 films respectively indicates low defect density in various perovskite films. Scanning electron microscopy (SEM) along with energy-dispersive X-ray spectroscopy (EDS) shows high surface coverage and uniform chemical composition of MAPbX 3 (X=Cl, Br and I) thin films deposited by the present method. We have successfully controlled the film thickness from 250 nm to 1 μm by varying the nanoparticle precursor amount. The perovskite thin films deposited by the present method are highly stable against the degradation under ambient conditions. Systematic XRD studies along with absorption data demonstrate that the MAPbCl 3 and MAPbBr 3 films stored under ambient conditions remained stable for more than 30 days and MAPbI 3 films for more than 7 days., (© 2022 Wiley-VCH GmbH.)