Amide‐Catalyzed Phase‐Selective Crystallization Reduces Defect Density in Wide‐Bandgap Perovskites

Wide‐bandgap (WBG) formamidinium–cesium (FA‐Cs) lead iodide–bromide mixed perovskites are promising materials for front cells well‐matched with crystalline silicon to form tandem solar cells. They offer avenues to augment the performance of widely deployed commercial solar cells. However, phase instability, high open‐circuit voltage (V_oc) deficit, and large hysteresis limit this otherwise promising technology. Here, by controlling the crystallization of FA‐Cs WBG perovskite with the aid of a formamide cosolvent, light‐induced phase segregation and hysteresis in perovskite solar cells are suppressed. The highly polar solvent additive formamide induces direct formation of the black perovskite phase, bypassing the yellow phases, thereby reducing the density of defects in films. As a result, the optimized WBG perovskite solar cells (PSCs) (E_g ≈ 1.75 eV) exhibit a high V_oc of 1.23 V, reduced hysteresis, and a power conversion efficiency (PCE) of 17.8%. A PCE of 15.2% on 1.1 cm² solar cells, the highest among the reported efficiencies for large‐area PSCs having this bandgap is also demonstrated. These perovskites show excellent phase stability and thermal stability, as well as long‐term air stability. They maintain ≈95% of their initial PCE after 1300 h of storage in dry air without encapsulation.     

Highly Efficient and Stable GABr-Modified Ideal-Bandgap (1.35 eV) Sn/Pb Perovskite Solar Cells Achieve 20.63% Efficiency with a Record Small Voc Deficit of 0.33 V

1.5–1.6 eV bandgap Pb-based perovskite solar cells (PSCs) with 30–31% theoretical efficiency limit by the Shockley–Queisser model achieve 21–24% power conversion efficiencies (PCEs). However, the best PCEs of reported ideal-bandgap (1.3–1.4 eV) Sn–Pb PSCs with a higher 33% theoretical efficiency limit are <18%, mainly because of their large open-circuit voltage (V_oc) deficits (>0.4 V). Herein, it is found that the addition of guanidinium bromide (GABr) can significantly improve the structural and photoelectric characteristics of ideal-bandgap (≈1.34 eV) Sn–Pb perovskite films. GABr introduced in the perovskite films can efficiently reduce the high defect density caused by Sn²⁺ oxidation in the perovskite, which is favorable for facilitating hole transport, decreasing charge-carrier recombination, and reducing the V_oc deficit. Therefore, the best PCE of 20.63% with a certificated efficiency of 19.8% is achieved in 1.35 eV PSCs, along with a record small V_oc deficit of 0.33 V, which is the highest PCE among all values reported to date for ideal-bandgap Sn–Pb PSCs. Moreover, the GABr-modified PSCs exhibit significantly improved environmental and thermal stability. This work represents a noteworthy step toward the fabrication of efficient and stable ideal-bandgap PSCs.     

Ideal Bandgap Organic–Inorganic Hybrid Perovskite Solar Cells

Extremely high power conversion efficiencies (PCEs) of ≈20–22% are realized through intensive research and development of 1.5–1.6 eV bandgap perovskite absorbers. However, development of ideal bandgap (1.3–1.4 eV) absorbers is pivotal to further improve PCE of single junction perovskite solar cells (PVSCs) because of a better balance between absorption loss of sub‐bandgap photons and thermalization loss of above‐bandgap photons as demonstrated by the Shockley–Queisser detailed balanced calculation. Ideal bandgap PVSCs are currently hindered by the poor optoelectronic quality of perovskite absorbers and their PCEs have stagnated at <15%. In this work, through systematic photoluminescence and photovoltaic analysis, a new ideal bandgap (1.35 eV) absorber composition (MAPb_0.5Sn_0.5(I_0.8Br_0.2)₃) is rationally designed and developed, which possesses lower nonradiative recombination states, band edge disorder, and Urbach energy coupled with a higher absorption coefficient, which yields a reduced V_oc,loss (0.45 V) and improved PCE (as high as 17.63%) for the derived PVSCs. This work provides a promising platform for unleashing the complete potential of ideal bandgap PVSCs and prospects for further improvement.     

Synergistic Effect of Surface p-Doping and Passivation Improves the Efficiency,Stability, and Reduces Lead Leakage in All-Inorganic CsPbIBr2-Based Perovskite Solar Cells

Wide-bandgap inorganic cesium lead halide CsPbIBr₂ is a popular optoelectronic material that researchers are interested in because of the character that balances the power conversion efficiency and stability of solar cells. It also has great potential in semitransparent solar cells, indoor photovoltaics, and as a subcell for tandem solar cells. Although CsPbIBr₂-based devices have achieved good performance, the open-circuit voltage (V_oc) of CsPbIBr₂-based perovskite solar cells (PSCs) is still lower, and it is critical to further reduce large energy losses (E_loss). Herein, a strategy is proposed for achieving surface p-type doping for CsPbIBr₂-based perovskite for the first time, using 1,5-Diaminopentane dihydroiodide at the perovskite surface to improve hole extraction efficiency. Meanwhile, the adjusted energy levels reduce E_loss and improve V_oc of the CsPbIBr₂ PSCs. Furthermore, the Cs- and Br-vacancies at the interface are filled, reducing structural disorder and defect states and thus improving the quality of the perovskite film. As a result, the target device achieves a high efficiency of 11.02% with a V_oc of 1.33 V, which is among the best values. In addition to the improved performance, the stability of the target device under various conditions is enhanced, and the lead leakage is effectively suppressed.     

A Tandem Organic Solar Cell with PCE of 14.52% Employing Subcells with the Same Polymer Donor and Two Absorption Complementary Acceptors

The tandem structure is an efficient way to simultaneously tackle absorption and thermalization losses of the single junction solar cells. In this work, a high‐performance tandem organic solar cell (OSC) using two subcells with the same donor poly[(2,6‐(4,8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)‐benzo[1,2‐b:4,5‐b′]dithiophene))‐alt‐(5,5‐(1′,3′‐di‐2‐thienyl‐5′,7′‐bis(2‐ethylhexyl)benzo[1′,2′‐c:4′,5′‐c′]dithiophene‐4,8‐dione))] (PBDB‐T) and two acceptors, F‐M and 2,9‐bis(2‐methylene‐(3(1,1‐dicyanomethylene)benz[f ]indanone))7,12‐dihydro‐(4,4,10,10‐tetrakis(4‐hexylphenyl)‐5,11‐diocthylthieno[3′,2′:4,5]cyclopenta[1,2‐b]thieno[2″,3″:3′,4′]cyclopenta[1′,2′:4,5]thieno[2,3‐f][1]benzothiophene (NNBDT), with complementary absorptions is demonstrated. The two subcells show high V_oc with value of 0.99 V for the front cell and 0.86 V for the rear cell, which is the prerequisite for obtaining high V_oc of their series‐connected tandem device. Although there is much absorption overlap for the subcells, a decent J_sc of the tandem cell is still obtained owing to the complementary absorption of the two acceptors in a wide range. With systematic device optimizations, a best power conversion efficiency of 14.52% is achieved for the tandem device, with a high V_oc of 1.82 V, a notable FF of 74.7%, and a decent J_sc of 10.68 mA cm^?2. This work demonstrates a promising strategy of fabricating high‐efficiency tandem OSCs through elaborate selection of the active layer materials in each subcell and tradeoff of the V_oc and J_sc of the tandem cells.     

Polymer‐Passivated Inorganic Cesium Lead Mixed‐Halide Perovskites for Stable and Efficient Solar Cells with High Open‐Circuit Voltage over 1.3 V

Cesium‐based trihalide perovskites have been demonstrated as promising light absorbers for photovoltaic applications due to their superb composition stability. However, the large energy losses (E_loss) observed in inorganic perovskite solar cells has become a major hindrance impairing the ultimate efficiency. Here, an effective and reproducible method of modifying the interface between a CsPbI₂Br absorber and polythiophene hole‐acceptor to minimize the E_loss is reported. It is demonstrated that polythiophene, deposited on the top of CsPbI₂Br, can significantly reduce electron‐hole recombination within the perovskite, which is due to the electronic passivation of surface defect states. In addition, the interfacial properties are improved by a simple annealing process, leading to significantly reduced energy disorder in polythiophene and enhanced hole‐injection into the hole‐acceptor. Consequently, one of the highest power conversion efficiency (PCE) of 12.02% from a reverse scan in inorganic mixed‐halide perovskite solar cells is obtained. Modifying the perovskite films with annealing polythiophene enables an open‐circuit voltage (V_OC) of up to 1.32 V and E_loss of down to 0.5 eV, which both are the optimal values reported among cesium‐lead mixed‐halide perovskite solar cells to date. This method provides a new route to further improve the efficiency of perovskite solar cells by minimizing the E_loss.     

Highly Efficient Nonfullerene Polymer Solar Cells Enabled by a Copper(I) Coordination Strategy Employing a 1,3,4‐Oxadiazole‐Containing Wide‐Bandgap Copolymer Donor

A novel wide‐bandgap copolymer of PBDT‐ODZ based on benzo[1,2‐b:4,5‐b′ ]dithiophene (BDT) and 1,3,4‐oxadiazole (ODZ) blocks is developed for efficient nonfullerene polymer solar cells (NF‐PSCs). PBDT‐ODZ exhibits a wide bandgap of 2.12 eV and a low‐lying highest occupied molecular orbital (HOMO) level of ?5.68 eV, which could match well with the low‐bandgap acceptor of 3,9‐bis(2‐methylene‐(3‐(1,1‐dicyanomethylene)‐indanone)‐5,5,11,11‐tetrakis(4‐hexylthienyl)‐dithieno[2,3‐d:2′,3′‐d′]‐s‐indaceno[1,2‐b:5,6‐b′]‐dithiophene (ITIC‐Th), inducing a good complementary absorption from 300 to 800 nm and a minimal HOMO level offset (0.1 eV). The PBDT‐ODZ:ITIC‐Th devices exhibit a large open‐circuit voltage (V_oc) of 1.08 eV and a low energy loss (E_loss) of 0.50 eV, delivering a high power conversion efficiency (PCE) of 10.12%. By adding a small amount of copper(I) iodide (CuI) as an additive to form coordination complexes in the active blends, much higher device performances are achieved due to the improved absorption and crystallinity. After incorporating 4% of CuI, the PCE is elevated to 12.34%, with a V_oc of 1.06 V, a J_sc of 17.1 mA cm^?2 and a fill factor of 68.1%. This work not only provides a novel oxadiazole‐containing wide‐bandgap polymeric donor candidate for high‐performance NF‐PSCs but also presents an efficient morphology‐optimization approach to elevate the PCE of NF‐PSCs for future practical applications.     

Realizing Over 13% Efficiency in Green‐Solvent‐Processed Nonfullerene Organic Solar Cells Enabled by 1,3,4‐Thiadiazole‐Based Wide‐Bandgap Copolymers

Two novel wide‐bandgap copolymers, PBDT‐TDZ and PBDTS‐TDZ, are developed based on 1,3,4‐thiadiazole (TDZ) and benzo[1,2‐b:4,5‐b′]dithiophene (BDT) building blocks. These copolymers exhibit wide bandgaps over 2.07 eV and low‐lying highest occupied molecular orbital (HOMO) levels below −5.35 eV, which match well with the typical low‐bandgap acceptor of ITIC, resulting in a good complementary absorption from 300 to 900 nm and a low HOMO level offset (≤0.13 eV). Compared to PBDT‐TDZ, PBDTS‐TDZ with alkylthio side chains exhibits the stronger optical absorption, lower‐lying HOMO level, and higher crystallinity. By using a single green solvent of o‐xylene, PBDTS‐TDZ:ITIC devices exhibit a large open‐circuit voltage (V_oc) up to 1.10 eV and an extremely low energy loss (E_loss) of 0.48 eV. At the same time, the desirable high short‐circuit current density (J_sc) of 17.78 mA cm⁻² and fill factor of 65.4% are also obtained, giving rise to a high power conversion efficiency (PCE) of 12.80% without any additive and post‐treatment. When adopting a homotandem device architecture, the PCE is further improved to 13.35% (certified as 13.19%) with a much larger V_oc of 2.13 V, which is the best value for any type of homotandem organic solar cells reported so far.     

Matching Charge Extraction Contact for Wide‐Bandgap Perovskite Solar Cells

Efficient wide‐bandgap (WBG) perovskite solar cells are needed to boost the efficiency of silicon solar cells to beyond Schottky–Queisser limit, but they suffer from a larger open circuit voltage (V_OC) deficit than narrower bandgap ones. Here, it is shown that one major limitation of V_OC in WBG perovskite solar cells comes from the nonmatched energy levels of charge transport layers. Indene‐C60 bisadduct (ICBA) with higher‐lying lowest‐unoccupied‐molecular‐orbital is needed for WBG perovskite solar cells, while its energy‐disorder needs to be minimized before a larger V_OC can be observed. A simple method is applied to reduce the energy disorder by isolating isomer ICBA‐tran3 from the as‐synthesized ICBA‐mixture. WBG perovskite solar cells with ICBA‐tran3 show enhanced V_OC by 60 mV, reduced V_OC deficit of 0.5 V, and then a record stabilized power conversion efficiency of 18.5%. This work points out the importance of matching the charge transport layers in perovskite solar cells when the perovskites have a different composition and energy levels.     

Europium and Acetate Co‐doping Strategy for Developing Stable and Efficient CsPbI2Br Perovskite Solar Cells

All‐inorganic perovskite solar cells have developed rapidly in the last two years due to their excellent thermal and light stability. However, low efficiency and moisture instability limit their future commercial application. The mixed‐halide inorganic CsPbI₂Br perovskite with a suitable bandgap offers a good balance between phase stability and light harvesting. However, high defect density and low carrier lifetime in CsPbI₂Br perovskites limit the open‐circuit voltage (V_oc < 1.2 V), short‐circuit current density (J_sc < 15 mA cm^?2), and fill factor (FF < 75%) of CsPbI₂Br perovskite solar cells, resulting in an efficiency below 14%. For the first time, a CsPbI₂Br perovskite is doped by Eu(Ac)₃ to obtain a high‐quality inorganic perovskite film with a low defect density and long carrier lifetime. A high efficiency of 15.25% (average efficiency of 14.88%), a respectable V_oc of 1.25 V, a reasonable J_sc of 15.44 mA cm^?2, and a high FF of 79.00% are realized for CsPbI₂Br solar cells. Moreover, the CsPbI₂Br solar cells with Eu(Ac)₃ doping demonstrate excellent air stability and maintain more than 80% of their initial power conversion efficiency (PCE) values after aging in air (relative humidity: 35–40%) for 30 days.     

Nonfullerene Tandem Organic Solar Cells with High Performance of 14.11%

Fabricating solar cells with tandem structure is an efficient way to broaden the photon response range without further increasing the thermalization loss in the system. In this work, a tandem organic solar cell (TOSC) based on highly efficient nonfullerene acceptors (NFAs) with series connection type is demonstrated. To meet the different demands of front and rear sub‐cells, two NFAs named F‐M and NOBDT with a whole absorption range from 300 to 900 nm are designed, when blended with wide bandgap polymer poly[(2,6‐(4,8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)‐benzo[1,2‐b:4,5‐b′]dithiophene))‐alt‐(5,5‐(1′,3′‐di‐2‐thienyl‐5′,7′‐bis(2‐ethylhexyl)benzo[1′,2′‐c:4′,5′‐c′]dithiophene‐4,8‐dione))] (PBDB‐T) and narrow bandgap polymer PTB7‐Th, respectively, the PBDB‐T: F‐M system exhibits a high V_oc of 0.98 V and the PTB7‐Th: NOBDT system shows a remarkable J_sc of 19.16 mA cm^?2, which demonstrate their potential in the TOSCs. With the guidance of optical simulation, by systematically optimizing the thickness of each layer in the TOSC, an outstanding power conversion efficiency of 14.11%, with a V_oc of 1.71 V, a J_sc of 11.72 mA cm^?2, and a satisfactory fill factor of 0.70 is achieved; this result is one of the top efficiencies reported to date in the field of organic solar cells.     

Solution-Processed Organic Solar Cells with High Open-Circuit Voltage of 1.3 V and Low Non-Radiative Voltage Loss of 0.16 V

Compared with inorganic or perovskite solar cells, the relatively large non-radiative recombination voltage losses (ΔV_non-rad) in organic solar cells (OSCs) limit the improvement of the open-circuit voltage (V_oc). Herein, OSCs are fabricated by adopting two pairs of D–π–A polymers (PBT1-C/PBT1-C-2Cl and PBDB-T/PBDB-T-2Cl) as electron donors and a wide-bandgap molecule BTA3 as the electron acceptor. In these blends, a charge-transfer state energy (E_CT) as high as 1.70–1.76 eV is achieved, leading to small energetic differences between the singlet excited states and charge-transfer states (ΔE_CT ≈ 0.1 eV). In addition, after introducing chlorine atoms into the π-bridge or the side chain of benzodithiophene (BDT) unit, electroluminescence external quantum efficiencies as high as 1.9 × 10⁻³ and 1.0 × 10⁻³ are realized in OSCs based on PBTI-C-2Cl and PBDB-T-2Cl, respectively. Their corresponding ΔV_non-rad are 0.16 and 0.17 V, which are lower than those of OSCs based on the analog polymers without a chlorine atom (0.21 and 0.24 V for PBT1-C and PBDB-T, respectively), resulting in high V_oc of 1.3 V. The ΔV_non-rad of 0.16 V and V_oc of 1.3 V achieved in PBT1-C-2Cl:BTA3 OSCs are thought to represent the best values for solution-processed OSCs reported in the literature so far.     

Electron‐Deficient and Quinoid Central Unit Engineering for Unfused Ring‐Based A1–D–A2–D–A1‐Type Acceptor Enables High Performance Nonfullerene Polymer Solar Cells with High Voc and PCE Simultaneously

Here, a pair of A₁–D–A₂–D–A₁ unfused ring core‐based nonfullerene small molecule acceptors (NF‐SMAs), BO2FIDT‐4Cl and BT2FIDT‐4Cl is synthesized, which possess the same terminals (A₁) and indacenodithiophene unit (D), coupling with different fluorinated electron‐deficient central unit (difluorobenzoxadiazole or difluorobenzothiadiazole) (A₂). BT2FIDT‐4Cl exhibits a slightly smaller optical bandgap of 1.56 eV, upshifted highest occupied molecular orbital energy levels, much higher electron mobility, and slightly enhanced molecular packing order in neat thin films than that of BO2FIDT‐4Cl . The polymer solar cells (PSCs) based on BT2FIDT‐4Cl:PM7 yield the best power conversion efficiency (PCE) of 12.5% with a V_oc of 0.97 V, which is higher than that of BO2FIDT‐4Cl ‐based devices (PCE of 10.4%). The results demonstrate that the subtle modification of A₂ unit would result in lower trap‐assisted recombination, more favorable morphology features, and more balanced electron and hole mobility in the PM7:BT2FIDT‐4Cl blend films. It is worth mentioning that the PCE of 12.5% is the highest value in nonfused ring NF‐SMA‐based binary PSCs with high V_oc over 0.90 V. These results suggest that appropriate modulation of the quinoid electron‐deficient central unit is an effective approach to construct highly efficient unfused ring NF‐SMAs to boost PCE and V_oc simultaneously.     

Fine‐Tuning the Energy Levels of a Nonfullerene Small‐Molecule Acceptor to Achieve a High Short‐Circuit Current and a Power Conversion Efficiency over 12% in Organic Solar Cells

Organic solar cell optimization requires careful balancing of current–voltage output of the materials system. Here, such optimization using ultrafast spectroscopy as a tool to optimize the material bandgap without altering ultrafast photophysics is reported. A new acceptor–donor–acceptor (A–D–A)‐type small‐molecule acceptor NCBDT is designed by modification of the D and A units of NFBDT. Compared to NFBDT, NCBDT exhibits upshifted highest occupied molecular orbital (HOMO) energy level mainly due to the additional octyl on the D unit and downshifted lowest unoccupied molecular orbital (LUMO) energy level due to the fluorination of A units. NCBDT has a low optical bandgap of 1.45 eV which extends the absorption range toward near‐IR region, down to ≈860 nm. However, the 60 meV lowered LUMO level of NCBDT hardly changes the V_oc level, and the elevation of the NCBDT HOMO does not have a substantial influence on the photophysics of the materials. Thus, for both NCBDT‐ and NFBDT‐based systems, an unusually slow (≈400 ps) but ultimately efficient charge generation mediated by interfacial charge‐pair states is observed, followed by effective charge extraction. As a result, the PBDB‐T:NCBDT devices demonstrate an impressive power conversion efficiency over 12%—among the best for solution‐processed organic solar cells.     

Highly Efficient Porphyrin‐Based OPV/Perovskite Hybrid Solar Cells with Extended Photoresponse and High Fill Factor

Employing a layer of bulk‐heterojunction (BHJ) organic semiconductors on top of perovskite to further extend its photoresponse is considered as a simple and promising way to enhance the efficiency of perovskite‐based solar cells, instead of using tandem devices or near infrared (NIR)‐absorbing Sn‐containing perovskites. However, the progress made from this approach is quite limited because very few such hybrid solar cells can simultaneously show high short‐circuit current (J_SC) and fill factor (FF). To find an appropriate NIR‐absorbing BHJ is essential for highly efficient, organic, photovoltaics (OPV)/perovskite hybrid solar cells. The materials involved in the BHJ layer not only need to have broad photoresponse to increase J_SC, but also possess suitable energy levels and high mobility to afford high V_OC and FF. In this work, a new porphyrin is synthesized and blended with [6,6]‐phenyl‐C61‐butyric acid methyl ester (PCBM) to function as an efficient BHJ for OPV/perovskite hybrid solar cells. The extended photoresponse, well‐matched energy levels, and high hole mobility from optimized BHJ morphology afford a very high power conversion efficiency (PCE) (19.02%) with high V_oc, J_SC, and FF achieved simultaneously. This is the highest value reported so far for such hybrid devices, which demonstrates the feasibility of further improving the efficiency of perovskite devices.     

FA‐Assistant Iodide Coordination in Organic–Inorganic Wide‐Bandgap Perovskite with Mixed Halides

Mixed‐halide wide‐bandgap perovskites are key components for the development of high‐efficiency tandem structured devices. However, mixed‐halide perovskites usually suffer from phase‐impurity and high defect density issues, where the causes are still unclear. By using in situ photoluminescence (PL) spectroscopy, it is found that in methylammonium (MA⁺)‐based mixed‐halide perovskites, MAPb(I_0.6Br_0.4)₃, the halide composition of the spin‐coated perovskite films is preferentially dominated by the bromide ions (Br^?). Additional thermal energy is required to initiate the insertion of iodide ions (I^?) to achieve the stoichiometric balance. Notably, by incorporating a small amount of formamidinium ions (FA⁺) in the precursor solution, it can effectively facilitate the I^? coordination in the perovskite framework during the spin‐coating and improve the composition homogeneity of the initial small particles. The aggregation of these homogenous small particles is found to be essential to achieve uniform and high‐crystallinity perovskite film with high Br^? content. As a result, high‐quality MA_0.9FA_0.1Pb(I_0.6Br_0.4)₃ perovskite film with a bandgap (E_g) of 1.81 eV is achieved, along with an encouraging power‐conversion‐efficiency of 17.1% and open‐circuit voltage (V_oc) of 1.21 V. This work also demonstrates the in situ PL can provide a direct observation of the dynamic of ion coordination during the perovskite crystallization.     

Precise Control of Crystallization and Phase-Transition with Green Anti-Solvent in Wide-Bandgap Perovskite Solar Cells with Open-Circuit Voltage Exceeding 1.25 V

Wide-bandgap perovskite solar cells (PSCs) have attracted a lot of attention due to their application in tandem solar cells. However, the open-circuit voltage (V_OC) of wide-bandgap PSCs is dramatically limited by high defect density existing at the interface and bulk of the perovskite film. Here, an anti-solvent optimized adduct to control perovskite crystallization strategy that reduces nonradiative recombination and minimizes V_OC deficit is proposed. Specifically, an organic solvent with similar dipole moment, isopropanol (IPA) is added into ethyl acetate (EA) anti-solvent, which is beneficial to form PbI₂ adducts with better crystalline orientation and direct formation of α-phase perovskite. As a result, EA-IPA (7-1) based 1.67 eV PSCs deliver a power conversion efficiency of 20.06% and a V_OC of 1.255 V, which is one of the remarkable values for wide-bandgap around 1.67 eV. The findings provide an effective strategy for controlling crystallization to reduce defect density in PSCs.     

Highly Stable and Efficient FASnI3‐Based Perovskite Solar Cells by Introducing Hydrogen Bonding

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 Narrow-Bandgap n-Type Polymer with an Acceptor–Acceptor Backbone Enabling Efficient All-Polymer Solar Cells

Narrow-bandgap polymer semiconductors are essential for advancing the development of organic solar cells. Here, a new narrow-bandgap polymer acceptor L14, featuring an acceptor–acceptor (A–A) type backbone, is synthesized by copolymerizing a dibrominated fused-ring electron acceptor (FREA) with distannylated bithiophene imide. Combining the advantages of both the FREA and the A–A polymer, L14 not only shows a narrow bandgap and high absorption coefficient, but also low-lying frontier molecular orbital (FMO) levels. Such FMO levels yield improved electron transfer character, but unexpectedly, without sacrificing open-circuit voltage (V_oc), which is attributed to a small nonradiative recombination loss (E_loss,nr) of 0.22 eV. Benefiting from the improved photocurrent along with the high fill factor and V_oc, an excellent efficiency of 14.3% is achieved, which is among the highest values for all-polymer solar cells (all-PSCs). The results demonstrate the superiority of narrow-bandgap A–A type polymers for improving all-PSC performance and pave a way toward developing high-performance polymer acceptors for all-PSCs.     

High‐Efficiency Nonfullerene Organic Solar Cells with a Parallel Tandem Configuration

In this work, a highly efficient parallel connected tandem solar cell utilizing a nonfullerene acceptor is demonstrated. Guided by optical simulation, each of the active layer thicknesses of subcells are tuned to maximize its light trapping without spending intense effort to match photocurrent. Interestingly, a strong optical microcavity with dual oscillation centers is formed in a back subcell, which further enhances light absorption. The parallel tandem device shows an improved photon‐to‐electron response over the range between 450 and 800 nm, and a high short‐circuit current density (J _SC) of 17.92 mA cm^?2. In addition, the subcells show high fill factors due to reduced recombination loss under diluted light intensity. These merits enable an overall power conversion efficiency (PCE) of >10% for this tandem cell, which represents a ≈15% enhancement compared to the optimal single‐junction device. Further application of the designed parallel tandem configuration to more efficient single‐junction cells enable a PCE of >11%, which is the highest efficiency among all parallel connected organic solar cells (OSCs). This work stresses the importance of employing a parallel tandem configuration for achieving efficient light harvesting in nonfullerene‐based OSCs. It provides a useful strategy for exploring the ultimate performance of organic solar cells.