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.     

Organic-Salt-Assisted Crystal Growth and Orientation of Quasi-2D Ruddlesden–Popper Perovskites for Solar Cells with Efficiency over 19%

Quasi-2D Ruddlesden–Popper (RP) perovskite solar cells (PSCs) have drawn significant attention due to their appealing environmental stability compared to their 3D counterparts. However, the relatively low power conversion efficiency (PCE) greatly limits their applications. Here, high photovoltaic performance is demonstrated for quasi-2D RP PSCs using 2-thiophenemethylammonium as spacer with nominal n-value of 5, which is based on the stoichiometry of the precursors. The incorporation of formamidinium (FA) in quasi-2D RP perovskites reduces the bandgap and improves the light absorption ability, resulting in enlarged photocurrent and an increased PCE of 16.18%, which is higher than that of reported analogous methylammonium (MA)-based quasi-2D PSC (≈15%). A record high PCE of 19.06% is further demonstrated by using an organic salt, namely, 4-(trifluoromethyl)benzylammonium iodide, assisted crystal growth (OACG) technique, which can induce the crystal growth and orientation, tune the surface energy levels, and suppress the charge recombination losses. More importantly, the devices based on OACG-processed quasi-2D RP perovskites show remarkable environmental stability and thermal stability, for example, the PCE retaining ≈96% of its initial value after storage at 80 °C for 576 h, while only ≈37% of the original efficiency left for FAPbI₃-based 3D PSCs.     

Compositional Control in 2D Perovskites with Alternating Cations in the Interlayer Space for Photovoltaics with Efficiency over 18%

2D perovskites stabilized by alternating cations in the interlayer space (ACI) represent a very new entry as highly efficient semiconductors for solar cells approaching 15% power conversion efficiency (PCE). However, further improvements will require understanding of the nature of the films, e.g., the thickness distribution and charge‐transfer characteristics of ACI quantum wells (QWs), which are currently unknown. Here, efficient control of the film quality of ACI 2D perovskite (GA)(MA)_nPb_nI_3n+1 (〈n〉 = 3) QWs via incorporation of methylammonium chloride as an additive is demonstrated. The morphological and optoelectronic characterizations unambiguously demonstrate that the additive enables a larger grain size, a smoother surface, and a gradient distribution of QW thickness, which lead to enhanced photocurrent transport/extraction through efficient charge transfer between low‐n and high‐n QWs and suppressed nonradiative charge recombination. Therefore, the additive‐treated ACI perovskite film delivers a champion PCE of 18.48%, far higher than the pristine one (15.79%) due to significant improvements in open‐circuit voltage and fill factor. This PCE also stands as the highest value for all reported 2D perovskite solar cells based on the ACI, Ruddlesden–Popper, and Dion–Jacobson families. These findings establish the fundamental guidelines for the compositional control of 2D perovskites for efficient photovoltaics.     

The Role of Bulk and Interface Recombination in High‐Efficiency Low‐Dimensional Perovskite Solar Cells

2D Ruddlesden–Popper perovskite (RPP) solar cells have excellent environmental stability. However, the power conversion efficiency (PCE) of RPP cells remains inferior to 3D perovskite‐based cells. Herein, 2D (CH₃(CH₂)₃NH₃)₂(CH₃NH₃)_n?1Pb_nI_3n+1 perovskite cells with different numbers of [PbI₆]^4? sheets (n = 2–4) are analyzed. Photoluminescence quantum yield (PLQY) measurements show that nonradiative open‐circuit voltage (V_OC) losses outweigh radiative losses in materials with n > 2. The n = 3 and n = 4 films exhibit a higher PLQY than the standard 3D methylammonium lead iodide perovskite although this is accompanied by increased interfacial recombination at the top perovskite/C₆₀ interface. This tradeoff results in a similar PLQY in all devices, including the n = 2 system where the perovskite bulk dominates the recombination properties of the cell. In most cases the quasi‐Fermi level splitting matches the device V_OC within 20 meV, which indicates minimal recombination losses at the metal contacts. The results show that poor charge transport rather than exciton dissociation is the primary reason for the reduction in fill factor of the RPP devices. Optimized n = 4 RPP solar cells had PCEs of 13% with significant potential for further improvements.     

Graded Heterojunction Engineering for Hole‐Conductor‐Free Perovskite Solar Cells with High Hole Extraction Efficiency and Conductivity

Despite great progress in the photovoltaic conversion efficiency (PCE) of inorganic–organic hybrid perovskite solar cells (PSCs), the large‐scale application of PSCs still faces serious challenges due to the poor‐stability and high‐cost of the spiro‐OMeTAD hole transport layer (HTL). It is of great fundamental importance to rationally address the issues of hole extraction and transfer arising from HTL‐free PSCs. Herein, a brand‐new PSC architecture is designed by introducing multigraded‐heterojunction (GHJ) inorganic perovskite CsPbBr_x I_3?x layers as an efficient HTL. The grade adjustment can be achieved by precisely tuning the halide proportion and distribution in the CsPbBr_x I_3?x film to reach an optimal energy alignment of the valance and conduction band between MAPbI₃ and CsPbBr_x I_3?x . The CsPbBr_x I_3?x GHJ as an efficient HTL can induce an electric field where a valance/conduction band edge is leveraged to bend at the heterojunction interface, boosting the interfacial electron–hole splitting and photoelectron extraction. The GHJ architecture enhances the hole extraction and conduction efficiency from the MAPbI₃ to the counter electrode, decreases the recombination loss during the hole transfer, and benefits in increasing the open‐circuit voltage. The optimized HTL‐free PCS based on the GHJ architecture demonstrates an outstanding thermal stability and a significantly improved PCE of 11.33%, nearly 40% increase compared with 8.16% for pure HTL‐free devices.     

Achieving Fast Charge Separation and Low Nonradiative Recombination Loss by Rational Fluorination for High‐Efficiency Polymer Solar Cells

Four low‐cost copolymer donors of poly(thiophene‐quinoxaline) (PTQ) derivatives are demonstrated with different fluorine substitution forms to investigate the effect of fluorination forms on charge separation and voltage loss (V_loss) of the polymer solar cells (PSCs) with the PTQ derivatives as donor and a A–DA'D–A‐structured molecule Y6 as acceptor. The four PTQ derivatives are PTQ7 without fluorination, PTQ8 with bifluorine substituents on its thiophene D‐unit, PTQ9, and PTQ10 with monofluorine and bifluorine substituents on their quinoxaline A‐unit respectively. The PTQ8‐ based PSC demonstrates a low power conversion efficiency (PCE) of 0.90% due to the mismatch in the highest occupied molecular orbital (HOMO) energy levels alignment between the donor and acceptor. In contrast, the devices based on PTQ9 and PTQ10 show enhanced charge‐separation behavior and gradually reduced V_loss, due to the gradually reduced nonradiative recombination loss in comparison with the PTQ7‐based device. As a result, the PTQ10‐based PSC demonstrates an impressive PCE of 16.21% with high open‐circuit voltage and large short‐circuit current density simultaneously, and its V_loss is reduced to 0.549 V. The results indicate that rational fluorination of the polymer donors is a feasible method to achieve fast charge separation and low V_loss simultaneously in the PSCs.     

High‐Performance Inverted Planar Perovskite Solar Cells Enhanced by Thickness Tuning of New Dopant‐Free Hole Transporting Layer

A new hole transporting material (HTM) named DMZ is synthesized and employed as a dopant‐free HTM in inverted planar perovskite solar cells (PSCs). Systematic studies demonstrate that the thickness of the hole transporting layer can effectively enhance the morphology and crystallinity of the perovskite layer, leading to low series resistance and less defects in the crystal. As a result, the champion power conversion efficiency (PCE) of 18.61% with J_SC = 22.62 mA cm^?2, V_OC = 1.02 V, and FF = 81.05% (an average one is 17.62%) is achieved with a thickness of ≈13 nm of DMZ (2 mg mL^?1) under standard global AM 1.5 illumination, which is ≈1.5 times higher than that of devices based on poly(3,4‐ethylenedioxythiophene)/poly(styrene sulfonic acid) (PEDOT:PSS). More importantly, the devices based on DMZ exhibit a much better stability (90% of maximum PCE retained after more than 556 h in air (relative humidity ≈ 45%–50%) without any encapsulation) than that of devices based on PEDOT:PSS (only 36% of initial PCE retained after 77 h in same conditions). Therefore, the cost‐effective and facile material named DMZ offers an appealing alternative to PEDOT:PSS or polytriarylamine for highly efficient and stable inverted planar PSCs.     

Defect‐Engineering‐Enabled High‐Efficiency All‐Inorganic Perovskite Solar Cells

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.     

Thermally Stable MAPbI3 Perovskite Solar Cells with Efficiency of 19.19% and Area over 1 cm2 achieved by Additive Engineering

Solution‐processed perovskite (PSC) solar cells have achieved extremely high power conversion efficiencies (PCEs) over 20%, but practical application of this photovoltaic technology requires further advancements on both long‐term stability and large‐area device demonstration. Here, an additive‐engineering strategy is developed to realize a facile and convenient fabrication method of large‐area uniform perovskite films composed of large crystal size and low density of defects. The high crystalline quality of the perovskite is found to simultaneously enhance the PCE and the durability of PSCs. By using the simple and widely used methylammonium lead iodide (MAPbI₃), a certified PCE of 19.19% is achieved for devices with an aperture area of 1.025 cm², and the high‐performing devices can sustain over 80% of the initial PCE after 500 h of thermal aging at 85 °C, which are among the best results of MAPbI₃‐based PSCs so far.     

Fine‐Tuning of Molecular Packing and Energy Level through Methyl Substitution Enabling Excellent Small Molecule Acceptors for Nonfullerene Polymer Solar Cells with Efficiency up to 12.54%

A novel small molecule acceptor MeIC with a methylated end‐capping group is developed. Compared to unmethylated counterparts (ITCPTC), MeIC exhibits a higher lowest unoccupied molecular orbital (LUMO) level value, tighter molecular packing, better crystallites quality, and stronger absorption in the range of 520–740 nm. The MeIC‐based polymer solar cells (PSCs) with J71 as donor, achieve high power conversion efficiency (PCE), up to 12.54% with a short‐circuit current (J_SC) of 18.41 mA cm^?2, significantly higher than that of the device based on J71:ITCPTC (11.63% with a J_SC of 17.52 mA cm^?2). The higher J_SC of the PSC based on J71:MeIC can be attributed to more balanced μ_h/μ_e, higher charge dissociation and charge collection efficiency, better molecular packing, and more proper phase separation features as indicated by grazing incident X‐ray diffraction and resonant soft X‐ray scattering results. It is worth mentioning that the as‐cast PSCs based on MeIC also yield a high PCE of 11.26%, which is among the highest value for the as‐cast nonfullerene PSCs so far. Such a small modification that leads to so significant an improvement of the photovoltaic performance is a quite exciting finding, shining a light on the molecular design of the nonfullerene acceptors.     

Fluorinated Low‐Dimensional Ruddlesden–Popper Perovskite Solar Cells with over 17% Power Conversion Efficiency and Improved Stability

Low‐dimensional Ruddlesden–Popper perovskites (RPPs) exhibit excellent stability in comparison with 3D perovskites; however, the relatively low power conversion efficiency (PCE) limits their future application. In this work, a new fluorine‐substituted phenylethlammonium (PEA) cation is developed as a spacer to fabricate quasi‐2D (4FPEA)₂(MA)₄Pb₅I₁₆ (n = 5) perovskite solar cells. The champion device exhibits a remarkable PCE of 17.3% with a J_sc of 19.00 mA cm^?2, a V_oc of 1.16 V, and a fill factor (FF) of 79%, which are among the best results for low‐dimensional RPP solar cells (n ≤ 5). The enhanced device performance can be attributed as follows: first, the strong dipole field induced by the 4‐fluoro‐phenethylammonium (4FPEA) organic spacer facilitates charge dissociation. Second, fluorinated RPP crystals preferentially grow along the vertical direction, and form a phase distribution with the increasing n number from bottom to the top surface, resulting in efficient charge transport. Third, 4FPEA‐based RPP films exhibit higher film crystallinity, enlarged grain size, and reduced trap‐state density. Lastly, the unsealed fluorinated RPP devices demonstrate superior humidity and thermal stability. Therefore, the fluorination of the long‐chain organic cations provides a feasible approach for simultaneously improving the efficiency and stability of low‐dimensional RPP solar cells.     

Infrared Solution‐Processed Quantum Dot Solar Cells Reaching External Quantum Efficiency of 80% at 1.35 µm and Jsc in Excess of 34 mA cm−2

Developing low‐cost photovoltaic absorbers that can harvest the short‐wave infrared (SWIR) part of the solar spectrum, which remains unharnessed by current Si‐based and perovskite photovoltaic technologies, is a prerequisite for making high‐efficiency, low‐cost tandem solar cells. Here, infrared PbS colloidal quantum dot (CQD) solar cells employing a hybrid inorganic–organic ligand exchange process that results in an external quantum efficiency of 80% at 1.35 µm are reported, leading to a short‐circuit current density of 34 mA cm^?2 and a power conversion efficiency (PCE) up to 7.9%, which is a current record for SWIR CQD solar cells. When this cell is placed at the back of an MAPbI₃ perovskite film, it delivers an extra 3.3% PCE by harnessing light beyond 750 nm.     

In Situ Real‐Time Study of the Dynamic Formation and Conversion Processes of Metal Halide Perovskite Films

Metal halide perovskite solar cells (PSCs) have advanced to the forefront of solution‐processed photovoltaic techniques and made stunning progress in power conversion efficiency (PCE). Further improvements in device performances rely on perfecting the structure and morphology of perovskite films. However, undesirable defects such as pinholes and grain boundaries are often created in film preparations due to lack of knowledge of the precise reaction mechanism. Here, in situ grazing‐incidence X‐ray diffraction (GI‐XRD) investigations are performed, facilitated by other techniques, on the formation of the widely adopted MAPbI₃ (MA = methylammonium) perovskite films from their intermediate adduct (IA) phases. The influences of solvent vapor atmospheres on MAPbI₃ films are also systematically investigated, where the dynamic conversion processes between different phases are visualized in real time. Further in situ GI‐XRD and infrared spectroscopy measurements reveal that the IA phases contain both N,N‐dimethylformamide and dimethyl sulfoxide (DMSO) as coordinating molecules. By tuning the DMSO concentration in perovskite precursors, the ideal perovskite film is formed and the best PCE is achieved for the planar MAPbI₃‐based PSCs. These findings highlight the role of IA phases and the effect of solvent atmospheres on the quality of perovskite films, providing direct insights into their growth mechanism.     

The Role of Rubidium in Multiple‐Cation‐Based High‐Efficiency Perovskite Solar Cells

Perovskite solar cells (PSCs) based on cesium (Cs)‐ and rubidium (Rb)‐containing perovskite films show highly reproducible performance; however, a fundamental understanding of these systems is still emerging. Herein, this study has systematically investigated the role of Cs and Rb cations in complete devices by examining the transport and recombination processes using current–voltage characteristics and impedance spectroscopy in the dark. As the credibility of these measurements depends on the performance of devices, this study has chosen two different PSCs, (MAFACs)Pb(IBr)₃ (MA = CH₃NH₃⁺, FA = CH(NH₂)₂⁺) and (MAFACsRb)Pb(IBr)₃, yielding impressive performances of 19.5% and 21.1%, respectively. From detailed studies, this study surmises that the confluence of the low trap‐assisted charge‐carrier recombination, low resistance offered to holes at the perovskite/2,2′,7,7′‐tetrakis(N,N‐di‐p‐methoxyphenylamine)‐9,9‐spirobifluorene interface with a low series resistance (R_s), and low capacitance leads to the realization of higher performance when an extra Rb cation is incorporated into the absorber films. This study provides a thorough understanding of the impact of inorganic cations on the properties and performance of highly efficient devices, and also highlights new strategies to fabricate efficient multiple‐cation‐based PSCs.     

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.     

Improved Performance of All‐Polymer Solar Cells Enabled by Naphthodiperylenetetraimide‐Based Polymer Acceptor

A new polymer acceptor, naphthodiperylenetetraimide‐vinylene (NDP‐V), featuring a backbone of altenating naphthodiperylenetetraimide and vinylene units is designed and applied in all‐polymer solar cells (all‐PSCs). With this polymer acceptor, a new record power‐conversion efficiencies (PCE) of 8.59% has been achieved for all‐PSCs. The design principle of NDP‐V is to reduce the conformational disorder in the backbone of a previously developed high‐performance acceptor, PDI‐V, a perylenediimide‐vinylene polymer. The chemical modifications result in favorable changes to the molecular packing behaviors of the acceptor and improved morphology of the donor–acceptor (PTB7‐Th:NDP‐V) blend, which is evidenced by the enhanced hole and electron transport abilities of the active layer. Moreover, the stronger absorption of NDP‐V in the shorter‐wavelength range offers a better complement to the donor. All these factors contribute to a short‐circuit current density (J _sc) of 17.07 mA cm^?2. With a fill factor (FF) of 0.67, an average PCE of 8.48% is obtained, representing the highest value thus far reported for all‐PSCs.     

Efficient Perovskite Solar Cells Fabricated Through CsCl‐Enhanced PbI2 Precursor via Sequential Deposition

The fabrication of high‐quality perovskite film highly relies on chemical composition and the synthesis method of perovskite. So far, sequentially deposited MA_0.03FA_0.97Pb(I_0.97Br_0.03)₃ polycrystalline film is adopted to produce high‐performance perovskite solar cells with record power conversion efficiency (PCE). Fewer grain boundaries and incorporation of inorganic cation (e.g., cesium) would further increase device performance via sequential deposition. Here, cesium chloride (CsCl) is introduced into lead iodide (PbI₂) precursor solution that beneficially modulates the property of PbI₂ film, leading to larger grains with cesium incorporation in the resulting perovskite film. The enlarged crystal grains originate from a slower nucleation process for CsCl‐containing PbI₂ film when reacting with formamidine iodide, confirmed by in situ confocal photoluminescence imaging. Photovoltaic devices based on CsCl‐containing PbI₂ film demonstrate a higher averaging efficiency of 21.3% than 20.3% of the devices without CsCl additives for reverse scan. More importantly, the device stability is improved by CsCl additives that retain over 90% of their initial PCE value after 4000 min tracking at maximum power point under 1‐sun illumination. This work paves a way to further improve the photovoltaic performance of mixed‐cation‐halide perovskite solar cells via a sequential deposition method.     

Merits and Challenges of Ruddlesden–Popper Soft Halide Perovskites in Electro‐Optics and Optoelectronics

Following the rejuvenation of 3D organic–inorganic hybrid perovskites, like CH₃NH₃PbI₃, (quasi)‐2D Ruddlesden–Popper soft halide perovskites R₂A_n?1Pb_nX_3n+1 have recently become another focus in the optoelectronic and photovoltaic device community. Although quasi‐2D perovskites were first introduced to stabilize optoelectronic/photovoltaic devices against moisture, more interesting properties and device applications, such as solar cells, light‐emitting diodes, white‐light emitters, lasers, and polaritonic emission, have followed. While delicate engineering design has pushed the performance of various devices forward remarkably, understanding of the fundamental properties, especially the charge‐transfer process, electron–phonon interactions, and the growth mechanism in (quasi)‐2D halide perovskites, remains limited and even controversial. Here, after reviewing the current understanding and the nexus between optoelectronic/photovoltaic properties of 2D and 3D halide perovskites, the growth mechanisms, charge‐transfer processes, vibrational properties, and electron–phonon interactions of soft halide perovskites, mainly in quasi‐2D systems, are discussed. It is suggested that single‐crystal‐based studies are needed to deepen the understanding of the aforementioned fundamental properties, and will eventually contribute to device performance.     

Reducing Hysteresis and Enhancing Performance of Perovskite Solar Cells Using Low‐Temperature Processed Y‐Doped SnO2 Nanosheets as Electron Selective Layers

Despite the rapid increase of efficiency, perovskite solar cells (PSCs) still face some challenges, one of which is the current–voltage hysteresis. Herein, it is reported that yttrium‐doped tin dioxide (Y‐SnO₂) electron selective layer (ESL) synthesized by an in situ hydrothermal growth process at 95 °C can significantly reduce the hysteresis and improve the performance of PSCs. Comparison studies reveal two main effects of Y doping of SnO₂ ESLs: (1) it promotes the formation of well‐aligned and more homogeneous distribution of SnO₂ nanosheet arrays (NSAs), which allows better perovskite infiltration, better contacts of perovskite with SnO₂ nanosheets, and improves electron transfer from perovskite to ESL; (2) it enlarges the band gap and upshifts the band energy levels, resulting in better energy level alignment with perovskite and reduced charge recombination at NSA/perovskite interfaces. As a result, PSCs using Y‐SnO₂ NSA ESLs exhibit much less hysteresis and better performance compared with the cells using pristine SnO₂ NSA ESLs. The champion cell using Y‐SnO₂ NSA ESL achieves a photovoltaic conversion efficiency of 17.29% (16.97%) when measured under reverse (forward) voltage scanning and a steady‐state efficiency of 16.25%. The results suggest that low‐temperature hydrothermal‐synthesized Y‐SnO₂ NSA is a promising ESL for fabricating efficient and hysteresis‐less PSC.     

High‐Performance Additive‐/Post‐Treatment‐Free Nonfullerene Polymer Solar Cells via Tuning Molecular Weight of Conjugated Polymers

In recent years, rapid advances are achieved in polymer solar cells (PSCs) using nonfullerene small molecular acceptors. However, no research disclosing the influence of molecular weight (M_n) of conjugated polymer on the nonfullerene device performance is reported. In this work, a series of polymers with different M_ns are synthesized to systematically investigate the connection between M_n and performance of nonfullerene devices for the first time. It is found that the device performance improves substantially as the M_n increases from 12 to 38 kDa and a power conversion efficiency (PCE) as high as 10.5% is realized. It has to be noted this PCE is achieved without using any additives and post‐treatments, which is among the top efficiencies of additive‐ and post‐treatment‐free PSCs. Most importantly, the variation trend of the optimal active layer thickness and morphology is significantly different from the device with fullerene as acceptor. The findings clarify the effect of M_n on the performance of nonfullerene PSCs, which would benefit further efficiency improvement of nonfullerene PSCs.