Yingzhi Jin

A new asymmetric, terminally tetrafluorinated nonfullerene acceptor, namely ITIF, was prepared for ternary solar cells based on PBDB‐T:ITIF:ITIC blends. Owing to the unique structure, ITIF is promised to work efficiently in ternary blends, simultaneously boosting the devices performance parameters. Therefore, the power conversion efficiencies of the ternary solar cells are boosted from 9.2% to 10.5%.

Abstract

Fabricating ternary solar cells is a pivotal strategy to improve the power conversion efficiencies (PCEs) of organic photovoltaic devices. However, it is still a challenge to simultaneously improve the performance parameters of ternary devices. Therefore, the third ingredient in ternary blends should be precisely designed or selected. Herein, a new medium‐bandgap small‐molecule acceptor, namely, 3,9‐bis(2‐methylene‐(3‐(1‐(3,5‐dimethylphenyl)‐1cyanomethylene)indanone))‐5,5,11,11‐tetrakis‐(4‐hexylphenyl)dithieno[2,3‐d:2′,3′‐d′]‐sindaceno[1,2‐b:5,6‐b′]dithiophene (ITIF), is synthesized by end‐capping with a new fluorinated, asymmetric terminal group, (Z)‐2‐(3,5‐difluorophenyl)‐2‐(3‐oxo‐2,3‐dihydro‐1H‐inden‐1‐ylidene) acetonitrile. Replacing the CN substituent with the asymmetric 3,5‐difluorophenyl substituent obviously up‐shifts the lowest unoccupied molecular orbital (LUMO) level of ITIF to −3.78 eV, enlarges the bandgap to 1.82 eV, and improves the absorption coefficient to ≈50% higher than that of 3,9‐bis(2‐methylene‐(3‐(1,1‐dicyanomethylene)indanone))‐5,5,11,11‐tetrakis‐(4‐hexylphenyl)dithieno[2,3‐d:2′,3′‐d′]‐sindaceno[1,2‐b:5,6‐b′]dithiophene (ITIC). Due to the similar structures, ITIF and ITIC can combine as an alloyed acceptor, which makes it convenient to tune the morphology and optical and electrochemical properties of ternary blends. The enhanced absorption coefficient of ITIF and the rapid fluorescence resonance energy transfer from ITIF to ITIC remarkably improve the absorption of the ternary blend film, hence compensating for the external quantum efficiency (EQE) curves. When ITIF is introduced into ternary solar cells based on 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):ITIF:ITIC blends, the PCEs of the ternary devices are increased from 9.2% to 10.5%, and the short‐circuit currents, open‐circuit voltages, and fill factors are simultaneously improved.

An effective general methodology to utilize triplet excitons to contribute to light amplification with excellent electrical performance is presented. The triplet energy is managed by converting triplet excitons to singlet excitons via Förster energy transfer. This methodology is believed to be beneficial for addressing the challenges toward attempting electrically driven organic semiconductor laser diodes.

Abstract

Organic semiconductor lasers (OSLs) have emerged as particularly challenging. One of the major issues preventing the successful realization of lasing from organic emitters under electrically pumped conditions is the inevitable population of triplet excitons. Herein, a novel concept is presented to construct triplet–singlet guest–host gain systems with incorporating iridium complexes as the triplet sensitizers and a fluorescent conjugated polymer as the gain media to achieve light amplification. The direct triplet–singlet energy transfer process is confirmed by photoluminescence excitation spectra, photoinduced absorption spectroscopy, and fluorescence transients of the blend samples. Successful light amplification with a threefold lower amplified spontaneous emission threshold and much better lasing performance is demonstrated for the resulting triplet–singlet guest–host system as compared with the corresponding gain system without triplet sensitizers. Moreover, under electrically driven conditions, the fluorescent organic light‐emitting diodes (OLEDs) based on the triplet–singlet guest–host systems with “triplet sensitizers” exhibit enhanced electrical performance relative to those without. The work suggests an effective general methodology to utilize both the singlet and triplet excitons to contribute to the light amplification with excellent electrical performance in OLEDs, opening prospects toward attempting electrically pumped OSLs.

A novel wide‐bandgap nonfullerene acceptor TfIF‐4FIC is synthesized. PBDB‐T‐2F:TfIF‐4FIC‐based organic solar cell acquires a power conversion efficiency (PCE) of 13.1%, a high open‐circuit voltage of 0.98 V, which is the best performed device with bandgap larger than 1.60 eV. When using PBDB‐T‐2F:TfIF‐4FIC as front cell and PTB7‐Th:PCDTBT:IEICO‐4F as back cell to construct tandem device, PCE of 15% is achieved.

Abstract

A tandem organic solar cell (OSC) is a valid structure to widen the photon response range and suppress the transmission loss and thermalization loss. In the past few years, the development of low‐bandgap materials with broad absorption in long‐wavelength region for back subcells has attracted considerable attention. However, wide‐bandgap materials for front cells that have both high short‐circuit current density (J _SC) and open‐circuit voltage (V _OC) are scarce. In this work, a new fluorine‐substituted wide‐bandgap small molecule nonfullerene acceptor TfIF‐4FIC is reported, which has an optical bandgap of 1.61 eV. When PBDB‐T‐2F is selected as the donor, the device offers an extremely high V _OC of 0.98 V, a high J _SC of 17.6 mA cm⁻², and a power conversion efficiency of 13.1%. This is the best performing acceptor with such a wide bandgap. More importantly, the energy loss in this combination is 0.63 eV. These properties ensure that PBDB‐T‐2F:TfIF‐4FIC is an ideal candidate for the fabrication of tandem OSCs. When PBDB‐T‐2F:TfIF‐4FIC and PTB7‐Th:PCDTBT:IEICO‐4F are used as the front cell and the back cell to construct tandem solar cells, a PCE of 15% is obtained, which is one of best results reported to date in the field of organic solar cells.

Nonfullerene‐based small‐molecule organic solar cells with a new record efficiency of 12.08% are achieved by first incorporation of near‐infrared absorbing molecules and by tuning the sequentially evolved crystalline morphology. The improved crystallinity of both donor and acceptor materials facilitates the formation of multilength scale morphologies, which further enhance charge mobility and extraction, and reduce the nongeminate recombination.

Abstract

In this paper, two near‐infrared absorbing molecules are successfully incorporated into nonfullerene‐based small‐molecule organic solar cells (NFSM‐OSCs) to achieve a very high power conversion efficiency (PCE) of 12.08%. This is achieved by tuning the sequentially evolved crystalline morphology through combined solvent additive and solvent vapor annealing, which mainly work on ZnP‐TBO and 6TIC, respectively. It not only helps improve the crystallinity of the ZnP‐TBO and 6TIC blend, but also forms multilength scale morphology to enhance charge mobility and charge extraction. Moreover, it simultaneously reduces the nongeminate recombination by effective charge delocalization. The resultant device performance shows remarkably enhanced fill factor and J _sc. These result in a very respectable PCE, which is the highest among all NFSM‐OSCs and all small‐molecule binary solar cells reported so far.

An effective but simple approach to rationally tune the crystallinity and miscibility of small‐molecular acceptors is reported. With a phenyl introduced at the tail of alkyl side chains, the morphology and molecular orientations of heterojunction are greatly improved. Outstanding efficiencies of 13.23% and 14.04% are detected from the as‐cast and annealed devices, promoted by the fairly high fill factors.

Abstract

Research on fused‐ring small‐molecular‐acceptors (SMAs) has deeply advanced the development of organic solar cells (OSCs). Compared to fruitful studies of ladder‐type cores and end‐caps of SMAs, the exploration of side chains is monotonous. The widely utilized alkyl and aryl side chains usually produce a conflicting association between SMAs' crystallinity and miscibility. Herein, a fresh idea about the modification of side chains is reported to explore the subtle balance between the crystallinity and miscibility. Specifically, a phenyl is introduced to the tail of the alkyl side chain whereby a new acceptor IDIC‐C4Ph is reported. Moderately weakened crystallinity is observed, while maintaining preferred absorption profiles and face‐on orientations. Concurrently, remarkably improved heterojunction morphologies and stacking orientations are detected. PBDB‐T:IDIC‐C4Ph devices exhibit greater efficiency of 11.50% than devices from alky and aryl modified acceptors. Notably, the as‐cast OSCs of PBDB‐TF:IDIC‐C4Ph reveal outstanding FF over 76% with the best efficiency up to 13.23%. The annealed devices reveal further increased efficiency exceeding 14% with the state of the art FF of 78.32%. Overall, an effective but easily navigable approach is demonstrated to modulate the crystallinity of SMAs toward synergistically improved morphologies and molecular orientations of bulk heterojunction enabling highly efficient OSCs.

A tandem organic solar cell is fabricated employing subcells with the same donor PBDB‐T and two acceptors F‐M and NNBDT with complementary absorptions. A power conversion efficiency of 14.52% is achieved 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.

Abstract

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.

Pure PEDOT:PSS hydrogels

Pure PEDOT:PSS hydrogels, Published online: 05 March 2019; doi:10.1038/s41467-019-09003-5

Intrinsic measurements of exciton transport in photovoltaic cells

Intrinsic measurements of exciton transport in photovoltaic cells, Published online: 11 March 2019; doi:10.1038/s41467-019-09062-8

Nonfullerene acceptors (NFAs) provide an exciting prospect for organic solar cells; however, their stability still lacks fundamental understanding. The promising high‐efficiency NFAs, IDTBR and IDFBR, show a three‐phase degradation mechanism, which involves a strong initial molecular conformational change prior to photodegradation under light and oxygen stress, indicating the important role of NFA molecular structure in solar cell stability.

Abstract

Nonfullerene acceptors (NFAs) dominate organic photovoltaic (OPV) research due to their promising efficiencies and stabilities. However, there is very little investigation into the molecular processes of degradation, which is critical to guiding design of novel NFAs for long‐lived, commercially viable OPVs. Here, the important role of molecular structure and conformation in NFA photostability in air is investigated by comparing structurally similar but conformationally different promising NFAs: planar O‐IDTBR and nonplanar O‐IDFBR. A three‐phase degradation process is identified: i) initial photoinduced conformational change (i.e., torsion about the core–benzothiadiazole dihedral), induced by noncovalent interactions with environmental molecules, ii) followed by photo‐oxidation and fragmentation, leading to chromophore bleaching and degradation product formation, and iii) finally complete chromophore bleaching. Initial conformational change is a critical prerequisite for further degradation, providing fundamental understanding of the relative stability of IDTBR and IDFBR, where the already twisted IDFBR is more prone to degradation. When blended with the donor polymer poly(3‐hexylthiophene), both NFAs exhibit improved photostability while the photostability of the polymer itself is significantly reduced by the more miscible twisted NFA. The findings elucidate the important role of NFA molecular structure in photostability of OPV systems, and provide vital insights into molecular design rules for intrinsically photostable NFAs.

A very simple rod‐shaped bithiophene‐based small molecule, T2‐ORH, is synthesized in only two steps to obtain a nonfullerene acceptor for use in efficient organic photovoltaic cells. The additive‐free inverted PTB7‐Th:T2‐ORH single‐junction device exhibits a power conversion efficiency of 9.33%, with a remarkably low E _loss of 0.51 eV due to a smooth homogeneous film morphology and vertical and parallel charge transport.

Abstract

The introduction of rigid and extended ladder‐type fused‐ring cores, such as indacenodithiophene, has enabled the synthesis of a variety of nonfullerene small molecules for use as electron acceptors in high‐performance organic photovoltaic cells. Contrasting with recent trends, a very simple‐structured nonfullerene acceptor (NFA), T2‐ORH, consisting of a bithiophene core and octyl‐substituted rhodanine ends, is synthesized in two steps from inexpensive commercially available raw materials. Its relatively short π‐conjugation results in a wide bandgap and a blue‐shifted UV–vis absorption profile complementary to those of poly[4,8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)benzo[1,2‐b:4,5‐b′]dithiophene‐co‐3‐fluorothieno[3,4‐b]thiophene‐2‐carboxylate] (PTB7‐Th). Despite a sufficient offset between T2‐ORH and PTB7‐Th, the lowest unoccupied molecular orbital (LUMO) energy level of T2‐ORH is still higher than the LUMOs of other NFAs (e.g., ITIC). Therefore, the PTB7‐Th:T2‐ORH blend film exhibits an efficiency of 9.33% with a high open‐circuit voltage of 1.07 V and a short‐circuit current of 14.72 mA cm⁻² in an additive‐free single‐junction cell. Importantly, the optimized device displays a remarkably low energy loss of 0.51 eV, in which bimolecular and monomolecular charge recombination is effectively suppressed by solvent vapor annealing treatment. The blend film has a very smooth and homogeneous morphology, providing both vertical and parallel charge transport in the devices.

Zwitterions have emerged as a novel class of materials for organic/perovskite solar cells, light‐emitting devices, and lithium ion batteries. These materials have demonstrated tremendous performance in the enabling of highly efficient devices. The mechanism of action, structure–property relationships, and more device applications of zwitterionic materials must be explored to exploit the potential of these materials to the full.

Abstract

Zwitterions, a class of materials that contain covalently bonded cations and anions, have been extensively studied in the past decades owing to their special features, such as excellent solubility in polar solvents, for solution processing and dipole formation for the transfer of carriers and ions. Recently, zwitterions have been developed as electrode modifiers for organic solar cells (OSCs), perovskite solar cells (PVSCs), and organic light‐emitting devices (OLEDs), as well as electrolyte additives for lithium ion batteries (LIBs). With the rapid advances of zwitterionic materials, high‐performance devices have been constructed with enhanced efficiencies by introducing them as interface layers and electrolyte additives. In this review, recent progress in OSCs, PVSCs, OLEDs, and LIBs by using zwitterions is highlighted. The authors also elaborate the role of various zwitterionic materials as interfacial layers and additives for highly efficient OSCs, PVSCs, OLEDs, and LIBs. This article presents an overview of device performance of zwitterionic materials. The structure–property relationship is also discussed. Finally, the prospects of zwitterion materials are also addressed.

To predict the open‐circuit voltage (V _oc) of polymer–fullerene solar cells, three independent methods, square‐wave voltammetry (SWV), ultraviolet photoelectron spectroscopy, and density functional theory, are compared. For 19 diketopyrrolopyrrole polymers, SWV gives the best correlation. Remarkably, the slope of V _oc with the blend's electrochemical gap is less than unity and possible reasons for this result are discussed.

Abstract

For 19 diketopyrrolopyrrole polymers, the highest occupied molecular orbital (HOMO) energies are determined from i) the oxidation potential with square‐wave voltammetry (SWV), ii) the ionization potential using ultraviolet photoelectron spectroscopy (UPS), and iii) density functional theory (DFT) calculations. The SWV HOMO energies show an excellent linear correlation with the open‐circuit voltage (V _oc) of optimized solar cells in which the polymers form blends with a fullerene acceptor ([6,6]‐phenyl‐C₆₁‐butyl acid methyl ester or [6,6]‐phenyl‐C₇₁‐butyl acid methyl ester). Remarkably, the slope of the best linear fit is 0.75 ± 0.04, i.e., significantly less than unity. A weaker correlation with V _oc is found for the HOMO energies obtained from UPS and DFT. Within the experimental error, the SWV and UPS data are correlated with a slope close to unity. The results show that electrochemically determined oxidation potentials provide an excellent method for predicting the V _oc of bulk heterojunction solar cells, with absolute deviations less than 0.1 V.

The ITC‐2Cl‐based device yields an excellent power conversion efficiency of 13.6% with a low E _loss of 0.67 eV, which is superior to those of the devices based on ITCPTC, IT‐4F, and IT‐4Cl.

Abstract

Generally, highly efficient organic solar cells require both a high open‐circuit voltage (V _OC) and a high short‐circuit current density (J _SC). Reducing the energy loss (E _loss) is an effective way to achieve a high V _OC without compromising the photocurrent, which is ideal for enhancing the power conversion efficiencies (PCEs). Herein, a new chlorinated nonfullerene acceptor (ITC‐2Cl) with chlorinated thiophene‐fused end groups is developed. In comparison with the unchlorinated counterpart (ITCPTC), the introduction of Cl improves not only the electronic properties by redshifting the absorption spectra and deepening the lowest unoccupied molecular orbital energy levels, but also the molecular packing and thus thin‐film morphology. The PM6:ITC‐2Cl‐based device yields a significantly higher PCE (13.6%) with a lower E _loss (0.67 eV) than the ITCPTC‐based device (PCE of 12.3% with E _loss of 0.70 eV). More importantly, compared to the archetypal nonfullerene acceptors such as IT‐4F (PCE of 12.9% with E _loss of 0.73 eV) and IT‐4Cl (PCE of 12.7% with E _loss of 0.76 eV), the ITC‐2Cl‐based device shows a higher PCE and a lower E _loss. These results demonstrate that the chlorinated thiophene‐fused end group is a promising candidate for a high‐performance nonfullerene acceptors with low energy loss.

Multijunction organic solar cells provide higher power conversion efficiencies than the corresponding single junction solar cells by reducing thermalization and transmission losses and are fabricated by sequential layer deposition from solution. In recent years, important progress has been made in terms of novel materials and device design and the most salient advances are discussed.

Abstract

The efficiency of organic solar cells can benefit from multijunction device architectures, in which energy losses are substantially reduced. Herein, recent developments in the field of solution‐processed multijunction organic solar cells are described. Recently, various strategies have been investigated and implemented to improve the performance of these devices. Next to developing new materials and processing methods for the photoactive and interconnecting layers, specific layers or stacks are designed to increase light absorption and improve the photocurrent by utilizing optical interference effects. These activities have resulted in power conversion efficiencies that approach those of modern thin film photovoltaic technologies. Multijunction cells require more elaborate and intricate characterization procedures to establish their efficiency correctly and a critical view on the results and new insights in this matter are discussed. Application of multijunction cells in photoelectrochemical water splitting and upscaling toward a commercial technology is briefly addressed.

A synergistic effect is proposed by employing a dielectric mirror and a ternary strategy to precisely tune the color perception as well as semitransparent organic solar cell (ST‐OSC) performance. It results in the highest efficiency reported for neutral‐color ST‐OSCs to date.

Abstract

Neutral‐colored semitransparent organic solar cells (ST‐OSCs) have attracted considerable attention owing to their unique application in no‐visual‐obstacle building‐integrated photovoltaics. Toward this promising potential application, a synergistic effect is first proposed by employing a dielectric mirror and ternary photoactive layer with near‐infrared absorption to tune the color perception as well as ST‐OSC performance precisely. As a result, a neutral‐color ST‐OSC with high average transmittance of over 21% is successfully constructed, and a remarkable color‐rendering index approaching 100 and high power conversion efficiency (PCE) of 9.37% are simultaneously achieved. To the best of our knowledge, this is the highest PCE reported for neutral‐color ST‐OSCs to date. Importantly, this synergistic effect is demonstrated to be a universal strategy that is not only suitable for various photoactive layer systems, but can also be implanted in flexible substrate. The resulting neutral‐color flexible ST‐OSCs also show a promising PCE of 8.76%.

The molecular orientation and charge extraction of PEDOT:PSS‐based hole‐transporting layers are effectively modulated through fine tuning of the surface energy by introducing poly(styrene sulfonic acid) sodium salts or nickel formate dihydrate, which boosts the fill factor and eventual efficiency of organic solar cells based on fullerene and nonfullerene acceptors.

Abstract

Interface properties are of critical importance for high‐performance bulk‐heterojunction (BHJ) organic solar cells (OSCs). Here, a universal interface approach to tune the surface free energy (γ_S) of hole‐transporting layers (HTLs) in a wide range through introducing poly(styrene sulfonic acid) sodium salts or nickel formate dihydrate into poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is reported. Based on the optimal γ_S of HTLs and thus improved face‐on molecular ordering in BHJs, enhanced fill factor and power conversion efficiencies in both fullerene and nonfullerene OSCs are achieved, which is attributed to the increased charge carrier mobility and sweepout with reduced recombination. It is found that the face‐on orientation‐preferred BHJs (PBDB‐TF:PC₇₁BM, PBDB‐T:PC₇₁BM, and PBDB‐TF:IT‐4F) favor HTLs with higher γ_S while the edge‐on orientation‐preferred BHJs (PDCDT:PC₇₁BM, P3HT:PC₇₁BM and PDCBT:ITIC) are partial to HTLs with lower γ_S. Based on the surface property–morphology–device performance correlations, a suggestion to select a suitable HTL in terms of γ_S for a specific BHJ with favored molecular arrangement is provided. This work enriches the fundamental understandings on the interface characteristics and morphological control toward high‐efficiency OSCs based on a wide range of BHJ materials.

A facile and eco‐friendly approach is introduced to greatly promote the molecular order of nominally amorphous polymers and thus realize high‐efficiency in sequentially deposited (SD) nonfullerene solar cells. Applying a green solvent, (R)‐(+)‐limonene, enhances the polymer order and yields the best efficiency. Additionally, strong relationships between solvent, interaction parameter, and long period are observed for these new SD devices.

Abstract

Casting of a donor:acceptor bulk‐heterojunction structure from a single ink has been the predominant fabrication method of organic photovoltaics (OPVs). Despite the success of such bulk heterojunctions, the task ofcontrolling the microstructure in a single casting process has been arduous and alternative approaches are desired. To achieve OPVs with a desirable microstructure, a facile and eco‐compatible sequential deposition approach is demonstrated for polymer/small‐molecule pairs. Using a nominally amorphous polymer as the model material, the profound influence of casting solvent is shown on the molecular ordering of the film, and thus the device performance and mesoscale morphology of sequentially deposited OPVs can be tuned. Static and in situ X‐ray scattering indicate that applying (R)‐(+)‐limonene is able to greatly promote the molecular order of weakly crystalline polymers and form the largest domain spacing exclusively, which correlates well with the best efficiency of 12.5% in sequentially deposited devices. The sequentially cast device generally outperforms its control device based on traditional single‐ink bulk‐heterojunction structure. More crucially, a simple polymer:solvent interaction parameter χ is positively correlated with domain spacing in these sequentially deposited devices. These findings shed light on innovative approaches to rationally create environmentally friendly and highly efficient electronics.

Employing an electron‐deficient‐core‐based fused structure instead of a fused donor unit represents a new strategy to adjust the optoelectronic properties of acceptor–donor–acceptor‐type n‐type organic semiconductors. The electron‐deficient‐core based on benzothiadiazole together with dicyanomethylene derivative realizes a low bandgap, high electron mobility, and suitable energy level simultaneously, affording universal and high performances when blending with different donor polymers.

Abstract

Narrow bandgap n‐type organic semiconductors (n‐OS) have attracted great attention in recent years as acceptors in organic solar cells (OSCs), due to their easily tuned absorption and electronic energy levels in comparison with fullerene acceptors. Herein, a new n‐OS acceptor, Y5, with an electron‐deficient‐core‐based fused structure is designed and synthesized, which exhibits a strong absorption in the 600–900 nm region with an extinction coefficient of 1.24 × 10⁵ cm⁻¹, and an electron mobility of 2.11 × 10⁻⁴ cm² V⁻¹ s⁻¹. By blending Y5 with three types of common medium‐bandgap polymers (J61, PBDB‐T, and TTFQx‐T1) as donors, all devices exhibit high short‐circuit current densities over 20 mA cm⁻². As a result, the power conversion efficiency of the Y5‐based OSCs with J61, TTFQx‐T1, and PBDB‐T reaches 11.0%, 13.1%, and 14.1%, respectively. This indicates that Y5 is a universal and highly efficient n‐OS acceptor for applications in organic solar cells.

A highly efficient, stable, and ductile nonfullerene ternary organic solar cell by integrating two polymer donors and one acceptor is achieved. The enhanced performance and stability are mainly attributed to the suppressed crystallization of the nonfullerene acceptor by introducing a stiff donor that shows low miscibility with the acceptor and a slightly higher highest occupied molecular orbital (HOMO) than the host polymer.

Abstract

Organic solar cells (OSCs) are one of the most promising cost‐effective options for utilizing solar energy, and, while the field of OSCs has progressed rapidly in device performance in the past few years, the stability of nonfullerene OSCs has received less attention. Developing devices with both high performance and long‐term stability remains challenging, particularly if the material choice is restricted by roll‐to‐roll and benign solvent processing requirements and desirable mechanical durability. Building upon the ink (toluene:FTAZ:IT‐M) that broke the 10% benchmark when blade‐coated in air, a second donor material (PBDB‐T) is introduced to stabilize and enhance performance with power conversion efficiency over 13% while keeping toluene as the solvent. More importantly, the ternary OSCs exhibit excellent thermal stability and storage stability while retaining high ductility. The excellent performance and stability are mainly attributed to the inhibition of the crystallization of nonfullerene small‐molecular acceptors (SMAs) by introducing a stiff donor that also shows low miscibility with the nonfullerene SMA and a slightly higher highest occupied molecular orbital (HOMO) than the host polymer. The study indicates that improved stability and performance can be achieved in a synergistic way without significant embrittlement, which will accelerate the future development and application of nonfullerene OSCs.