High Performance As-Cast Organic Solar Cells Enabled by a Refined Double-Fibril Network Morphology and Improved Dielectric Constant of Active Layer.

High performance organic solar cells (OSCs) are usually realized by using post-treatment and/or additive, which can induce the formation of metastable morphology, leading to unfavorable device stability. In terms of the industrial production, the development of high efficiency as-cast OSCs is crucially important, but it remains a great challenge to obtain appropriate active layer morphology and high power conversion efficiency (PCE). Here, efficient as-cast OSCs are constructed via introducing a new polymer acceptor PY-TPT with a high dielectric constant into the D18:L8-BO blend to form a double-fibril network morphology. Besides, the incorporation of PY-TPT enables an enhanced dielectric constant and lower exciton binding energy of active layer. Therefore, efficient exciton dissociation and charge transport are realized in D18:L8-BO:PY-TPT-based device, affording a record-high PCE of 18.60% and excellent photostability in absence of post-treatment. Moreover, green solvent-processed devices, thick-film (300 nm) devices, and module (16.60 cm2) are fabricated, which show PCEs of 17.45%, 17.54%, and 13.84%, respectively. This work brings new insight into the construction of efficient as-cast devices, pushing forward the practical application of OSCs.

On the role of asymmetric molecular geometry in high-performance organic solar cells.

Although asymmetric molecular design has been widely demonstrated effective for organic photovoltaics (OPVs), the correlation between asymmetric molecular geometry and their optoelectronic properties is still unclear. To access this issue, we have designed and synthesized several symmetric-asymmetric non-fullerene acceptors (NFAs) pairs with identical physical and optoelectronic properties. Interestingly, we found that the asymmetric NFAs universally exhibited increased open-circuit voltage compared to their symmetric counterparts, due to the reduced non-radiative charge recombination. From our molecular-dynamic simulations, the asymmetric NFA naturally exhibits more diverse molecular interaction patterns at the donor (D):acceptor (A) interface as compared to the symmetric ones, as well as higher D:A interfacial charge-transfer state energy. Moreover, it is observed that the asymmetric structure can effectively suppress triplet state formation. These advantages enable a best efficiency of 18.80%, which is one of the champion results among binary OPVs. Therefore, this work unambiguously demonstrates the unique advantage of asymmetric molecular geometry, unveils the underlying mechanism, and highlights the manipulation of D:A interface as an important consideration for future molecular design.

High-efficiency flexible organic solar cells with a polymer-incorporated pseudo-planar heterojunction.

Organic solar cells (OSCs) are considered as a crucial energy source for flexible and wearable electronics. Pseudo-planar heterojunction (PPHJ) OSCs simplify the solution preparation and morphology control. However, non-halogenated solvent-printed PPHJ often have an undesirable vertical component distribution and insufficient donor/acceptor interfaces. Additionally, the inherent brittleness of non-fullerene small molecule acceptors (NFSMAs) in PPHJ leads to poor flexibility, and the NFSMAs solution shows inadequate viscosity during the printing of acceptor layer. Herein, we propose a novel approach termed polymer-incorporated pseudo-planar heterojunction (PiPPHJ), wherein a small amount of polymer donor is introduced into the NFSMAs layer. Our findings demonstrate that the incorporation of polymer increases the viscosity of acceptor solution, thereby improving the blade-coating processability and overall film quality. Simultaneously, this strategy effectively modulates the vertical component distribution, resulting in more donor/acceptor interfaces and an improved power conversion efficiency of 17.26%. Furthermore, PiPPHJ-based films exhibit superior tensile properties, with a crack onset strain of 12.0%, surpassing PPHJ-based films (9.6%). Consequently, large-area (1 cm2) flexible devices achieve a considerable efficiency of 13.30% and maintain excellent mechanical flexibility with 82% of the initial efficiency after 1000 bending cycles. These findings underscore the significant potential of PiPPHJ-based OSCs in flexible and wearable electronics.

Green-Solvent Processed Blade-Coating Organic Solar Cells with an Efficiency Approaching 19% Enabled by Alkyl-Tailored Acceptors.

Power-conversion-efficiencies (PCEs) of organic solar cells (OSCs) in laboratory, normally processed by spin-coating technology with toxic halogenated solvents, have reached over 19%. However, there is usually a marked PCE drop when the blade-coating and/or green-solvents toward large-scale printing are used instead, which hampers the practical development of OSCs. Here, a new series of N-alkyl-tailored small molecule acceptors named YR-SeNF with a same molecular main backbone are developed by combining selenium-fused central-core and naphthalene-fused end-group. Thanks to the N-alkyl engineering, NIR-absorbing YR-SeNF series show different crystallinity, packing patterns, and miscibility with polymeric donor. The studies exhibit that the molecular packing, crystallinity, and vertical distribution of active layer morphologies are well optimized by introducing newly designed guest acceptor associated with tailored N-alkyl chains, providing the improved charge transfer dynamics and stability for the PM6:L8-BO:YR-SeNF-based OSCs. As a result, a record-high PCE approaching 19% is achieved in the blade-coating OSCs fabricated from a green-solvent o-xylene with high-boiling point. Notably, ternary OSCs offer robust operating stability under maximum-power-point tracking and well-keep > 80% of the initial PCEs for even over 400 h. Our alkyl-tailored guest acceptor strategy provides a unique approach to develop green-solvent and blade-coating processed high-efficiency and operating stable OSCs, which paves a way for industrial development.

Nonhalogenated Dual-Slot-Die Processing Enables High-Efficiency Organic Solar Cells.

Organic solar cells (OSCs) are promising candidates for next-generation photovoltaic technologies, with their power conversion efficiencies (PCEs) reaching 19%. However, the typically used spin-coating method, toxic halogenated processing solvents, and the conventional bulk-heterojunction (BHJ), which causes excessive charge recombination, hamper the commercialization and further efficiency promotion of OSCs. Here, a simple but effective dual-slot-die sequential processing (DSDS) strategy is proposed to address the above issues by achieving a continuous solution supply, avoiding the solubility limit of the nonhalogen solvents, and creating a graded-BHJ morphology. As a result, an excellent PCE of 17.07% is obtained with the device processed with o-xylene in an open-air environment with no post-treatment required, while a PCE of over 14% is preserved in a wide range of active-layer thickness. The unique film-formation mechanism is further identified during the DSDS processing, which suggests the formation of the graded-BHJ morphology by the mutual diffusion between the donor and acceptor and the subsequent progressive aggregation. The graded-BHJ structure leads to improved charge transport, inhibited charge recombination, and thus an excellent PCE. Therefore, the newly developed DSDS approach can effectively contribute to the realm of high-efficiency and eco-friendly OSCs, which can also possibly be generalized to other organic photoelectric devices.

Molecular-Shape-Controlled Nonfused Ring Electron Acceptors for High-Performance Organic Solar Cells with Tunable Phase Morphology.

Two nonfused ring electron acceptors (NFREAs), BTh-OC8-2F and DTh-OC8-2F, with different molecular shapes are designed and synthesized. Both acceptors can form planar molecular shapes by the assistance of S···O intramolecular interactions. Differently, BTh-OC8-2F, with a linear molecular backbone and two trans-arranged side chains at the core unit, exhibits much stronger crystallinity than DTh-OC8-2, with a C-shape molecular shape and two cis-arranged steric side chains at the core unit. Thus, the DTh-OC8-2F based blend film displays a better nanoscale phase separation, more suppressed charge recombination, more efficient exciton dissociation, and lower nonradiative energy loss. Organic solar cells based on DTh-OC8-2F can deliver a power conversion efficiency of 14.13%, which is much higher than BTh-OC8-2F based ones (11.95%) and is also one of the highest values reported for organic solar cells based on NFREAs.

Unraveling the Photovoltaic, Mechanical, and Microstructural Properties and Their Correlations in Simple Poly(3-pentylthiophene) Solar Cells.

The power conversion efficiency of polythiophene organic solar cells is constantly refreshed. Despite the renewed device efficiency, very few efforts have been devoted to understanding how the type of electron acceptor alters the photovoltaic and mechanical properties of these low-cost solar cells. Herein, the authors conduct a thorough investigation of photovoltaic and mechanical characteristics of a simple yet less-explored polythiophene, namely poly(3-pentylthiophene) (P3PT), in three different types of organic solar cells, where ZY-4Cl, PC71 BM, and N2200 are employed as three representative acceptors, respectively. Compared with the reference poly(3-hexylthiophene) (P3HT)-based solar cells, P3PT-based devices, all perform more efficiently. Particularly, the P3PT:ZY-4Cl blend exhibits the highest efficiency (ca. 10%) among the six combinations and outperforms the prior top-performance system P3HT:ZY-4Cl. Furthermore, the blend films based on N2200 exhibit a high crack-onset strain of ∼38% on average, which is approximately 15- and 17-times higher than those of ZY-4Cl and PC71 BM, respectively. The microstructural origins for the above difference are well elucidated by detailed grazing incidence X-ray scattering and microscopy analysis. This work not only underlines the potential of P3PT in prolific solar cell research but also demonstrates the superior tensile properties of polythiophene-based all-polymer blends for the preparation of stretchable solar cells.

Reducing Energy Disorder in Perovskite Solar Cells by Chelation.

In inverted perovskite solar cells (PSCs), the fullerene derivative [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) is a widely used electron transport material. However, a high degree of energy disorder and inadequate passivation of PCBM limit the efficiency of devices, and severe self-aggregation and unstable morphology limit the lifespan of devices. Here, we design a series of fullerene dyads FP-Cn (n = 4, 8, 12) to replace PCBM as an electron transport layer, where [60]fullerene is linked with a terpyridine chelating group via a flexible alkyl chain of different lengths as a spacer. Among three fullerene dyads, FP-C8 shows the most enhanced molecule ordering and adhesion with the perovskite surface due to the balanced decoupling between the chelation effect from terpyridine and the self-assembly of fullerene, leading to lower energy disorder and higher morphological stability relative to PCBM. The FP-C8/C60-based devices using Cs0.05FA0.90MA0.05PbI2.85Br0.15 as a light absorber show a power conversion efficiency of 21.69%, higher than that of PCBM/C60 (20.09%), benefiting from improved electron extraction and transport as well as reduced charge recombination loss. When employing FAPbI3 as a light absorber, the FP-C8/C60-based devices exhibit an efficiency of 23.08%, which is the champion value of inverted PSCs with solution-processed fullerene derivatives. Moreover, the FP-C8/C60-based devices show better moisture and thermal stability than PCBM/C60-based devices and maintain 96% of their original efficiency after 1200 h of operation, while their counterpart PCBM/C60 maintains 60% after 670 h.

Strengthening the Intermolecular Interaction of Prototypical Semicrystalline Conjugated Polymer Enables Improved Photocurrent Generation at the Heterojunction.

The intra and intermolecular interactions (J- and H-type aggregation) in the conjugated polymer films are found to readily facilitate the electron and hole transport, respectively. However, how those different aggregation types influence the photocurrent generation at the heterojunction is still mysterious, especially for the newly developed semicrystalline conjugated polymers. Here, the prototypical copolymer PM6 is used to tune the relative content of aggregation types with various halogen-free processing solvents. Various measurements reveal that the toluene-processed PM6 film exhibits the increased H-aggregates and crystallinity in the π-π stacking direction compared to its o-xylene- and trimethylbenzene (TMB)-processed counterparts. This is partly resulted from the weak steric effect and good solubility in the PM6 solution prepared with toluene, which strengthens the intermolecular interaction of adjacent polymer segments. After analyzing the photovoltaic properties of PM6/Y6 bilayer devices, the faster charge carrier transport, smaller charge recombination, lower energy losses, and interfacial energetic disorder can be observed in the toluene-processed device, leading to the synergistically improved short-circuit current density (JSC ) and open-circuit voltage (VOC ). These findings indicate the control of the molecular packing structure in terms of aggregation types is a powerful strategy to promote the photocurrent generation process at the conjugated polymer-based heterojunction.

Different Morphology Dependence for Efficient Indoor Organic Photovoltaics: The Role of the Leakage Current and Recombination Losses.

Efficient indoor organic photovoltaics (OPVs) have attracted strong attention for their application in indoor electronic devices. However, the route to optimal photoactive film morphology toward high-performance indoor devices has remained obscure. The leakage current dominated by morphology exerts distinguishing influence on the performance under different illuminations. We have demonstrated that morphology reoptimization plays an important role in indoor OPVs, and their optimal structural features are different from what we laid out for outdoor devices. For indoor OPVs, in order to facilitate low leakage current, it is essential to enhance the crystallinity, phase separation, and domain purity, as well as keeping small surface roughness of the active layer. Furthermore, considering the reduced bimolecular recombination at low light intensity, we have shown that PM6:M36-based indoor devices can work effectively with a large ratio of the donor and acceptor. Our work correlating structure-performance relation and the route to optimal morphology outlines the control over device leakage current and recombination losses boosting the progress of efficient indoor OPVs.

Intermolecular Interaction Control Enables Co-optimization of Efficiency, Deformability, Mechanical and Thermal Stability of Stretchable Organic Solar Cells.

Promoting efficiency, deformability, and life expectancy of stretchable organic solar cells (OSCs) have always been key concerns that researchers are committed to solving. However, how to improve them simultaneously remains challenging, as morphology parameters, such as ordered molecular arrangement, beneficial for highly efficient devices actually limits mechanical stability and deformability. In this study, the unfavorable trade-off among these properties has been reconciled in an all-polymer model system utilizing a mechanically deformable guest component. The success of this strategy stems from introducing a highly ductile component without compromising the pristine optimized morphology. Preferable interaction between two donors can maintain the fiber-like structure while enhancing the photocurrent to improve efficiency. Morphology evolution detected via grazing incidence X-ray scattering and in situ UV-vis absorption spectra during stretching have verified the critical role of strengthened interaction on stabilizing morphology against external forces. The strengthened interaction also benefits thermal stability, enabling the ternary films with small efficiency degradation after heating 1500 h under 80 °C. This work highlights the effect of morphology evolution on mechanical stability and provides new insights from the view of intermolecular interaction to fabricate highly efficient, stable, and stretchable/wearable OSCs.

Efficient Ternary Organic Solar Cells with a New Electron Acceptor Based on 3,4-(2,2-Dihexylpropylenedioxy)thiophene.

In this work, a ternary blend strategy based on PBDB-T and two small molecular acceptors (IDTT-OB and IDT-PDOT-C6) is demonstrated to simultaneously improve the photocurrent and reduce the voltage loss in organic solar cells (OSCs). The improved photocurrent is partially due to a broad absorption spectrum of the active layer. In addition, we find that the ternary system possesses a higher degree of crystallinity, smaller domain size, higher domain purity, and higher and more balanced charge-carrier mobilities in comparison with the two corresponding binary systems. The reduced voltage loss in the ternary device is mainly due to a lower energy loss (Eloss) of charge carriers. We achieve a Eloss of only 0.50 eV, which is one of the lowest values reported for the ternary nonfullerene OSCs. Our results have demonstrated that all photovoltaic parameters of ternary OSCs can be simultaneously improved by elaborately selecting the three active layer components.

Noncovalently fused-ring electron acceptors with near-infrared absorption for high-performance organic solar cells.

Non-fullerene fused-ring electron acceptors boost the power conversion efficiency of organic solar cells, but they suffer from high synthetic cost and low yield. Here, we show a series of low-cost noncovalently fused-ring electron acceptors, which consist of a ladder-like core locked by noncovalent sulfur-oxygen interactions and flanked by two dicyanoindanone electron-withdrawing groups. Compared with that of similar but unfused acceptor, the presence of ladder-like structure markedly broadens the absorption to the near-infrared region. In addition, the use of intramolecular noncovalent interactions avoids the tedious synthesis of covalently fused-ring structures and markedly lowers the synthetic cost. The optimized solar cells displayed an outstanding efficiency of 13.24%. More importantly, solar cells based on these acceptors demonstrate very low non-radiative energy losses. This research demonstrates that low-cost noncovalently fused-ring electron acceptors are promising to achieve high-efficiency organic solar cells.

Single-Junction Polymer Solar Cells with 16.35% Efficiency Enabled by a Platinum(II) Complexation Strategy.

A new strategy of platinum(II) complexation is developed to regulate the crystallinity and molecular packing of polynitrogen heterocyclic polymers, optimize the morphology of the active blends, and improve the efficiency of the resulting nonfullerene polymer solar cells (NF-PSCs). The newly designed s-tetrazine (s-TZ)-containing copolymer of PSFTZ (4,8-bis(5-((2-butyloctyl)thio)-4-fluorothiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene-alt-3,6-bis(4-octylthiophen-2-yl)-1,2,4,5-tetrazine) has a strong aggregation property, which results in serious phase separation and large domains when blending with Y6 ((2,2'-((2Z,2'Z)-((12,13-bis(2-ethylhexyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2″,3″:4',5']thieno[2',3':4,5]pyrrolo[3,2-g]thieno[2',3':4,5]thieno[3,2-b]indole-2,10-diyl)bis(methanylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile)), and produces a power-conversion efficiency (PCE) of 13.03%. By adding small amount of Pt(Ph)2 (DMSO)2 (Ph, phenyl and DMSO, dimethyl sulfoxide), platinum(II) complexation would occur between Pt(Ph)2 (DMSO)2 and PSFTZ. The bulky benzene ring on the platinum(II) complex increases the steric hindrance along the polymer main chain, inhibits the polymer aggregation strength, regulates the phase separation, optimizes the morphology, and thus improves the efficiency to 16.35% in the resulting devices. 16.35% is the highest efficiency for single-junction PSCs reported so far.

Fine Optimization of Morphology Evolution Kinetics with Binary Additives for Efficient Non-Fullerene Organic Solar Cells.

The power conversion efficiency of polymer solar cells (PSCs) is strongly affected by active layer morphology. Here, two solvent additives (ODT: octance-1,8-dithiol; DIO: 1,8-diiodooctane) are used to optimize the bulk heterojunction morphology of FTAZ:ITIC-Th based PSCs and ≈11% efficiency is obtained, which is 10% higher than the untreated device. Based on the morphological characterizations, the influence of binary solvent additives on manipulating molecular packing and phase separation of blend films is successfully revealed. More importantly, in situ grazing incidence wide-angle X-ray scattering characterization is adopted to explore the crucial role played by these two solvent additives at different stages of the film-forming process, that is, ODT influences the initial stage of the film-forming process, while DIO later establishes the ultimate photoactive film formation. Due to the impacts of two additives at different film processing stages, an optimal ratio of ODT:DIO (0.375%:0.125%) is obtained, which helps in realizing the optimized morphology.

Low-Energy-Loss Polymer Solar Cells with 14.52% Efficiency Enabled by Wide-Band-Gap Copolymers.

Two wide band-gap copolymers poly[4,8-bis(5-(2-butylhexylthio)thiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene-2,6-diyl-alt-TZNT] (PBDTS-TZNT) and poly[4,8-bis(4-fluoro-5-(2-butylhexylthio)thiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene-2,6-diyl-alt-TZNT] (PBDTSF-TZNT) based on naphtho[1,2-c:5,6-c]bis(2-octyl-[1,2,3]triazole) (TZNT) and benzo[1,2-b:4,5-b']dithiophene (BDT) with different conjugated side chains have been developed for efficient nonfullerene polymer solar cells (NF-PSCs). The rigid planar backbone of BDT and TZNT units imparted high crystallinity and good molecular stacking property to these copolymers. Using 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone)-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2',3'-d']-s-indaceno[1,2-b:5,6-b']-dithiophene (ITIC) as the acceptor, PBDTSF-TZNT devices showed a high Voc of 0.98 V with an Eloss of 0.61 eV. On selecting 3,9-bis(2-methylene-(5,6-difluoro-(3-(1,1-dicyanomethylene)-indanone)-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2',3'-d']-s-indaceno[1,2-b:5,6-b']-dithiophene (IT-4F) instead of ITIC, the devices maintained the high Voc of 0.93 V with an even lower Eloss of 0.59 eV. The combination of the above-mentioned low Eloss, broadened absorption, better matched energy level, improved crystallinity, and fine-tuned morphology promoted the power conversion efficiency (PCE) of PBDTSF-TZNT:IT-4F devices from 12.16% to 13.25%. Homo-tandem devices based on PBDTSF-TZNT:IT-4F subcells further enhanced the light-harvesting ability and boosted the PCE of 14.52%, which is the best value for homo-tandem NF-PSCs at present.

Controlling Molecular Packing and Orientation via Constructing a Ladder-Type Electron Acceptor with Asymmetric Substituents for Thick-Film Nonfullerene Solar Cells.

A nonfullerene acceptor, IDTT-OB, employing indacenodithieno[3,2- b]thiophene (IDTT) decorated with asymmetric substituents as the core, is designedly prepared. In comparison with the analogue IDT-OB, extending the five-heterocyclic indacenodithiophene (IDT) core to seven-heterocyclic fused ring endows IDTT-OB with more broad absorption and elevated highest occupied molecular orbital energy level. In addition, IDTT-OB shows a more intense molecular packing and a higher crystalline behavior with a strong face-on orientation in the neat film and the PBDB-T:IDTT-OB blend film. Furthermore, an ideal nanomorphology with a domain size of 19 nm can be obtained, which is in favor of exciton diffusion and charge separation. Accordingly, PBDB-T:IDTT-OB-based polymer solar cells demonstrate a maximum power conversion efficiency (PCEmax) of 11.19% with an impressive fill factor of 0.74, comparable to the state-of-the-art acceptors with similar molecular backbones. More importantly, IDTT-OB-based devices show good tolerance to the film thickness, which maintain a high PCE of 10.20% with a 250 nm thick active layer, demonstrating that the asymmetric acceptor is profound for fabricating high-efficiency thick-film nonfullerene solar cells.

Dithienothiapyran: An Excellent Donor Block for Building High-Performance Copolymers in Nonfullerene Polymer Solar Cells.

In this work, a new but excellent donor block dithienothiapyran (DTTP) was developed for constructing highly efficient wide band gap copolymer donors. Compared to dithienopyran (DTP), DTTP features weaken electron-donating ability and more planar-conjugated backbones. Polymer-fluorinated benzotriazole (FBTA) based on DTTP exhibits lower highest occupied molecular orbital level (-5.30 vs -5.21 eV), higher molar extinction coefficient (1.54 × 105 vs 8.65 × 104 M-1 cm-1), and better crystallinity than -FBTA based on DTP, thus producing a higher device performance of 10.51% in binary blend nonfullerene polymer solar cells (NF-PSCs) blended with IT-M. To improve the absorption strength of PDTTP-FBTA: devices in the shorter wavelength range and further optimize the blend morphology, a small molecule of , which has strong absorption at short wavelength (300-600 nm), was incorporated. Finally, the performance of the ternary blends was successfully enhanced to 11.57% and a very high fill factor of 76.5%. Our work provided a new but excellent donor block for building high-performance conjugated copolymers to achieve highly efficient NF-PSCs.

Achieving Balanced Crystallinity of Donor and Acceptor by Combining Blade-Coating and Ternary Strategies in Organic Solar Cells.

As a prototype tool for slot-die coating, blade-coating exhibits excellent compatibility with large-area roll-to-roll coating. A ternary organic solar cell based on PBDB-T:PTB7-Th:FOIC blends is fabricated by blade-coating and exhibits a power conversion efficiency of 12.02%, which is one of the highest values for the printed organic solar cells in ambient environment. It is demonstrated that blade-coating can enhance crystallization of these three materials, but the degree of induction is different (FOIC > PBDB-T > PTB7-Th). Thus, the blade-coated PBDB-T:FOIC device presents much higher electron mobility than hole mobility due to the very high crystallinity of FOIC. Upon the addition of PTB7-Th into the blade-coated PBDB-T:FOIC blends, the crystallinity of FOIC decreases together with the corresponding electron mobility, due to the better miscibility between PTB7-Th and FOIC. The ternary strategy not only maintains the well-matched crystallinity and mobilities, but also increases the photocurrent with complementary light absorption as well as the Förster resonant energy transfer. Furthermore, small domains with homogeneously distributed nanofibers are observed in favor of the exciton dissociation and charge transport. This combination of blade-coating and ternary strategies exhibits excellent synergistic effect in optimizing morphology, showing great potential in the large-area fabrication of highly efficient organic solar cells.

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 (Voc ) of 1.08 eV and a low energy loss (Eloss ) 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 Voc of 1.06 V, a Jsc 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.