Efficient and Stable All-Polymer Solar Cells Enabled by Dual Working Mechanism.

Ternary strategy with integration characteristics and adaptability is a simple and effective method for blooming of the performance of photovoltaic devices. Herein, a novel wideband gap polymer donor PBB2-Hs is synthesized as the guest component to optimize all-polymer solar cells (all-PSCs). High-energy photon absorption and long exciton lifetime of PBB2-Hs constitute efficient energy transfer. Good miscibility and cascade energy levels promote the formation of alloy-like structure between PBB2-Hs and host system. The dual working mechanisms greatly improve photon capture and charge transfer in active layers. Additionally, the introduction of PBB2-Hs also optimizes the ordered molecular stacking of acceptors and suppresses molecular peristalsis. Upon adding 15 wt% PBB2-Hs, the ternary all-PSC achieved a champion efficiency of 17.66%, and can still maintain 82% photostability (24 h) and 91% storage stability (1000 h) of the original PCE. Moreover, the strong molecular stacking and entanglement between PBB2-Hs and the host material increased the elongation at break of ternary blend film by 1.6 times (16.2%), allowing the flexible device to maintain 83% of the original efficiency after 800 bends (R = 5 mm). This work highlights the effectiveness of guest polymer on simultaneously improving photovoltaic performance, photostability and mechanical stability in all-PSCs.

Efficient Dual Mechanisms Boost the Efficiency of Ternary Solar Cells with Two Compatible Polymer Donors to Exceed 19.

Ternary strategyopens a simple avenue to improve the power conversion efficiency (PCE) of organic solar cells (OSCs). The introduction of wide bandgap polymer donors (PDs) as third component canbetter utilize sunlight and improve the mechanical and thermal stability of active layer. However, efficient ternary OSCs (TOSCs) with two PDs are rarely reported due to inferior compatibility and shortage of efficient PDs match with acceptors. Herein, two PDs-(PBB-F and PBB-Cl) are adopted in the dual-PDs ternary systems to explore the underlying mechanisms and improve their photovoltaic performance. The findings demonstrate that the third components exhibit excellent miscibility with PM6 and are embedded in the host donor to form alloy-like phase. A more profound mechanism for enhancing efficiency through dual mechanisms, that are the guest energy transfer to PM6 and charge transport at the donor/acceptor interface, has been proposed. Consequently, the PM6:PBB-Cl:BTP-eC9 TOSCs achieve PCE of over 19%. Furthermore, the TOSCs exhibit better thermal stability than that of binary OSCs due to the reduction in spatial site resistance resulting from a more tightly entangled long-chain structure. This work not only provides an effective approach to fabricate high-performance TOSCs, but also demonstrates the importance of developing dual compatible PD materials.

Structure-Activity Relationship between Crystallinity and Carrier Transport of Two-Dimensional Donor Units in Organic Solar Cells.

Benzo[1,2-b:4,5-b']dithiophene (BDT) and its derivatives have made important contributions to constructing high-performance polymers. However, it is difficult to clarify the real role of donor units due to the interference of strong electronegativity and crystallinity of acceptor units in the D-A copolymer. Here, we design a cyclohexane-substituted dithieno[3,2-f:2',3'-h]quinoxaline (DTQ)-based acceptor unit with successfully destroyed crystallinity and charge transport. Three donor-dominated materials PQH-BTF, PQH-BTCl, and PQH-BFCl are obtained. It is found that the materials exhibit obvious differences after destroying the crystallization and charge transport of the acceptor unit, and the real role of different two-dimensional donor units in designed polymers is confirmed. The backbone BDF exhibits much stronger intermolecular interactions compared to BDT, while the side chain ThF demonstrates a higher crystallization capacity than that of ThCl. More interestingly, it can be inferred that the molecular backbone is likely to construct miscible-phase crystallization (D-A crystal) while the side chain tends to demonstrate a capacity for pure-phase crystallization (D-D crystal) in a 2D donor system. Different crystallization leads to different exciton transport: pure-phase crystallization is conducive to the reduction of trap-assisted recombination, while miscible crystallization is beneficial to the reduction of bimolecular recombination. This work can help to choose donor units more accurately when preparing D-A copolymers.

Embedded Host/Guest Alloy Aggregations Enable High-Performance Ternary Organic Photovoltaics.

The ternary strategy has been intensively studied to improve the power conversion efficiencies of organic photovoltaics. Thereinto, the location of the guest component plays a critical role, but few reports have been devoted to this concern. Hereon, the distribution of LA1 as a guest acceptor in a variety of ternary scenarios is reported and the dominating driving forces of managing the guest distribution and operating modes are outlined. Governed by the appropriate relationship of compatibility, crystallinity, and surface energies between host and guest acceptors, as well as interfacial interactions between donor and dual acceptors, most of the LA1 molecules permeate into the internal of host acceptor phases, forming embedded host/guest alloy-like aggregations. The characteristic distributions greatly optimize the morphologies, maximize energy transfer, and enhance exciton/charge behaviors. Particularly, PM6:IT-4F:LA1 ternary cells afford high efficiency of 15.27% with impressive fill factors (FF) over 81%. The popularization studies further verify the superiority of the LA1-involved alloy structures, and with the Y6-family acceptor as the host component, an outstanding efficiency of 19.17% is received. The results highlight the importance of guest distribution in ternary systems and shed light on the governing factors of distributing the guests in ternary cells.

Enhancing thermal conductivity and chemical protection of bacterial cellulose/silver nanowires thin-film for high flexible electronic skin.

Silver nanowires (AgNWs) thin films have emerged as a promising next-generation flexible electronic device. However, the current AgNWs thin films are often plagued by high AgNWs-AgNWs contact resistance and poor long-term stability. Here, to enhance the AgNWs stability on the surface of bacterial cellulose (BC), a novel flexible high conductivity thin-film was prepared by spin-coating a layer of polyvinyl alcohol (PVA) on the BC/AgNWs (BA) film. Firstly, BC film with high uniformity to better fit the AgNWs was obtained. It is observed that inadequately protected AgNWs can be corroded when AgNWs together with PVA were attached to the BC surface (BAP film), Yet, a layer of PVA was spin-coated on the surface of BA film, the BC/AgNWs/spin-coated 0.5 % PVA (BASP) thin-film (10.1 µm) exhibits that the PVA interfacial protective layer effectively mitigated the intrinsic incompatibility of BC with AgNWs as well as external corrosion (Na2S for 3 h) and immobilization of AgNWs, thus having a low conductive sheet resistance of 0.42 Ω/sq., which was better than most of the AgNWs-containing conductive materials reported so far. In addition, the resistance of the BASP thin-film changed little after 10,000 bending cycles, and the conductivity remained stable over BC directly immersed in 0.5 % PVA/AgNWs. This "soft" conductive material can be used to manufacture a new generation of electronic skin.

Formation of Efficient Quasi-All-Polymer Solar Cells by Synergistic Effect of the Ternary Strategy and Solid Additives.

All-polymer solar cells (all-PSCs) have been widely studied owing to their unique mechanical flexibility and stability. However, all-PSCs have a lower efficiency than small-molecule acceptor-based PSCs. In the work, a ternary quasi-all-polymer solar cell (Q-all-PSC) using a synergy of the ternary strategy and solid additive engineering is reported. The introduction of PC71BM can not only match the energy level of the photoactive materials with an improved open circuit voltage (VOC) of the ternary devices but also enhance photon capture, which can improve short circuit current density. It is found that there is effective charge transfer between PC71BM and PY-IT, which can form an electron transport channel and promote efficient charge transport. Moreover, the introduction of PC71BM made the PM6/PY-IT/PC71BM ternary blends more crystalline while slightly reducing phase separation, resulting in a suitable domain size. Importantly, by introducing a high dielectric-constant PFBEK solid additive as the fasten matrix, the Q-all-PSC's efficiency can reach 16.42%. This method provides a new idea for future research on all-polymer solar cells.

Over 19% Efficiency Organic Solar Cells by Regulating Multidimensional Intermolecular Interactions.

Research on organic solar cells (OSCs) has progressed through material innovation and device engineering. However, well-known and ubiquitous intermolecular interactions, and particularly their synergistic effects, have received little attention. Herein, the complicated relationship between photovoltaic conversion and multidimensional intermolecular interactions in the active layers is investigated. These interactions are dually regulated by side-chain isomerization and end-cap engineering of the acceptors. The phenylalkyl featured acceptors (LA-series) exhibit stronger crystallinity with preferential face-on interactions relative to the alkylphenyl attached isomers (ITIC-series). In addition, the PM6 and LA-series acceptors exhibit moderate donor/acceptor interactions compared to those of the strongly interacting PM6/ITIC-series pairs, which helps to enhance phase separation and charge transport. Consequently, the output efficiencies of all LA series acceptors are over 14%. Moreover, LA-series acceptors show appropriate compatibility, host/guest interactions, and crystallinity relationships with BTP-eC9, thereby leading to uniform and well-organized "alloy-like" mixed phases. In particular, the highly crystalline LA23 further optimizes multiple interactions and ternary microstructures, which results in a high efficiency of 19.12%. Thus, these results highlight the importance of multidimensional intermolecular interactions in the photovoltaic performance of OSCs.

End Group Effect of Asymmetric Benzodithiophene-Based Donor with Liquid-Crystal State for Small-Molecule Binary Solar Cell.

Liquid-crystal small molecule donor (LC-SMD) is a new type organic semiconductor, which is attractive not only for the easy synthesis and purification, well-defined chemical structures, etc., but also for the LC state that makes the crystallinity and aggregation state of molecules adjustable. Here, one new LC-SMD (a-BTR-H4) is synthesized with 1D alkoxyl and 2D thiophene-alkylthiol side-chained benzo[1,2-b:4,5-b']dithiophene core, trithiophene π-bridge, and 3-(2-ethylhexyl) rhodanine end group. a-BTR-H4 shows low LC transition temperature, 117 °C, however, counterpart material (a-BTR-H5) with the same main structure but 3-ethyl rhodanine terminal group does not show LC properties. Although a-BTR-H4/H5 show similar Ultraviolet-visible absorption spectrum and energy levels, a-BTR-H4 affords relatively high photovoltaic performances due to favorable blend morphology produced by the consistent annealing temperature of Y6-based accepters and liquid crystal temperature of donors. Preliminary results indicate that a-BTR-H4 gains a power conversion efficiency (PCE) of 11.36% for Y6-based devices, which is ascribed to better light harvest as well as balanced carrier generation and transport, while a-BTR-H5 obtains 7.57% PCE. Therefore, some materials with unique nematic LC phase have great application potential in organic electronics, and further work to utilize a-BTR-H4 for high-performance device is underway.

Photoinduced large polaron transport and dynamics in organic-inorganic hybrid lead halide perovskite with terahertz probes.

Organic-inorganic hybrid metal halide perovskites (MHPs) have attracted tremendous attention for optoelectronic applications. The long photocarrier lifetime and moderate carrier mobility have been proposed as results of the large polaron formation in MHPs. However, it is challenging to measure the effective mass and carrier scattering parameters of the photogenerated large polarons in the ultrafast carrier recombination dynamics. Here, we show, in a one-step spectroscopic method, that the optical-pump and terahertz-electromagnetic probe (OPTP) technique allows us to access the nature of interplay of photoexcited unbound charge carriers and optical phonons in polycrystalline CH3NH3PbI3 (MAPbI3) of about 10 µm grain size. Firstly, we demonstrate a direct spectral evidence of the large polarons in polycrystalline MAPbI3. Using the Drude-Smith-Lorentz model along with the FrÓ§hlich-type electron-phonon (e-ph) coupling, we determine the effective mass and scattering parameters of photogenerated polaronic carriers. We discover that the resulting moderate polaronic carrier mobility is mainly influenced by the enhanced carrier scattering, rather than the polaron mass enhancement. While, the formation of large polarons in MAPbI3 polycrystalline grains results in a long charge carrier lifetime at room temperature. Our results provide crucial information about the photo-physics of MAPbI3 and are indispensable for optoelectronic device development with better performance.

Biomimetic FeCo@PDA nanozyme platform with Fenton catalytic activity as efficient antibacterial agent.

The multidrug resistance of bacteria caused by the abuse of traditional antibiotics poses a great threat to public health, so it is urgent to develop effective antibacterial agents to deal with this dilemma. Biomimetics and nanotechnology are expected to provide new strategies for solving this problem. This study takes inspiration from the adhesive protein properties of mussels to design and synthesise biomimetic polydopamine nanospheres (FeCo@PDA NPs), which have strong adhesion and catalytic Fenton reactive enzyme activity. The antibacterial activity of FeCo@PDA NPs against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) is significantly better than that of traditional antibiotics daptomycin (Dap) and vancomycin (Van). PDA NPs with an intrinsic hierarchical structure have the ability to adhere to bacterial surfaces and improve the loading rate of metal ions Fe2+/Co2+. In addition, due to the dual effects of strong adhesion and Co2+, FeCo@PDA NPs can destroy the bacterial membrane structure and release endogenous hydrogen peroxide, which increases the generation of reactive oxygen species by synergistic catalysis of bimetal ions Fe2+/Co2+ to further kill bacteria thoroughly. The cytotoxicity test results show that FeCo@PDA NPs have good cytocompatibility. The impressive antibacterial properties and good biocompatibility of FeCo@PDA NPs make them a potential antibacterial drug.

Impact of backbone linkage positions on the molecular aggregation behavior of polymer photovoltaic materials.

It is imperative to advance the structural design of conjugated materials to achieve a practical impact on the performance of photovoltaic devices. However, the effect of the linkage positions (meta-, para-) of the backbone on the molecular packing has been relatively little explored. In this study, we have synthesized two wide-bandgap polymer photovoltaic materials from identical monomers with different linkage positions, using dibenzo[c,h][2,6]-naphthyridine-5,11-(6H,12H)-dione (DBND) as the building block. This study shows that the para-connected polymer exhibits an unexpected 0.2 eV higher ionization potential and a resultant higher open-circuit voltage than the meta-connected counterpart. We found that different linkage positions result in different intermolecular binding energies and molecular aggregation conformations, leading to different HOMO energy levels and photovoltaic performances. Specifically, theoretical calculations and 2D-NMR indicate that P(p-DBND-f-2T) performs a segregated stacking of f-2T and DBND units, while P(m-DBND-f-2T) films form π-overlaps between f-2T and DBND. These results show that linkage position adjustment on the polymeric backbone exerts a profound influence on the molecular aggregation of the materials. Also, the effect of isomerism on the polymer backbone is crucial in designing polymer structures for photovoltaic applications.

Two Compatible Acceptors as an Alloy Model with a Halogen-Free Solvent for Efficient Ternary Polymer Solar Cells.

A ternary strategy of halogen-free solvent processing can open up a promising pathway for the preparation of polymer solar cells (PSCs) on a large scale and can effectively improve the power conversion efficiency with an appropriate third component. Herein, the green solvent o-xylene (o-XY) is used as the main solvent, and the non-fullerene acceptor Y6-DT-4F as the third component is introduced into the PBB-F:IT-4F binary system to broaden the spectral absorption and optimize the morphology to achieve efficient PSCs. The third component, Y6-DT-4F, is compatible with IT-4F and can form an "alloy acceptor", which can synergistically optimize the photon capture, carrier transport, and collection capabilities of the ternary device. Meanwhile, Y6-DT-4F has strong crystallinity, so when introduced into the binary system as the third component can enhance the crystallization, which is conducive to the charge transport. Consequently, the optimal ternary system based on PBB-F:IT-4F:Y6-DT-4F achieved an efficiency of 15.24%, which is higher than that of the binary device based on PBB-F:IT-4F (13.39%).

Subtle Side Chain Triggers Unexpected Two-Channel Charge Transport Property Enabling 80% Fill Factors and Efficient Thick-Film Organic Photovoltaics.

To clearly show how important the impact of side chains on organic solar cells (OSCs) is, we designed three acceptors IDIC-CxPh (x = 4, 5, or 6) via subtle side-chain regulation. Despite this small change, significant distinctions were detected. IDIC-C4Ph devices achieve an optimal efficiency of 13.94% under thermal annealing, but thermal-assistant solvent-vapor annealing hugely suppresses the efficiencies to 10%. However, the C6Ph side chain endows extremely disordered stacking orientations, generating moderate efficiencies of ~12.50%. Excitingly, the IDIC-C5Ph affords an unexpected two-channel π-π charge transport (TCCT) property, boosting the fill factor (FF) by up to 80.02% and efficiency to 14.56%, ranking the best among five-ring fused-ladder-type acceptors. Impressively, the special TCCT behavior of IDIC-C5Ph enables 470 nm thick-film OSC with a high FF of up to 70.12% and efficiency of 13.01%, demonstrating the great promise in fabricating large-scale OSCs.

Benzobis(Thiazole)-Based Conjugated Polymer with Varying Alkylthio Side-Chain Positions for Efficient Fullerene-Free Organic Solar Cells.

Alkylthio groups can be used to modulate energy levels and molecular packing of organic semiconductors, which makes it important in the design of materials for organic solar cell. However, its effect has not been sufficiently exploited as most of the studies report introducing an alkylthio group to the donor unit and seldom to the acceptor unit of donor-acceptor conjugated polymers. In this report, two alkylthio-substituted polymers, namely, PBB-TSA and PBB-TSD, with benzo[1,2-d:4,5-d']bis(thiazole) (BBT) as the acceptor unit and benzo[1,2-b:4,5-b']dithiophene (BDT) as the donor unit, were rationally designed, synthesized, and applied in organic photovoltaics. An alkylthio side chain was substituted on the BBT-accepting unit for PBB-TSA, while for PBB-TSD, the alkylthio side chain was substituted on the BDT donor unit. PBB-TSA and PBB-TSD show upshifted and downshifted energy levels, respectively, compared to the nonsulfur-substituted material. Both polymers exhibit dominate face-on orientation, while PBB-TSD exhibits higher crystallinity compared to PBB-TSA. With the contribution of lower energy level and beneficial film morphology, the device based on PBB-TSD/IT-4F has much higher power conversion efficiency (PCE) of 14.6%, whereas the PBB-TSA blend had a lower PCE of 10.7%. 1,8-Diiodooctane can effectively optimize the blend film morphology, and the effect on device performance has also been demonstrated in detail. This result indicates that introducing an alkylthio side chain into the donor or acceptor moieties would result in materials with different energy levels and thus would be utilized to match with various acceptors, achieving optimized performance in organic solar cells.

Significantly Boosting Efficiency of Polymer Solar Cells by Employing a Nontoxic Halogen-Free Additive.

Traditional additives like 1,8-diiodooctane and 1-chloronaphthalene were successfully utilized morphology optimization of various polymer solar cells (PSCs) in an active layer, but their toxicity brought by halogen atoms limits their corresponding large-scale manufacturing. Herein, a new nontoxic halogen-free additive named benzyl benzoate (BB) was introduced into the classic PSCs (PTB7-Th:PC71BM), and an optimal power conversion efficiency (PCE) of 9.43% was realized, while there was a poor PCE for additive free devices (4.83%). It was shown that BB additives could inhibit PC71BM's overaggregation, which increased the interface contact area and formed a better penetration path of an active layer. In addition, BB additives could not only boost the distribution of a PTB7-Th donor at the surface, beneficial to suppressing exciton recombination in inverted devices but also boost the crystallinity of a blend layer, which is conducive to exciton dissociation and charge transport. Our work effectively improved a device performance by using a halogen-free additive, which can be referential for industrialization.

Suppressing the Photocatalytic Activity of Zinc Oxide Electron-Transport Layer in Nonfullerene Organic Solar Cells with a Pyrene-Bodipy Interlayer.

Organic solar cells based on nonfullerene acceptors have recently witnessed a significant rise in their power conversion efficiency values. However, they still suffer from severe instability issues, especially in an inverted device architecture based on the zinc oxide bottom electron transport layers. In this work, we insert a pyrene-bodipy donor-acceptor dye as a thin interlayer at the photoactive layer/zinc oxide interface to suppress the degradation reaction of the nonfullerene acceptor caused by the photocatalytic activity of zinc oxide. In particular, the pyrene-bodipy-based interlayer inhibits the direct contact between the nonfullerene acceptor and zinc oxide hence preventing the decomposition of the former by zinc oxide under illumination with UV light. As a result, the device photostability was significantly improved. The π-π interaction between the nonfullerene acceptor and the bodipy part of the interlayer facilitates charge transfer from the nonfullerene acceptor toward pyrene, which is followed by intramolecular charge transfer to bodipy part and then to zinc oxide. The bodipy-pyrene modified zinc oxide also increased the degree of crystallization of the photoactive blend and the face-on stacking of the polymer donor molecules within the blend hence contributing to both enhanced charge transport and increased absorption of the incident light. Furthermore, it decreased the surface work function as well as surface energy of the zinc oxide film all impacting in improved power conversion efficiency values of the fabricated cells with champion devices reaching values up to 9.86 and 11.80% for the fullerene and nonfullerene-based devices, respectively.

Optimized Molecular Packing and Nonradiative Energy Loss Based on Terpolymer Methodology Combining Two Asymmetric Segments for High-Performance Polymer Solar Cells.

In this work, a random terpolymer methodology combining two electron-rich units, asymmetric thienobenzodithiophene (TBD) and thieno[2,3-f]benzofuran segments, is systematically investigated. The synergetic effect is embodied on the molecular packing and nanophase when copolymerized with 1,3-bis(2-ethylhexyl)benzo[1,2-c:4,5-c']dithiophene-4,8-dione, producing an impressive power conversion efficiency (PCE) of 14.2% in IT-4F-based NF-PSCs, which outperformed the corresponding D-A copolymers. The balanced aggregation and better interpenetrating network of the TBD50:IT-4F blend film can lead to mixing region exciton splitting and suppress carrier recombination, along with high yields of long-lived carriers. Moreover, the broad applicability of terpolymer methodology is successfully validated in most electron-deficient systems. Especially, the TBD50/Y6-based device exhibits a high PCE of 15.0% with a small energy loss (0.52 eV) enabled by the low nonradiative energy loss (0.22 eV), which are among the best values reported for polymers without using benzodithiophene unit to date. These results demonstrate an outstanding terpolymer approach with backbone engineering to raise the hope of achieving even higher PCEs and to enrich organic photovoltaic materials reservoir.

Insights into Excitonic Dynamics of Terpolymer-Based High-Efficiency Nonfullerene Polymer Solar Cells: Enhancing the Yield of Charge Separation States.

Ternary copolymerization strategy is considered an effective method to achieve high-performance photovoltaic conjugated polymers. Herein, a donor-acceptor1-donor-acceptor2-type random copolymer, named PBDTNS-TZ-BDD (T1), containing one electron-rich unit alkylthionaphthyl-flanked benzo[1,2-b/4,5-b'] di-thiophene (BDTNS) as D and two electron-deficient moieties benzo[1,2-c/4,5-c']dithiophene-4,8-dione (BDD) and fluorinated benzotriazole as A, was synthesized to investigate the excitonic dynamic effect. Also, the D-A-type alternating copolymer PBDTNS-BDD (P1) was also prepared for a clear comparison. Although the UV-Vis spectra and energy levels of P1 and T1 are similar, the power conversion efficiencies (PCEs) of the related devices are 11.50% (T1/ITIC) and 8.89% (P1/ITIC), respectively. The reason for this is systematically investigated and analyzed by theoretical calculation, photoluminescence, and pump-probe transient absorption spectroscopy. The density functional theory (DFT) and time-dependent density functional theory (TD-DFT) calculation results show that the terpolymer T1 with a lower exciton binding energy and a longer lifetime of spontaneous luminescence can synergistically increase the number of excitons reaching the donor/acceptor interface. The results of the pump-probe transient absorption spectroscopy show that the yield of charge separation of T1/ITIC is higher than that of the P1/ITIC blend film, and improved PCE could be achieved via copolymerization strategies. Moreover, the fabrication of the T1-based device is also simple without any additive or postprocessing. Therefore, it provides a promising and innovative method to design high-performance terpolymer materials.

Enhanced Organic and Perovskite Solar Cell Performance through Modification of the Electron-Selective Contact with a Bodipy-Porphyrin Dyad.

Photovoltaic devices based on organic semiconductors and organo-metal halide perovskites have not yet reached the theoretically predicted power conversion efficiencies while they still exhibit poor environmental stability. Interfacial engineering using suitable materials has been recognized as an attractive approach to tackle the above issues. We introduce here a zinc porphyrin-triazine-bodipy donor-π bridge-acceptor dye as a universal electron transfer mediator in both organic and perovskite solar cells. Thanks to its "push-pull" character, this dye enhances electron transfer from the absorber layer toward the electron-selective contact, thus improving the device's photocurrent and efficiency. The direct result is more than 10% average power conversion efficiency enhancement in both fullerene-based (from 8.65 to 9.80%) and non-fullerene-based (from 7.71 to 8.73%) organic solar cells as well as in perovskite ones (from 14.56 to 15.67%), proving the universality of our approach. Concurrently, by forming a hydrophobic network on the surface of metal oxide substrates, it improves the nanomorphology of the photoactive overlayer and contributes to efficiency stabilization. The fabricated devices of both kinds preserved more than 85% of their efficiency upon exposure to ambient conditions for more than 600 h without any encapsulation.

Rational Design of Low Band Gap Polymers for Efficient Solar Cells with High Open-Circuit Voltage: The Profound Effect of Me and Cl Substituents with a Similar van Der Waals Radius.

Generally, low band gap material-based photovoltaic devices have reduced open circuit voltage (VOC), and realizing the trade-off between the low band gap (Eg < 1.6 eV) and high VOC (>0.9 V) could be critical to give efficient polymer solar cells, especially for high-performance semitransparent PSCs and tandem solar cells. Although lots of efforts have been made to address the issue, most results have not been gratifying. In this work, the polymer PTBTz-Cl based on the chlorination method and efficient thiazole-induced strategy was designed and synthesized, aiming at the deep HOMO energy level, and the enhanced backbone planarity caused by the weak noncovalent Cl···S interaction. In addition, the methyl-substituted polymer PTBTz-Me was constructed as the reference due to the similar van der Waals radius of the side chain (CH3: 0.20 nm vs Cl: 0.18 nm). Encouragingly, in comparison with that of PTBTz-2, the newly synthesized polymers exhibit the red-shifted absorption spectra ranging from 300 to 770 nm, with an obviously reduced Eg of ∼1.6 eV. However, the function of Cl and Me substituents is different. Compared to the polymer PTBTz-Me, PTBTz-Cl exhibits a lower HOMO value, stronger crystallinity, and more compact intramolecular interactions. Consequently, the polymer PTBTz-Cl exhibits excellent photovoltaic performance with a notable VOC of 0.94 V and a power conversion efficiency of 10.35%, which is ∼11% higher than the 9.12% efficiency based on PTBTz-Me, and is also one of the highest values among polymer/fullerene solar cells. Moreover, a smaller photo energy loss (Eloss) of 0.64 eV is achieved, which is rare among the current high-performance polymer systems.