π-Extended giant dimeric acceptor as a third component enables highly efficient ternary organic solar cells with efficiency over 19.2%

Ternary strategy with a suitable third component is a successful strategy to improve the photovoltaic performance of organic solar cells(OSCs).Very recently,Y-series based giant molecule acceptors or oligomerized acceptors have emerged as promising materials for achieving highly efficient and stable binary OSCs,while application as third component for ternary OSCs is limited.Here a novelπ-extended giant dimeric acceptor,GDF,is developed based on central Y series core fusion and rigid BDT as linker,and then incorporated into the state-of-the-art PM1:PC6 system to construct ternary OSCs.The GDF has a near planar backbone,resulting in increasedπ-conjugation,excellent crystallinity,and good electron transport capacity.When GDF is introduced into the PM1:PC6 system,it ensues in a cascade like the lowest unoccupied molecular orbitals(LUMO)energy level alignment,a complementary absorption band with PM1 and PC6,higher and balanced hole and electron mobility,slightly smaller domain size,and a higher exciton dissociation probability for PM1:PC6:GDF(1:1.1:0.1)blend film.As a consequence,the PM1:PC6:GDF(1:1.1:0.1)ternary OSC achieves a champion PCE of 19.22%,with a significantly higher open-circuit voltage and short-circuit current density,compared to 18.45%for the PM1:PC6(1:1.2)binary OSC.Our findings show that employing aπ-extended giant dimeric acceptor as a third component significantly improves the photovoltaic performance of ternary OSCs.

A new perspective to develop regiorandom polymer acceptors with high active layer ductility,excellent device stability,and high efficiency approaching 17%

The recently reported efficient polymerized small-molecule acceptors(PSMAs)usually adopt a regioregular backbone by polymerizing small-molecule acceptors precursors with a low-reactivity 5-brominated 3-(dicyanomethylidene)indan-1-one(IC)end group or its derivatives,leading to low molecular weight,and thus reduce active layer mechanical properties.Herein,a series of newly designed chlorinated PSMAs originating from isomeric IC end groups are developed by adjusting chlorinated positions and copolymerized sites on end groups to achieve high molecular weight,favorable intermolecular interaction,and improved physicochemical properties.Compared with regioregular PY2Se-Cl-o and PY2Se-Cl-m,regiorandom PY2Se-Cl-ran has a similar absorption profile,moderate lowest unoccupied molecular orbital level,and favorable intermolecular packing and crystallization properties.Moreover,the binary PM6:PY2Se-Cl-ran blend achieves better ductility with a crack-onset strain of 17.5% and improved power conversion efficiency(PCE)of 16.23% in all-polymer solar cells(all-PSCs)due to the higher molecular weight of PY2Se-Cl-ran and optimized blend morphology,while the ternary PM6:J71:PY2Se-Cl-ran blend offers an impressive PCE approaching 17% and excellent device stability,which are all crucial for potential practical applications of all-PSCs in wearable electronics.To date,the efficiency of 16.86% is the highest value reported for the regiorandom PSMAs-based all-PSCs and is also one of the best values reported for the all-PSCs.Our work provides a new perspective to develop efficient all-PSCs,with all high active layer ductility,impressive PCE,and excellent device stability,towards practical applications.

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 bladecoating 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 endgroup.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:YRSeNF-based OSCs.As a result,a record-high PCE approaching 19%is achieved in the blade-coating OSCs fabricated from a greensolvent 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.

Non-Fully Conjugated Photovoltaic Materials with Y-Series Acceptor Backbone for High-Performance Organic Solar Cells

In the last few years,organic solar cells(OSCs)have made significant progress in photovoltaic performance,mainly due to the innovative development of active layer materials,especially Y-series and related derivatives as acceptors which have become the key factor that boosts the power conversion efficiency.Recently,to achieve high-performance OSCs,an emerging molecular design strategy of applying flexible alkyl units as linkers to construct non-fully conjugated acceptors has been developed and addressed great attention.This review highlights the non-fully conjugated photovoltaic materials with Y-series backbone that enable high-performance OSCs.Impressive OSCs have been achieved by some representative non-fully conjugated material systems.The related molecular design strategies are discussed in detail.Finally,a brief summary and future prospect are provided in advancing the non-fully conjugated photovoltaic materials with Y-series backbone towards the brighter future.

Trialkylsilyl-thiophene-conjugated acceptor for efficient organic solar cells compatible with spin-coating and blade-coating technologies

Sidechain engineering as an efficient and convenient strategy has been widely used to optimize molecular structure of photovoltaic materials for boosting power conversion efficiency(PCE)of organic solar cells(OSCs).Herein,a new Y-series acceptor named Y-Th Si with trialkylsilyl-substituted thiophene as conjugated sidechain is developed.Compared with its parental Y6 with multiple intermolecular interactions,Y-Th Si has a unitary molecular packing due to the additional steric hindrance from twodimensional(2D)-conjugated trialkylsilyl-thiophene.Therefore,Y-Th Si shows an obviously blue-shifted absorption with an onset of~850 nm but significantly up-shifted lowest unoccupied molecular orbital energy level.For the PM6:Y-Th Si pair,the spin-coating OSCs achieve a decent PCE of 14.56%with an impressively high photovoltage(V_(OC))of 0.936 V.Inspired by its high V_(OC)and narrow absorption,Y-Th Si is introduced into near-infrared absorbing binary PM6:BTP-eC9 host to construct ternary OSCs.Thanks to the complementary absorption,optimized morphology,and minimized energy loss properties,the PM6:BTP-e C9:Y-Th Si-based OSCs offer a higher PCE of 18.34%.Moreover,our developed strategy can overcome the commonly existed PCE drop when the blade-coating towards large-scale printing is used instead.Therefore,a comparable PCE of 18.34%is achieved,which is one of the best values for the blade-coating OSCs so far.

Non-fullerene acceptors with heteroatom substitution on the core moiety for efficient organic photovoltaics

Organic photovoltaics(OPVs)represent one of the most promising photovoltaic technologies owing to their high capacity to convert solar energy to electricity.With the continuous structure upgradation of photovoltaic materials,especially that of non-fullerene acceptors(NFAs),the OPV field has witnessed rapid progress with power conversion efficiency(PCE)exceeding 19%.However,it remains challenging to overcome the intrinsic trade-off between the photocurrent and photovoltage,restricting the further promotion of the OPV efficiency.In this regard,it is urgent to further tailor the structure of NFAs to broaden their absorption spectra while mitigating the energy loss of relevant devices concomitantly.Heteroatom substitution on the fused-ringπ-core of NFAs is an efficient way to achieve this goal.In addition to improve the nearinfrared light harvest by strengthening the intramolecular charge transfer,it can also enhance the molecular stacking via forming multiple noncovalent interactions,which is favorable for reducing the energetic disorder.Therefore,in this review we focus on the design rules of NFAs,including the polymerized NFAs,of which the core moiety is substituted by various kinds of heteroatoms.We also afford a comprehensive understanding on the structure–propertyperformance relationships of these NFAs.Finally,we anticipate the challenges restricting the efficiency promotion and industrial utilization of OPV,and provide potential solutions based on the further heteroatom optimization on NFA core-moiety.

Approaching 19%efficiency and stable binary polymer solar cells enabled by a solidification strategy of solvent additive

Additives play a crucial role in enhancing the photovoltaic performance of polymer solar cells(PSCs).However,the typical additives used to optimize blend morphology of PSCs are still high boiling-point solvents,while their trace residues may reduce device stability.Herein,an effective strategy of“solidification of solvent additive(SSA)”has been developed to convert additive from liquid to solid,by introducing a covalent bond into low-cost solvent diphenyl sulfide(DPS)to synthesize solid dibenzothiophene(DBT)in one-step,which achieves optimized morphology thus promoting efficiency and device stability.Owing to the fine planarity and volatilization of DBT,the DBT-processed films achieve ordered molecular crystallinity and suitable phase separation compared to the additive-free or DPS-treated ones.Importantly,the DBT-processed device also possesses improved light absorption,enhanced charge transport,and thus a champion efficiency of 17.9%is achieved in the PM6:Y6-based PSCs with an excellent additive component tolerance,reproducibility,and stability.Additionally,the DBT-processed PM6:L8-BO-based PSCs are further fabricated to study the universality of SSA strategy,offering an impressive efficiency approaching19%as one of the highest values in binary PSCs.In conclusion,this article developed a promising strategy named SSA to boost efficiency and improve stability of PSCs.

Host-Guest Strategy Enabling Nonhalogenated Solvent Processing for High-Performance All-Polymer Hosted Solar Cells

The power conversion efficiencies(PCEs)of all-polymer solar cells(all-PSCs),usually processed from low-boiling-point and toxic sol-vents,have reached high values of 18%.However,poor miscibility and uncontrollable crystallinity in polymer blends lead to a nota-ble drop in the PCEs when using green solvents,limiting the practical development of all-PSCs.Herein,a third component(guest)BTO was employed to optimize the miscibility and enhance the crystallinity of PM6/PY2Se-F host film processed from green solvent toluene(TL),which can effectively suppress the excessive aggregation of PY2Se-F and facilitate a nano-scale interpenetrating net-work morphology for exciton dissociation and charge transport.As a result,TL-processed all-polymer hosted solar cells(all-PHSCs)exhibited an impressive PCE of 17.01%.Moreover,the strong molecular interaction between the host and guest molecules also en-hances the thermal stability of the devices.Our host-guest strategy provides a unique approach to developing high-efficiency and stable all-PHSCs processed from green solvents,paving the way for the industrial development of all-PHSCs.

Selenium-fused Y6 derivatives and their derived polymerized small molecule acceptors for efficient organic solar cells

Before 2015,only few organic solar cells(OSCs)obtained power conversion efficiencies(PCEs)over 10%because the commonly used fullerene derivatives as acceptors have narrow absorption,low extinction coefficient,and are difficult to adjust energy levels.To overcome these shortcomings,in 2015,Zhan et al.[1]developed acceptor(A)-donor(D)-A-type fused-ring small-molecule acceptors(SMAs)with good planarity and strong intramolecular charge transfer(ICT)effect to fulfill both broad absorption and high extinction coefficient,offering the revolutionary PCEs of 13%–15%.In 2019,another milestone SMA(Y6)with A-DA′D-A structure was developed by Zou et al.

High-performance all-polymer solar cells enabled by a novel low bandgap non-fully conjugated polymer acceptor

The non-fully conjugated polymer as a new class of acceptor materials has shown some advantages over its small molecular counterpart when used in photoactive layers for all-polymer solar cells(all-PSCs),despite a low power conversion efficiency(PCE)caused by its narrow absorption spectra.Herein,a novel non-fully conjugated polymer acceptor PFY-2TS with a low bandgap of~1.40 eV was developed,via polymerizing a largeπ-fused small molecule acceptor(SMA)building block(namely YBO)with a non-conjugated thioalkyl linkage.Compared with its precursor YBO,PFY-2TS retains a similar low bandgap but a higher LUMO level.Moreover,compared with the structural analog of YBO-based fully conjugated polymer acceptor PFY-DTC,PFY-2TS shows a similar absorption spectrum and electron mobility,but significantly different molecular crystallinity and aggregation properties,which results in optimal blend morphology with a polymer donor PBDB-T and physical processes of the device in all-PSCs.As a result,PFY-2TS-based all-PSCs achieved a PCE of 12.31%with a small energy loss of 0.56 eV enabled by the reduced non-radiative energy loss(0.24 eV),which is better than that of 11.08%for the PFY-DTC-based ones.Our work clearly demonstrated that non-fully conjugated polymers as a new class of acceptor materials are very promising for the development of high-performance all-PSCs.

Polymer acceptors based on Y6 derivatives for all-polymer solar cells

Significant progress has been witnessed in the development of organic solar cells(OSCs)with power conversion efficiency(PCE)over 18%due to the tremendous breakthrough of non-fullerene fused-ring small molecule acceptors(SMAs)in recent years[1–3].Although OSCs comprising of a polymer donor and a SMA have achieved the highest PCE,all-polymer solar cells(all-PSCs)consisting of tightly entangled polymer donor and polymer acceptor are generally considered to be the most promising practical wearable power generators in the future due to their outstanding device stability under mechanical and thermal stresses[4,5].Fan et al.

Reducing energy loss via tuning energy levels of polymer acceptors for efficient all-polymer solar cells

The open-circuit voltage(Voc) of all-polymer solar cells(all-PSCs) is typically lower than 0.9 V even for the most efficient ones.Large energy loss is the main reason for limiting Voc and efficiency of all-PSCs. Herein, through materials design using electron deficient building blocks based on bithiophene imides, the lowest unoccupied molecular orbital(LUMO) energy levels of polymer acceptors can be effectively tuned, which resulted in a reduced energy loss induced by charge generation and recombination loss due to the suppressed charge-transfer(CT) state absorption. Despite a negligible driving force, all-PSC based on the polymer donor and acceptor combination with well-aligned energy levels exhibited efficient charge transfer and achieved an external quantum efficiency over 70% while maintaining a large Voc of 1.02 V, leading to a 9.21% efficiency. Through various spectroscopy approaches, this work sheds light on the mechanism of energy loss in all-PSCs, which paves an avenue to achieving efficient all-PSCs with large Voc and drives the further development of all-PSCs.

Synergistic effect of fluorination on both donor and acceptor materials for high performance non-fullerene polymer solar cells with 13.5% efficiency

A high performance polymer solar cells(PSCs) based on polymer donor PM6 containing fluorinated thienyl benzodithiophene unit and n-type organic semiconductor acceptor IT-4 F containing fluorinated end-groups were developed. In addition to complementary absorption spectra(300–830 nm) with IT-4 F, the PM6 also has a deep HOMO(the highest occupied molecular) level(-5.50 e V), which will lower the open-circuit voltage(V_(oc)) sacrifice and reduce the E_(loss) of the IT-4 F-based PSCs. Moreover, the strong crystallinity of PM6 is beneficial to form favorable blend morphology and hence to suppress recombination. As a result, in comparison with the PSCs based on a non-fluorinated D/A pair of PBDB-T:ITIC with a medium PCE of 11.2%, the PM6:IT-4 Fbased PSCs yielded an impressive PCE of 13.5% due to the synergistic effect of fluorination on both donor and acceptor, which is among the highest values recorded in the literatures for PSCs to date. Furthermore, a PCE of 12.2% was remained with the active layer thickness of up to 285 nm and a high PCE of 11.4% was also obtained with a large device area of 1 cm^2. In addition, the devices also showed good storage, thermal and illumination stabilities with respect to the efficiency. These results indicate that fluorination is an effective strategy to improve the photovoltaic performance of materials, as well as the both fluorinated donor and acceptor pair-PM6:IT-4 F is an ideal candidate for the large scale roll-to-roll production of efficient PSCs in the future.

16.3%Efficiency binary all-polymer solar cells enabled by a novel polymer acceptor with an asymmetrical selenophene-fused backbone

Despite the significant progress made recently in all-polymer solar cells(all-PSCs),it is still quite challenging to achieve high open-circuit voltage(V_(oc))and short-circuit current density(J_(sc))simultaneously in order to further improve their performance.The recent strategy of using selenophene to replace thiophene on the Y6 based polymer acceptors has resulted in significantly improved J_(sc)s of the resulting all-PSCs.However,such modifications have also depressed V_(oc),which compromises the overall performance of the devices.Herein,we present the design and synthesis of a novel polymer acceptor,PYT-1S1Se,created by inserting an asymmetrical selenophene-fused framework to precisely manipulate optical absorption and electronic properties.Compared with the selenium-free analog,PYT-2S,and symmetrical selenium-fused analog,PYT-2Se,the PYT-1S1Se derived all-PSCs not only deliver optimized J_(sc)(24.1 mA cm^(−2))and V_(oc)(0.926 V)metrics,but also exhibit a relatively low energy loss of 0.502 eV.Consequently,these devices obtain a record-high power conversion efficiency(PCE)of 16.3%in binary all-PSCs.This work demonstrates an effective molecular design strategy for balancing the trade-off between V_(oc) and J_(sc) to achieve highefficiency all-PSCs.

Modulating Crystallinity and Miscibility via Side-chain Variation Enable High Performance All-Small-Molecule Organic Solar Cells

Side-chain engineering as one of the most important molecular design strategies has been widely used to improve photovoltaic effi-ciency of active layer materials.Herein,a series of acceptor-n-donor-n-acceptor typed small molecule(SM)-donors(SL1,SL2,SL3,and SL4),on the basis of high-performance SM-donor BTTzR(SL1)with thiazolo[5,4-d]thiazole as the n-bridging units and 3-butylrho-danine as the terminal electron-withdrawing groups,were designed and synthesized to study the effect of the side-chain substitu-tions of BDT-T on the photovoltaic performanee.

Polymer light-emitting devices based on europium(Ⅲ) complex with 11-bromo-dipyrido[3,2-a:2′,3′-c]phenazine

Polymer light-emitting diodes(PLEDs) containing Eu(DBM)3(Br DPPz)(DBM is dibenzoylmethane, and Br DPPz is 11- bromo-dipyrido[3,2-a:2′,3′-c]phenazine) doped in a blend of poly(9,9-dioctylfluorene)(PFO) and 2-tert-butylphenyl-5- biphenyl-1,3,4-oxadiazole(PBD) as the host matrix were reported. Eu(DBM)3(Br DPPz) exhibited high thermal stability and intense UV-Vis absorption. Narrow-bandwidth red emission at 612 nm with a full width at half-maximum(FWHM) of 14.0 nm was observed from Eu(DBM)3(Br DPPz) in these double-layered PLEDs at dopant concentrations from 1 wt% to 8 wt%. For the PLED containing 1 wt% Eu(DBM)3(Br DPPz), a maximum luminance of 829 cd/m2 at 153.5 m A/cm2, highest external quantum efficiency of 1.70% at 2.1 m A/cm2 and maximum luminance of 0.74 cd/A at 4.31 m A/cm2 were obtained.

All-polymer solar cells with over 16%efficiency and enhanced stability enabled by compatible solvent and polymer additives

Considering the robust and stable nature of the active layers,advancing the power conversion efficiency(PCE)has long been the priority for all-polymer solar cells(all-PSCs).Despite the recent surge of PCE,the photovoltaic parameters of the stateof-the-art all-PSC still lag those of the polymer:small molecule-based devices.To compete with the counterparts,judicious modulation of the morphology and thus the device electrical properties are needed.It is difficult to improve all the parameters concurrently for the all-PSCs with advanced efficiency,and one increase is typically accompanied by the drop of the other(s).In this work,with the aids of the solvent additive(1-chloronaphthalene)and the n-type polymer additive(N2200),we can fine-tune the morphology of the active layer and demonstrate a 16.04%efficient all-PSC based on the PM6:PY-IT active layer.The grazing incidence wideangle X-ray scattering measurements show that the shape of the crystallites can be altered,and the reshaped crystallites lead to enhanced and more balanced charge transport,reduced recombination,and suppressed energy loss,which lead to concurrently improved and device efficiency and stability.

Broadband photomultiplication-type polymer photodetectors and its application in light-controlled circuit

Photomultiplication-type polymer photodetectors(PM-PPDs)were achieved with polymer P3HT as donor and PY3Se-1V as acceptor based on structure of ITO/PEDOT:PSS/active layer/Al.The optimal weight ratio of P3HT to PY3Se-1V is about 100:3.Amounts of isolated electron traps are formed with PY3Se-1V surrounded by P3HT due to rather less content of PY3Se-1V in active layers and about 0.94 e V energy offset between the lowest unoccupied molecular orbitals(LUMO)of P3HT and PY3Se-1V.The optimal PM-PPDs exhibit broad spectral response from 350 to 950 nm and external quantum efficiency(EQE)values of68,200%at 360 nm,26,400%at 630 nm and 19,500%at 850 nm under-15 V bias.The working mechanism of PM-PPDs is attributed to the interfacial trap-assisted hole tunneling injection from external circuit.The performance of PM-PPDs can be further improved by incorporating appropriate PMBBDT with high hole mobility as the third component.The EQE values of optimal ternary PM-PPDs are increased to 105,000%at 360 nm,40,000%at 630 nm and 31,800%at 850 nm under-15 V bias,benefiting from the enhanced hole transport in ternary active layers.The optimal ternary PM-PPDs were successfully applied in a light-controlled circuit to turn on or turn off light emitting diode(LED).