Alkyl chain modulation of asymmetric hexacyclic fused acceptor synergistically with wide bandgap third component for high efficiency ternary organic solar cells

Herein,two asymmetric hexacyclic fused small molecule acceptors(SMAs),namely BP4F-HU and BP4F-UU,were synthesized.The elongated outside chains in the BP4F-UU molecule played a crucial role in optimizing the morphology of blend film,thereby improving charge mobility and reducing energy loss within the corresponding film.Notably,the PM6:BP4F-UU device exhibited a higher open-circuit voltage(V_(oc))of 0.878 V compared to the PM6:BP4F-HU device with a V_(oc)of 0.863 V.Further,a new wide bandgap SMA named BTP-TA was designed and synthesized as the third component to the PM6:BP4F-UU host binary devices,which showed an ideal complementary absorption spectrum in PM6:BP4F-UU system.In addition,BTP-TA can achieve efficient intermolecular energy transfer to BP4F-UU by fluorescence resonance energy transfer(FRET)pathway,due to the good overlap between the photoluminescence(PL)spectrum of BTP-TA and the absorption region of BP4F-UU.Consequently,ternary devices with 15wt%BTP-TA exhibits broader photon utilization,optimal blend morphology,and reduced charge recombination compared to the corresponding binary devices.Consequently,PM6:BP4F-UU:BTP-TA ternary device achieved an optimal power conversion efficiency(PCE)of 17.83%with simultaneously increased V_(oc)of 0.905 V,short-circuit current density(J_(sc))of 26.14 mA/cm^(2),and fill factor(FF)of 75.38%.

Molecular-level proton acceptor boosts oxygen evolution catalysis to enable efficient industrial-scale water splitting

Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy to produce an efficient OER catalyst that can boost industrial-scale water splitting.Molecular-level phosphate(-PO_(4))group is introduced to modify the surface of PrBa_(0.5)Ca_(0.5)Co_(2)O_(5)+δ(PBCC).The achieved catalyst(PO_(4)-PBCC)exhibits significantly enhanced catalytic performance in alkaline media.Based on the X-ray absorption spectroscopy results and density functional theory(DFT)calculations,the PO_(4)on the surface,which is regarded as the Lewis base,is the key factor to overcome the kinetic limitation of the proton transfer process during the OER.The use of the catalyst in a membrane electrode assembly(MEA)is further evaluated for industrial-scale water splitting,and it only needs a low voltage of 1.66 V to achieve a large current density of 1 A cm^(-2).This work provides a new molecular-level strategy to develop highly efficient OER electrocatalysts for industrial applications.

End-group modulation of phenazine based non-fullerene acceptors for efficient organic solar cells with high open-circuit voltage

Phenazine-based non-fullerene acceptors(NFAs)have demonstrated great potential in improving the power conversion efficiency(PCE)of organic solar cells(OSCs).Halogenation is known to be an effective strategy for increasing optical absorption,refining energy levels,and improving molecular packing in organic semiconductors.Herein,a series of NFAs(Pz IC-4H,Pz IC-4F,Pz IC-4Cl,Pz IC-2Br)with phenazine as the central core and with/without halogen-substituted(dicyanomethylidene)-indan-1-one(IC)as the electron-accepting end group were synthesized,and the effect of end group matched phenazine central unit on the photovoltaic performance was systematically studied.Synergetic photophysical and morphological analyses revealed that the PM6:Pz IC-4F blend involves efficient exciton dissociation,higher charge collection and transfer rates,better crystallinity,and optimal phase separation.Therefore,OSCs based on PM6:Pz IC-4F as the active layer exhibited a PCE of 16.48%with an open circuit voltage(Voc)and energy loss of 0.880 V and 0.53 e V,respectively.Accordingly,this work demonstrated a promising approach by designing phenazine-based NFAs for achieving high-performance OSCs.

Designing simple non-fused terthiophene-based electron acceptors for efficient organic solar cells

Low-cost photovoltaic materials are essential for realizing large-scale commercial applications of organic solar cells(OSCs).However,highly efficient OSCs based on low-cost photovoltaic materials are scarce due to a deficiency in understanding the structure-property relationship.Herein,we investigated two low-cost terthiophene-based electron acceptors,namely,3TC8 and 3TEH,with 3,4-bis(octan-3-yloxy)thiophene,differing only in the alkylated thiophene-bridges.Both acceptors exhibit low optical gaps(∼1.43 eV)and possess deep highest occupied molecular orbital(HOMO)levels(∼−5.8 eV).Notably,the single-crystal structure of 3TEH demonstrates highly planar conjugated backbone and strongπ-πstacking between intermolecular terminal groups,attributed to the presence of the bulky alkylated noncovalently conformational locks.Upon utilizing both acceptors to fabricate OSCs,the 3TC8-based device exhibited a power conversion efficiency(PCE)of 11.1%,while the 3TEH-based OSC demonstrated an excellent PCE of 14.4%.This PCE is the highest among OSCs based on terthiophene-containing electron acceptors.These results offer a new strategy for designing low-cost electron acceptors for highly efficient OSCs.

Enhancing efficiency and stability of organic solar cells through a simplified four-step synthesis of fully non-fused ring electron acceptor

Design and synthesis of superior cost-effective non-fullerene acceptors(NFAs)are still big challenges for facilitating the commercialization of organic solar cells(OSCs),yet to be realized.Herein,two medium bandgap fully non-fused ring electron acceptors(NFREAs,medium bandgap,i,e.,1,3-1,8 eV),namely PTR-2Cl and PTR-4Cl are synthesized with only four steps by using intramolecular noncovalent interaction central core,structured alkyl side chain orientation linking units and flanking with different electron-withdrawing end group.Among them,PTR-4C1 exhibits increased average electrostatic potential(ESP)difference with polymer donor,enhanced crystallinity and compactπ-πstacking compared with the control molecule PTR-2CI.As a result,the PTR-4Cl-based OSC achieved an impressive power conversion efficiency(PCE)of 14.72%,with a much higher open-circuit voltage(V_(OC))of 0.953 V and significantly improved fill factor(FF)of 0.758,demonstrating one of the best acceptor material in the top-performing fully NFREA-based OSCs with both high PCE and V_(OC).Notably,PTR-4Cl-based cells maintain a good T_80lifetime of its initial PCE after over 936 h under a continuous thermal annealing treatment and over1300 h T_(80)lifetime without encapsulation.This work provides a cost-effective design strategy for NFREAs on obtaining high V_(OC),efficient exciton dissociation,and ordered molecular packing and thus high-efficiency and stable OSCs.

Rational molecular engineering towards efficient heterojunction solar cells based on organic molecular acceptors

The selection of photoactive layer materials for organic solar cells(OSCs) is essential for the photoelectric conversion process.It is well known that chlorophyll is an abundant pigment in nature and is extremely valuable for photosynthesis.However,there is little research on how to improve the efficiency of chlorophyll-based OSCs by matching chlorophyll derivatives with excellent non-fullerene acceptors to form heterojunctions.Therefore in this study we utilize a chlorophyll derivative,Ce_(6)Me_(3),as a donor material and investigate the performance of its heterojunction with acceptor materials.Through density functional theory,the photoelectric performances of acceptors,i ncluding the fullerene derivative PC_(71)BM and the terminal halogenated non-fullerene DTBCIC series,are compared in detail.It is found that DTBCIC-C1 has better planarity,light absorption,electron affinity,charge reorganization energy and charge mobility than others.Ce_(6)Me_(3) has good energy level matching and absorption spectral complementarity with the investigated acceptor molecules and also shows good electron donor properties.Furthermore,the designed Ce_(6)Me_(3)/DTBCIC interfaces have improved charge separation and reorganization rates(K_(CS)/K_(CR)) compared with the Ce_(6)Me_(3)/PC_(71)BM interface.This research provides a theoretical basis for the design of photoactive layer materials for chlorophyll-based OSCs.

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.

Features of Recombination Radiation of GaAs Type Semiconductors with the Participation of Fine Acceptor Levels in a Magnetic Field

Using the method of Picus and Beer invariants, general expressions are obtained for the total intensity I and the degree of circular polarization Рcirc.of the luminescence of GaAs-type semiconductors with the participation of shallow acceptor levels in a longitudinal magnetic field H. Special cases are analyzed depending on the value and direction of the magnetic field strength, as well as on the constants of the g-factor of the acceptor g1,g2and the conduction band electron ge. In the case of a strong magnetic field H// [100], [111], [110], a numerical calculation of the angular dependence of the quantities I and Рcirc.was performed for some critical values of g2/g1, at which Рcirc.exhibits a sharp anisotropy in the range from −100% to +100%, and the intensity of the crystal radiation along the magnetic field tends to a minimum value.

Banana-shaped electron acceptors with an electron-rich core fragment and 3D packing capability

The emergence of Y6-type nonfullerene acceptors has greatly enhanced the power conversion efficiency(PCE)of organic solar cells(OSCs).However,which structural feature is responsible for the excellent photovoltaic performance is still under debate.In this study,two Y6-like acceptors BDOTP-1 and BDOTP-2 were designed.Different from previous Y6-type acceptors featuring an A–D–Aʹ–D–A structure,BDOTP-1,and BDOTP-2 have no electron-deficient Aʹfragment in the core unit.Instead,there is an electron-rich dibenzodioxine fragment in the core.Although this modification leads to a marked change in the molecular dipole moment,electrostatic potential,frontier orbitals,and energy levels,BDOTP acceptors retain similar three-dimensional packing capability as Y6-type acceptors due to the similar banana-shaped molecular configuration.BDOTP acceptors show good performance in OSCs.High PCEs of up to 18.51%(certified 17.9%)are achieved.This study suggests that the banana-shaped configuration instead of the A–D–Aʹ–D–A structure is likely to be the determining factor in realizing high photovoltaic performance.

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.

Metal-oxoacid-mediated oxyhydroxide with proton acceptor to break adsorption energy scaling relation for efficient oxygen evolution

Metal oxyhydroxides(MOOH)generated from irreversible reconstructions of transition metal compounds are intrinsic active species for oxygen evolution reaction,whose activities are still constrained by sluggish deprotonation kinetics and inherent adsorption energy scaling relations.Herein,we construct a tunable proton acceptor(TPA)on oxyhydroxides by in-situ reconstruction of metal oxoacids such as NiC2O4to accelerate deprotonation and break adsorption energy scaling relations during OER.The modified C_(2)O_(4)^(2-)as a TPA can easily extract H of*OH(forming*HC2O4intermediate)and then promote deprotonation by the transmitted hydrogen bond with*OOH along conjugated(H...)O=C-O(-H)chain.As a result,Ni OOH-C2O4shows non-concerted proton-electron transfer and improved deprotonation rate,and delivers a good OER activity(270 mV@10 mA cm-2).The conjugate acidity coefficient(pKa)of the modified oxoacid group can be a descriptor for TPA selection.This TPA strategy can be universally applied to Co-,Fe-,and Ni-based oxyhydroxides to facilitate OER efficiency.

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.

Single photon emitters originating from donor-acceptor pairs

Starting from the groundbreaking work in graphene[1],the active research in two-dimensional(2D)layered materials has unveiled a number of exotic phenomena that are unique in the 2D limit.In addition to the semimetal graphene,the semiconducting transition metal dichalcogenides(TMDs)and the insulating hexagonal boron nitride(hBN)are also the main driving forces of the field.

π-Extension and chlorination of non-fullerene acceptors enable more readily processable and sustainable high-performance organic solar cells

Organic solar cells(OSCs)processed without halogenated solvents and complex treatments are essential for future commercialization.Herein,we report three novel small molecule acceptors(NFAs)consisting of a Y6-like core but withπ-extended naphthalene with progressively more chlorinated end-capping groups and a longer branched chain on the Nitrogen atom.These NFAs exhibit good solubilities in nonchlorinated organic solvents,broad optical absorptions,closeπ-πstacking distances(3.63–3.84A),and high electron mobilities(~10^(-3)cm^(2)V^(-1)s^(-1)).The o-xylene processed and as-cast binary devices using PM6 as the donor polymer exhibit a PCE increasing upon progressive chlorination of the naphthalene end-capping group from 8.93%for YN to 14.38%for YN-Cl to 15.00%for YN-2Cl.Furthermore similarly processed ternary OSCs were fabricated by employing YN-Cl and YN-2Cl as the third component of PM6:CH1007 blends(PCE=15.75%).Compared to all binary devices,the ternary PM6:CH1007:YN-Cl(1:1:0.2)and PM6:CH1007:YN-2Cl(1:1:0.2)cells exhibit significantly improved PCEs of 16.49%and15.88%,respectively,which are among the highest values reported to date for non-halogenated solvent processed OSCs without using any additives and blend post-deposition treatments.

Enhanced charge separation by interchain hole delocalization in nonfullerene acceptor-based bulk heterojunction materials

Bulk heterojunction(BHJ)composites show improved power conversion efficiencies when optimized in terms of morphology using various film processing methods.A reduced carrier recombination loss in an optimized BHJ was characterized previously.However,the driving force that leads to this reduction was not clearly understood.In this study,we focus on the decreased carrier recombination loss and its driving force in optimized nonfullerene acceptor-based PTB7-Th:IEICO-4F BHJ composites.We demonstrate that the optimized BHJ shows deactivation in the sub-nanosecond nongeminate carrier recombination process.The driving force for this deactivation was determined to be the improved interchain hole delocalization between the polymers.An enhanced interchain hole delocalization was observed using steady-state photoinduced absorption(PIA)spectroscopy.In particular,increased splitting between the polaron PIA bands was noted.Moreover,improved interchain hole delocalization was observed for other state-of-the-art BHJ materials,including D18:Y6 with optimized morphologies.

A new non-fullerene acceptor based on the heptacyclic benzotriazole unit for efficient organic solar cells

Non-fullerene acceptors(NFAs)become an interesting family of organic photovoltaic materials,and have attracted considerable interest for their great potential in manufacturing large-area flexible solar panels by low cost coating methods[1–5].Recently,our group proposed in the first time an A-DA’D-A molecular strategy and synthesized a new class of non-fullerene acceptor Y6 with a record efficiency above 15%with single junction organic solar cells(OSCs)[6].To further improve the photovoltaic performance of OSCs,many effective strategies have been successfully explored,such as side-chain engineering and extension of fused core and terminal group engineering[7–12].As well-known,PCE of devices is determined by the open circuit voltage(Voc),short-circuit current density(Jsc)and fill factor(FF)[13].Among them,Voc is associated with low-lying highest occupied molecular orbital(HOMO)of donor and lowest unoccupied molecular orbital(LUMO)of acceptor of the active layer[14–16].Side-chain engineering is an effective strategy for manipulating energy levels and improving photovoltaic performance of devices[17–19].For example,introducing the alkyl/alkoxy chains can effectively tune the HOMO/LUMO energy levels[20–22].Tang et al.have reported a novel non-fullerene acceptor ITC6-IC.ITC6-IC has relatively high LUMO level and high Voc than those of ITIC due to the introduction of weak electrondonating hexyl group on thiophene[23].

用Reactor、Acceptor模式构建CORBA通信层

CORBA是一种面向对象的分布式计算环境 ,其核心部分是实现对象间的通信。为了构建通用性高、扩展性强的CORBA通信层 ,引入了Reactor模式、Acceptor模式。Reactor模式能以单进程来完成并发处理 ,而Acceptor模式有效地将服务初始化过程与服务处理过程相分离。首先阐述了Reactor模式、Acceptor模式的结构 ,包括 :句柄、同步事件多路分解器、初始分派器、具体事件处理器、Acceptor和服务处理器。然后讲述了该模式的运行过程 :如何建立连接以及如何处理服务。接着重点阐述了初始分派器、具体事件服务器、Acceptor和服务处理器的实现。并在此基础上说明了该模式的一个特性 :并发性 ;最后总结了该模式的优点和不足。

Highly crystalline acceptor materials based on benzodithiophene with different amount of fluorine substitution on alkoxyphenyl conjugated side chains for organic photovoltaics

Organic solar cells based on narrow bandgap small-molecule acceptors(SMAs)with highly crystalline characteristics have attracted great attentions for their superiority in obtaining high photovoltaic efficiency.Employing highly crystalline SMAs to enhance power conversion efficiencies(PCEs)by regulating and controlling morphology and compatibility of donor and acceptor materials has turned out to be an effective approach.In this study,we synthesized three different crystalline SMAs by using fluorine substitution on alkoxyphenyl conjugated side chains to modulate the relationship of crystallinity and morphologies,namely ZY1(zero F atoms),ZY2(two F atoms),and ZY3(four F atoms).The three SMAs show the broad absorption edges and similar frontier orbital energy levels,generating the analogical(over 0.9 V)open circuit voltage(VOC)of the polymer solar cells(PSCs).As a result,the PM6:ZY2-based PSCs yield a PCE of 10.81%with a VOC of 0.95 V,a short-circuit current density(JSC)of 16.154 mA cm^(-2),and a fill factor(FF)of 0.71,which is higher than that of 9.17%(PM6:ZY1)and 6.37%(PM6:ZY3).And the PCE(17.23%)of the PM6:Y6:ZY2 based ternary PSCs is also higher than that of 16.32%PM6:Y6 based binary device.Obviously,the results demonstrate that adding fluorine atoms on the conjugated side chains to construct high crystalline materials is a positive strategy to effectively increase the efficiencies of binary and ternary PSCs.

使用Posting Acceptor实现Form基的文件上载

许多 Web基应用都涉及到基于 From的文件上载。实现 From基的文件上载有许多方法可供选择 ,本文介绍利用微软的 Posting Acce Ptor实现基于 Form的文件上载过程以及如何实现匿名上载。

Effect of Polyaniline as Hole-Acceptor and Energy-Acceptor on the Photoluminescence of CdSe

The results of interaction between CdSe quantum dots and polyaniline were reported. Polyaniline effectively decreases the emission of CdSe quantum dots, and the CdSe luminescence lifetime is decreased by the addition of polyaniline. The mechanism of the emission observed in CdSe is assumed to result from the energy transfer and from the combination of surface-trapped electrons and holes energy is transferred from CdSe to polyaniline, and polyaniline occupies the hole sites.