26.75 cm^(2) organic solar modules demonstrate a certified efficiency of 14.34%

Organic solar cells(OSCs)have been developed rapidly in past years,due to the fast evolution of wide-bandgap copoly-mer donors and low-bandgap non-fullerene acceptors[1−9].At present,the highest power conversion efficiencies(PCEs)for single-junction OSCs and tandem OSCs exceed 19%and 20%,respectively[10,11].These OSCs are typically fabricated by us-ing low-boiling-point solvent chloroform(CF)with an effect-ive area<0.1 cm^(2).The doctor-blading deposition is the most advantageous technique to fabricate OSCs with low-boiling-point solvent for upscaling lab cells to industrial-scale mod-ules[12],exhibiting simple operation,low cost,and high materi-al utilization[13−15].Herein,a typical OSC material system PM6:Y6(Fig.1(a))was used to fabricate OSCs modules via doc-tor-blading deposition in ambient condition,and the influ-ence of the ambient temperature and substrate temperature on the film quality was investigated.

Surface treatment on polyethylenimine interlayer to improve inverted OLED performance

Polyethylenimine(PEI) interlayer rinsing with different solvents for inverted organic light emitting diodes(OLEDs)is systematically studied in this paper. In comparison with the pristine one, the maximum current efficiency(CE) and power efficiency(PE) are enhanced by 21% and 22% for the device rinsing by ethylene glycol monomethyl ether(EEA).Little effect is found on the work function of the PEI interlayer rinsed by deionized water(DI), ethanol(EtOH), and EEA.On the other hand, the surface morphologies of PEI through different solvent treatments are quite different. Our results indicates that the surface morphology is the key to improving the device performance for IOLED as the work function of PEI keeps stable.

Nonlinear Doping, Chemical Passivation and Photoluminescence Mechanism in Water-Soluble Silicon Quantum Dots by Mechanochemical Synthesis

A series of boron- and phosphorus-doped silicon wafers are used to prepare a series of doped silicon nanocrystals （nc-Si） by high-energy ball milling with carboxylic acid-terminated surface. The sizes of the nc-Si samples are demonstrated to be 〈 S nm. The doping levels of the nc-Si are found to be nonlinearly dependent on the original doping level of the wafers by x-ray photoelectron spectroscopy measurement. It is found that the nonlinear doping process will lead to the nonlinear chemical passivation and photoluminescence （I3L） intensity evolution. The doping, chemical passivation and PL mechanisms of the doped nc-Si samples prepared by mechanochemical synthesis are analyzed in detail.

Large-Area Gravure-Printed AgNWs Electrode on Water/Oxygen Barrier Substrate for Long-Term Stable Large-Area Flexible Organic Solar Cells

Large-area AgNWs electrodes(25 cm×10 cm)were fabricated through roll-to-roll printing on the polyvinyl alcohol(PVA)modified water and oxygen barrier substrate.The modification of the barrier film with PVA improved the wettability of silver nanowires on the barrier films and led to the formation of homogenous large-area AgNWs networks.The mechanical flexibility,especially the adhesion force between the silver electrode and the barrier film substrate was dramatically improved through PVA modification.The efficiency of 13.51%for the flexible OSCs with an area of 0.64 cm2 was achieved based on the PET/barrier film/PVA/AgNWs electrode.The long-term stability showed the flexible OSCs based on the PET/barrier film/PVA/AgNWs electrode have a significantly improved stability relative to the device on PET/AgNWs electrode,and comparable air stability as the rigid device with glass/ITO device.The unencapsulated devices maintained nearly 50%of the original efficiency after storage for 600 h in air.After a simple top encapsulation,the flexible devices remained at 60%of the initial efficiency after 2000 h in the air.Therefore,the flexible AgNWs electrode based on the barrier film would have the potential to improve the air storage stability of organic flexible solar cells.

通过具有高表面能和延长共轭链段的耐溶剂空穴传输材料实现高效喷墨打印QLED

量子点发光二极管(QLED)溶液法制备的特点和喷墨打印高度契合,在印刷显示器领域展现出巨大的应用潜力.制作QLED器件时,下层薄膜的表面能对上层薄膜的铺展起着至关重要的作用,高表面能可以促进不同功能膜层之间的紧密接触并减少漏电流.然而,已报道的交联空穴传输材料(HTM)低的表面能不利于喷墨打印.在此,我们通过分子设计开发了一种可交联HTM及其聚合物,新的聚合物命名为[9-(4-(乙氧基甲基)苯基)-3-(7-(9-(4-(己炔基)乙氧基甲基)苯基)-9H-咔唑-3-基)-9H-芴]-9H-咔唑(PDA-FLCZ),由3,3′-(9,9-二甲基-9H-芴-2,7-二基)双[9-(4-(丙-2-炔-1-氧基)甲基)苯基]-9H-咔唑(DA-FLCZ)聚合得到.这种新型HTM采用原位光热交联和预聚后热交联两种交联策略,都可以在较低的交联温度下形成稳定的网络结构,具有优异的耐溶剂性和较高的表面能.通过优化交联工艺,交联PDA-FLCZ薄膜实现了更高的空穴迁移率和更低的陷阱密度,其对应的旋涂QLED器件的最大外量子效率(EQE)达到17.59%,比基于DA-FLCZ的器件(14.25%)高出23%.此外,基于交联PDA-FLCZ的喷墨打印QLED显示出15.28%的最大EQE,接近其旋涂器件值的90%.

In-situ-selective-UV crosslinking fabrication of solid liquid host guest electrolyte: A facile one-step method realizing highly flexible electrochromic device

Flexible electrochromic devices (FECDs) are promising candidates for the next generation of wearable electronics due to their low operating voltage and energy consumption. For the flexible electrochromic devices, the electrolyte is an important component. Typically, the electrolyte needs to be formulated according to the device structure and usage scenario. A high-performance electrolyte involves consideration of many factors, including choosing the right polymer, solvent, curing agent, and ion type to satisfy particular device specifications. In this work, a ultraviolet-curable solid–liquid host–guest (UV-SLHG) electrolyte is developed. Several aspects of performance are improved by introducing the solid–liquid coexisting microstructure without changing the electrolyte formulation, including excellent adhesion, a 30% increase in tensile characteristics, and a seven-fold increase in ionic conductivity when compared to a fully cured solid-state electrolyte. More importantly, the unique advantage of SLHG electrolytes lies that the thickness will not change significantly during bending. The FECD made by using the UV-SLHG-based electrolyte sustained 10,000 bending cycles at the bending radius of 2.5 mm while maintaining outstanding optical modulation. A wearable ring-type ECD and a battery-free FECD wine label were made as demonstrators. The UV-SLHG strategy is not only suitable for the FECDs but also universally applicable to other electrolyte-based of flexible electronics such as flexible capacitors and batteries.

Highly ordered inkjet-printed quantum-dot thin films enable efficient and stable QLEDs with EQE exceeding 23%

Inkjet-printed quantum dot light-emitting diodes(QLEDs)are emerging as a promising technology for next-generation displays.However,the progress in fabricating QLEDs using inkjet printing technique has been slower compared to spin-coated devices,particularly in terms of efficiency and stability.The key to achieving high performance QLEDs lies in creating a highly ordered and uniform inkjet-printed quantum dot(QD)thin film.In this study,we present a highly effective strategy to significantly improve the quality of inkjet-printed CdZnSe/CdZnS/ZnS QD thin films through a pressure-assisted thermal annealing(PTA)approach.Benefiting from this PTA process,a high quality QD thin film with ordered packing,low surface roughness,high photoluminescence and excellent electrical property is obtained.The mechanism behind the PTA process and its profound impact on device performance have been thoroughly investigated and understood.Consequently,a record high external quantum efficiency(EQE)of 23.08%with an impressive operational lifetime(T50)of up to 343,342h@100cdm−2,and a record EQE of 22.43%with T50 exceeding to 1,500,463h@100cdm−2 are achieved in inkjet-printed red and green CdZnSe-based QLEDs,respectively.This work highlights the PTA process as an important approach to realize highly efficient and stable inkjet-printed QLEDs,thus advancing QLED technology to practical applications.

Printing practice for the fabrication of flexible and stretchable electronics

Recently, flexible and stretchable electronics have experienced tremendous surge due to their promised applications in fields such as wearable electronics, portable energy devices, flexible display, and human-skin sensors. In order to fabricate flexible and stretchable electronics, a high-throughput, cost-saving, and eco-friendly manufacturing technology is required. Printing, which is an additive patterning process, can meet those requirements. In this article, printing fabrication is compared with conventional lithography process. Practices at the author's group utilizing printing for the fabrication of flexible thin-film transistors, flexible hybrid circuits and stretchable systems are presented, which has proven that printing can indeed be a viable method to fabricate flexible and stretchable electronics.

Self-assembled nanostructures of a series of linear oligothiophene derivatives adsorbed on surfaces

Many previous studies have shown that the molecular structures of oligothiophene derivatives including molecular skeleton and alkyl chains have a significant effect on their self-assemblies on the surface.In this work, a series of linear oligothiophene derivatives(DCV-n T-Hex, n = 3~11) modified with terminal dicyanovinyls and alkyl chains were adopted to further investigate the different assembly behaviors at liquid-solid interface by scanning tunneling microscopy(STM). Interestingly, via the hydrogen bonding and van der Waals interactions, DCV-3T-Hex formed zigzag and flower structures while DCV-n T-Hex(n = 4~11) formed lamellar structures. Density functional theory(DFT) calculations show that for the most energetically favorable configurations of DCV-n T-Hex, the different distribution of alkyl chains affected intermolecular interactions, and ultimately led to the different assembled structures. The zigzag and flower structures of DCV-3T-Hex had preferential thermodynamic stability compared to other structures of DCV-n T-Hex(n = 4~11). In addition, self-assembled nanostructures of DCV-n T-Hex molecules with even numbers(n = 4, 6, 8, 10) were overall more stable than those with odd numbers(n = 5, 7, 9,11), and the stability of the self-assembled structure was weakened with the extension of the molecular backbone, individually. The orientation of molecular alkyl chains was found to greatly affect the intermolecular interactions and thus leading to various self-assembly structures of DCV-n T-Hex(n = 3~11).

High performance inkjet-printed QLEDs with 18.3% EQE: improving interfacial contact by novel halogen-free binary solvent system

Poly[(9,9-dioctylfluorenyl-2,7-diyl)-alt(4,4′-(N-(4-butylphenyl))](TFB),one of the most popular and widely used hole-transport layer(HTL)materials,has been successfully applied in high performance spin-coated quantum dots-based light-emitting diodes(QLEDs)due to its suitable energy level and high mobility.However,there are still many challenging issues in inkjet-printed QLED devices when using TFB as HTL.TFB normally suffers from the interlayer mixing and erosion,and low surface energy against the good film formation.Here,a novel environment-friendly binary solvent system was established for formulating quantum dot(QD)inks,which is based on mixing halogen-free alkane solvents of decalin and n-tridecane.The optimum volume ratio for the mixture of decalin and n-tridecane was found to be 7:3,at which a stable ink jetting flow and coffee-ring free QD films could be formed.To research the influence of substrate surface on the formation of inkjet-printed QD films,TFB was annealed at different temperatures,and the optimum annealing temperature was found to enable high quality inkjet-printed QD film.Inkjet-printed red QLED was ultimately manufactured.A maximum 18.3%of external quantum efficiency(EQE)was achieved,reaching 93%of the spin-coated QLED,which is the best reported high efficiency inkjet-printed red QLEDs to date.In addition,the inkjet-printed QLED achieved similar T75 operational lifetime(27 h)as compared to the spin-coated reference QLED(28 h)at 2,000 cd·m−2.This work demonstrated that the novel orthogonal halogen-free alkane co-solvents can improve the interfacial contact and facilitate high-performance inkjet printing QLEDs with high EQE and stability.

Layer-by-layer slot-die coated high-efficiency organic solar cells processed using twin boiling point solvents under ambient condition

Layer-by-layer (LbL) strategy has been developed to form bulk heterojunction (BHJ) structure for processing efficient organic solar cells (OSCs). Herein, LbL slot-die coating with twin boiling point solvents (TBPS) strategy was developed to fabricate highly efficient OSCs, which matches with large-scale, high throughput roll-to-roll (R2R) industrialized mass process. The TBPS strategy could produce high-quality thin film without any additive, leading to the optimized vertical phase separation with interpenetrating nanostructures, as well as the enhanced charge transport and extraction. Thus, the power conversion efficiency up to 14.42% was achieved for [(2,6-(4,8-bis(5-(2-ethylhexyl-3-fluoro)thiophen-2-yl)-benzo [1,2-b:4,5-b′]dithiophene))-alt-(5,5-(1′,3′-di-2-thienyl-5′,7′-bis(2-ethylhexyl)benzo[1′,2′-c:4′,5′-c′]dithiophene-4,8-dione)]: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 (PM6:Y6) OSCs fabricated via sequentially LbL slot-die coating using the TBPS strategy under ambient condition. The research provides a potential route for industrialized production of high-efficiency and large-area OSC devices.

Large-area(64 × 64 array) inkjet-printed high-performance metal oxide bilayer heterojunction thin film transistors and n-metal-oxide-semiconductor(NMOS) inverters

It is a big challenge to construct large-scale,high-resolution and high-performance inkjet-printed metal oxide thin film transistor(TFT)arrays with independent gates for the new printed displays.Here,a self-confined inkjet printing technology has been developed to construct large-area(64×64 array),high-resolution and high-performance metal oxide bilayer(In_(2)O_(3)/IGZO)heterojunction TFTs with independent bottom gates on transparent glass substrates.Inkjet printing In_(2)O_(3) dot arrays with the diameters from 55 to 70μm and the thickness of~10 nm were firstly deposited on UV/ozone treated AlO_(x) dielectric layers,and then IGZO dots were selectively printed on the top of In_(2)O_(3) dots by self-confined technology to form In_(2)O_(3)/IGZO heterojunction channels.When the inkjet-printed IO layers treated by UV/ozone for more than 30 min or oxygen plasma for 5 min prior to print IGZO thin films,the mobility of the resulting printed In_(2)O_(3)/IGZO heterojunction TFTs are correspondingly enhanced to be 18.80 and 28.44 cm^(2) V^(-1) s^(-1) with excellent on/off ratios(>10^(8))and negligible hysteresis.Furthermore,the printed N-Metal-Oxide-Semiconductor(NMOS)inverter consisted of an In_(2)O_(3)/IGZO TFT and an IGZO TFT has been demonstrated,which show excellent performance with the voltage gain up to 112.The strategy demonstrated here can be considered as general approaches to realize a new generation of high-performance printed logic gates,circuits and display driving circuits.

Phthalimide and Naphthalimide end-Capped Diketopyrrolopyrrole for Organic Photovoltaic Applications

Two small molecules named PI-DPP and NI-DPP with a DPP core as the central strong acceptor unit and phthalimide/naphthalimide as the terminal weak acceptor were designed and synthesized. The effects of terminal phthalimide/naphthalimide units on the thermal behavior, optical and electrochemical properties, as well as the photovoltaic performance of these two materials were systematically studied. Cyclic voltammetry revealed that the lowest unoccupied molecular orbitals （LUMO） （- -3.6 eV） of both molecules were intermediate to common electron donor （P3HT） and acceptor （PCBM）. This indicated that PI-DPP and NI-DPP may uniquely serve as electron donor when blended with PCBM, and as electron acceptor when blended with P3HT, where sufficient driving forces between DPPs and PCBM, as well as between P3HT and DPPs should be created for exciton dissociation. Using as electron donor materials, PI-DPP and NI-DPP devices exhibited low power conversion efficiencies （PCEs） of 0.90% and 0.76% by blending with PCBM, respectively. And a preliminary evaluation of the potential of the NI-DPP as electron acceptor material was carried out using P3HT as a donor material, and P3HT：NI-DPP device showed a PCE of 0.6%, with an open circuit voltage （Voc） of 0.7 V, a short circuit current density （Jsc） of 1.91 mA·cm^-2, and a fill factor （FF） of 45%.

White-Light Electroluminescence with Tetraphenylethylene as Emitting Layer of Aggregation-Induced Emissions Enhancement

Tetraphenylethylene （TPE） based molecules with easy synthesis, good thermal stability, and especially their aggregation-induced emissions enhancement （AIEE） effect recently become attractive organic emitting materials due to their potentially practical application in OLEDs. Herein, the AIEE behaviors of tetraphenylethylene dyes （TMTPE and TBTPE） were investigated. Fabricated luminesent device using TMTPE dye as emitting layer displays two strong emitting bands： the blue emission coming from the first-step aggregation and the yellow emission attrib- uted to the second-step aggregation. Thus, it can be utilized to fabricate the white-light OLEDs （WOLEDs） of the single-emitting-component. A three-layer device with the brightness of 1200 cd·m^-2 and current efficiency of 0.78 cd·A^-1 emits the close to white light with the CIE coordinates of x=0.333 and y=0.358, when applied voltage from 8-13 V, verifying that the TPE-based dyes of AIEE effect can be effectively applied in single-emitting- component WOLEDs fabrication.

Thermoplastic elastomer enhanced interface adhesion and bending durability for flexible organic solar cells

Stable interface adhesion and bending durability of flexible organic solar cells(FOSCs)is a basic requirement for its real application in wearable electronics.Unfortunately,the device performance always degraded during continuous bending.Here,we revealed the weak interface adhesion force between MoO_(3) hole transporting layer(HTL)and the organic photoactive layer was the main reason of poor bending durability.The insertion of an interface bonding layer with a thermoplastic elastomer,polystyrene-blockpoly(ethylene-ran-butylene)-block-polystyrene(SEBS)effectively improved the interface adhesion force of MoO_(3) HTL and the active layer and decreased the modulus,which ensured higher than 90%of the initial efficiency remaining after 10000 bending.Meanwhile,the FOSCs gave an efficiency of 14.18%and 16.15%for the PM6:Y6 and PM6:L8-BO devices,which was among the highest performance of FOSCs.These results demonstrated the potential of improving the mechanical durability of FOSCs through thermoplastic elastomer interface modification.

Intrinsically Viscoelastic Supramolecular Conjugated Polymer toward Suppressing Coffee-Ring Effect

The rational molecular design of light-emitting conjugated polymers that inherently suppress the ubiquitous coffee-ring effect(CRE)is a great challenge and the critical bottleneck for printing displays.Herein,we describe a supramolecular route to construct an intrinsically viscoelastic rigid conjugated polymer(RCP)(PHDPF-Cz)toward avoiding the CRE without sacrificing optoelectronic properties.Theπ-πstacking interactions derived fromthe pendant carbazole(Cz)units enable PHDPF-Cz to self-assemble into criss-cross nanofibers and endow its solutionwith great viscosity.Consequently,a high-quality and continuous PHDPFCz film was obtained by impeding the transport of aggregates to the droplet edge due to outward capillary flow during evaporation,in sharp contrast to the random aggregate migration and rapid precipitation generated fromthe controlled poly[4-(6-(9H-diphenylaniline-9-yl)hexyloxy)-9,9-diphenylfluorene]-co-[5-(6-(9H-diphenylaniline-9-yl)hexyloxy)-9,9-diphenylfluorene]and poly(9,9-dioctylfluorene)solutions.Finally,an efficient random laser is also achieved based on these cross-linked films with ultrastable single-chain excitonic behavior,confirming the effectiveness of our design strategy.