Droplet morphology analysis of drop-on-demand inkjet printing

As an accurate 2D/3D fabrication tool,inkjet printing technology has great potential in preparation of micro electronic devices.The morphology of droplets produced by the inkjet printer has a great impact on the accuracy of deposition.In this study,the drop-on-demand(DoD)inkjet simulation model was established,and the accuracy of the simulation model was verified by corresponding experiments.The simulation result shows that the velocity of the droplet front and tail,as well as the time to disconnect from the nozzle is mainly affected by density(ρ),viscosity(μ)and surface tension(σ)of droplets.When the liquid filament is about to disconnect from the nozzle,the filament length and filament front velocity are found to have a linear correlation withσ/ρμand ln(ρ/(μσ1/2)).

Carbon-Based Flexible and All-Solid-State Micro-supercapacitors Fabricated by Inkjet Printing with Enhanced Performance

By means of inkjet printing technique, flexible and all-solid-state micro-supercapacitors(MSCs) were fabricated with carbon-based hybrid ink composed of graphene oxide(GO,98.0vol.%) ink and commercial pen ink(2.0vol.%). A small amount of commercial pen ink was added to effectively reduce the agglomeration of theGO sheets during solvent evaporation and the following reduction processes in which the presence of graphite carbon nanoparticles served as nano-spacer to separate GO sheets. The printed device fabricated using the hybrid ink,combined with the binder-free microelectrodes and interdigital microelectrode configuration, exhibits nearly 780%enhancement in areal capacitance compared with that of pure GO ink. It also shows excellent flexibility and cycling stability with nearly 100% retention of the areal capacitance after 10,000 cycles. The all-solid-state device can be optionally connected in series or in parallel to meet the voltage and capacity requirements for a given application.This work demonstrates a promising future of the carbonbased hybrid ink for directly large-scale inkjet printing MSCs for disposable energy storage devices.

An overview on the principle of inkjet printing technique and its application in micro-display for augmented/virtual realities

Augmented reality(AR)and virtual reality(VR)are two novel display technologies that are under updates.The essential feature of AR/VR is the full-color display that requires high pixel densities.To generate three-color pixels,the fluorescent color conversion layer inevitably includes green and red pixels.To fabricate such sort of display kits,inkjet printing is a promising way to position the color conversion layers.In this review article,the progress of AR/VR technologies is first reviewed,and in succession,the state of the art of inkjet printing,as well as two key issues-the optimization of ink and the reduction of coffee-ring effects,are introduced.Finally,some potential problems associated with the color converting layer are highlighted.

Drying-Mediated Self-Assembly of Graphene for Inkjet Printing of High-Rate Micro-supercapacitors

Scalable fabrication of high-rate micro-supercapacitors(MSCs)is highly desired for on-chip integration of energy storage components.By virtue of the special self-assembly behavior of 2D materials during drying thin films of their liquid dispersion,a new inkjet printing technique of passivated graphene micro-flakes is developed to directly print MSCs with 3D networked porous microstructure.The presence of macroscale through-thickness pores provides fast ion transport pathways and improves the rate capability of the devices even with solid-state electrolytes.During multiple-pass printing,the porous microstructure effectively absorbs the successively printed inks,allowing full printing of 3D structured MSCs comprising multiple vertically stacked cycles of current collectors,electrodes,and sold-state electrolytes.The all-solid-state heterogeneous 3D MSCs exhibit excellent vertical scalability and high areal energy density and power density,evidently outperforming the MSCs fabricated through general printing techniques.

Single droplet formation by controlling the viscoelasticity of polymer solutions during inkjet printing

Inkjet printing has emerged as a potential solution processing method for large-area patterned films.During inkjet printing,a single droplet without satellite droplet is required for high-quality film.Herein,we propose a strategy for obtaining a single droplet by adjusting the reduced concentration(c/c^(*),where c^(*)is the critical overlap concentration)in the range of 1.0-1.5.Droplet formation can be categorized into three distinct regimes:(1)c/c^(*)<1.0,satellite droplet;(2)c/c^(*)=1.0-1.5,single droplet;(3)c/c^(*)>2.0,no droplet.Furthermore,an inertial-capillary balance led to the 2/3-power scaling of the minimum radius with time for the solutions of c/c^(*)<1.0.However,for the solutions of c/c^(*)=1.0-1.5,the ligament radius decreased exponentially with time.Moreover,the Weissenberg number was higher than the critical value of 0.5,indicating that the polymer chains underwent coil-stretch transition.The viscoelastic-capillary balance dominated instead of the inertial-capillary balance.The resulting viscoelastic resistance reduced the length of the ligament and increased the velocity difference between the satellite and main droplets.Consequently,a single droplet was formed.In addition,the law can be successfully generalized to various molecular weights,molecular structures and solvents.

Additive manufacturing of thin electrolyte layers via inkjet printing of highly-stable ceramic inks

Inkjet printing is a promising alternative for the fabrication of thin film components for solid oxide fuel cells(SOFCs) due to its contactless, mask free, and controllable printing process. In order to obtain satisfying electrolyte thin layer structures in anode-supported SOFCs, the preparation of suitable electrolyte ceramic inks is a key. At present, such a kind of 8 mol% Y_(2)O_(3)-stabilized ZrO_(2)(8 YSZ) electrolyte ceramic ink with long-term stability and high solid loading(> 15 wt%) seems rare for precise inkjet printing, and a number of characterization and performance aspects of the inks, such as homogeneity, viscosity, and printability, should be studied. In this study, 8 YSZ ceramic inks of varied compositions were developed for inkjet printing of SOFC ceramic electrolyte layers. The dispersing effect of two types of dispersants, i.e., polyacrylic acid ammonium(PAANH4) and polyacrylic acid(PAA), were compared. The results show that ultrasonic dispersion treatment can help effectively disperse the ceramic particles in the inks. PAANH4 has a better dispersion effect for the inks developed in this study. The inks show excellent printable performance in the actual printing process. The stability of the ink can be maintained for a storage period of over 30 days with the help of initial ultrasonic dispersion. Finally, micron-size thin 8 YSZ electrolyte films were successfully fabricated through inkjet printing and sintering, based on the as-developed high solid loading 8 YSZ inks(20 wt%). The films show fully dense and intact structural morphology and smooth interfacial bonding, offering an improved structural quality of electrolyte for enhanced SOFC performance.

Inkjet printing for electroluminescent devices： emissive materials, film formation, and display prototypes

Inkjet priming （IJP） is a versatile technique for realizing high-accuracy patterns in a cost-effective manner. It is considered to be one of the most promising candidates to replace the expensive thermal evaporation technique, which is hindered by the difficulty of fabricating low-cost, large electroluminescent devices, such as organic light- emitting diodes （OLEDs） and quantum dot light-emitting diodes （QLEDs）. In this invited review, we first introduce the recent progress of some printable emissive materials, including polymers, small molecules, and inorganic colloidal quantum dot emitters in OLEDs and QLEDs. Subsequently, we focus on the key factors that influence film formation. By exploring stable ink formulation, selecting print parameters, and implementing droplet deposition control, a uniform film can be obtained, which in turn improves the device performance. Finally, a series of impressive inkjet-printed OLEDs and QLEDs prototype display panels are summarized, suggesting a promising future for IJP in the fabrication of large and high-resolution flat panel displays.

Effects of the actuation waveform on the drop size reduction in drop-on-demand inkjet printing

In this study the effects of the actuation waveforms on the droplet generation in a drop-on-demand inkjet printing are studied systematically by numerical simulations.Two different types of waveforms,namely the unipolar and bipolar actuations,are investigated for three fluids with different physical properties.We focus on two key parameters,which are the dwell time and the velocity amplitude.For the unipolar driving,the ejection velocity and the ejected liquid volume are both increased as the velocity amplitude becomes larger.The dwell time only has minor effects on both the ejection velocity and the ejected liquid volume.The ejection velocity decreases significantly for large liquid viscosity,while the influences of viscosity on the ejected liquid volume are much weaker.Four different droplet morphologies and the corresponding parameter ranges are identified.The droplet radius can be successfully reduced to about 40%e of the nozzle exit radius.For the bipolar waveforms,same droplet morphologies are observed but with shifted boundaries in the phase space.The minimal radius of stable droplet produced by the bipolar waveforms is even smaller compared to the unipolar ones.

Inkjet printing technology for increasing the I/O density of 3D TSV interposers

Interposers with through-silicon vias(TSVs)play a key role in the three-dimensional integration and packaging of integrated circuits and microelectromechanical systems.In the current practice of fabricating interposers,solder balls are placed next to the vias;however,this approach requires a large foot print for the input/output(I/O)connections.Therefore,in this study,we investigate the possibility of placing the solder balls directly on top of the vias,thereby enabling a smaller pitch between the solder balls and an increased density of the I/O connections.To reach this goal,inkjet printing(that is,piezo and super inkjet)was used to successfully fill and planarize hollow metal TSVs with a dielectric polymer.The under bump metallization(UBM)pads were also successfully printed with inkjet technology on top of the polymer-filled vias,using either Ag or Au inks.The reliability of the TSV interposers was investigated by a temperature cycling stress test(−40℃ to+125℃).The stress test showed no impact on DC resistance of the TSVs;however,shrinkage and delamination of the polymer was observed,along with some micro-cracks in the UBM pads.For proof of concept,SnAgCu-based solder balls were jetted on the UBM pads.

Recent advances in inkjet printing synthesis of functional metal oxides

lnkjet printing （IJP） synthesis has emerged as a useful technique for the fabrication of functional metal oxides in the fields of nanotechnology and materials science. In this paper, we will review the fundamental state-of-the-art principles of the special ink formulations used for IJP synthesis of functional metal oxides and the applications of these oxides.

Zwitterion-assisted transition metal dichalcogenide nanosheets for scalable and biocompatible inkjet printing

Inkjet printing of two-dimensional(2D)transition metal dichalcogenide(TMD)nanosheets fabricated by liquid-phase exfoliation(LPE)allows simple,mass-producible,and low-cost photo-electronic devices.Many LPE processes involve toxic and environmentally hazardous solvents;however,dispersants have restricted the extent of applications of 2D-TMD inks.Herein,various 2D-TMD nanosheets,including MoS2,MoSe2,WS2,and WSe2,in addition to few-layered graphene,are inkjet-printed using a LPE process based on zwitterionic dispersants in water.Zwitterions with cationic and anionic species are water-soluble,while alkyl chain moieties associated with two ionic species adhere universally on the surface of TMD nanosheets,resulting in high throughput liquid exfoliation of the nanosheets.The zwitterion-assisted TMD nanosheets in water are successtully employed as an ink without the need for additives to adjust the viscosity and surface tension of the ink for use in an office inkjet printer;this gives rise to A4 scale,large-area inkjet-printed images on diverse substrates,such as metals,oxides,and polymer substrates patchable onto human skin.Combination with conductive graphene nanosheet inks allowed the development of mechanically flexible,biocompatible-printed arrays of photodetectors with pixelated MoSe2 channels on a paper exhibiting a photocurrent ON/OFF ratio of approximately 1038 and photocurrent switching of 500 ms.

Inkjet printing of epitaxially connected nanocrystal superlattices

Access to a blossoming library of colloidal nanomaterials provides building blocks for complex assembled materials.The journey to bring these prospects to fruition stands to benefit from the application of advanced processing methods.Epitaxially connected nanocrystal(or quantum dot)superlattices present a captivating model system for mesocrystals with intriguing emergent properties.The conventional processing approach to creating these materials involves assembling and attaching the constituent nanocrystals at the interface between two immiscible fluids.Processing small liquid volumes of the colloidal nanocrystal solution involves several complexities arising from the concurrent spreading,evaporation,assembly,and attachment.The ability of inkjet printers to deliver small(typically picoliter)liquid volumes with precise positioning is attractive to advance fundamental insights into the processing science,and thereby potentially enable new routes to incorporate the epitaxially connected superlattices into technology platforms.In this study,we identified the processing window of opportunity,including nanocrystal ink formulation and printing approach to enable delivery of colloidal nanocrystals from an inkjet nozzle onto the surface of a sessile droplet of the immiscible subphase.We demonstrate how inkjet printing can be scaled-down to enable the fabrication of epitaxially connected superlattices on patterned sub-millimeter droplets.We anticipate that insights from this work will spur on future advances to enable more mechanistic insights into the assembly processes and new avenues to create high-fidelity superlattices.

Efficient emission of quasi-two-dimensional perovskite films cast by inkjet printing for pixel-defined matrix light-emitting diodes

Quasi-two-dimensional(quasi-2D)perovskites are promising materials for potential application in light-emitting diodes(LEDs)due to their high exciton binding energy and efficient emission.However,their luminescent performance is limited by the low-n phases that act as quenching luminescence centers.Here,a novel strategy for eliminating low-n phases is proposed based on the doping of strontium bromide(SrBr_(2))in perovskites,in which SrBr_(2)is able to manipulate the growth of quasi-2D perovskites during their formation.It was reasonably inferred that SrBr_(2)readily dissociated strontium ions(Sr^(2+))in dimethyl sulfoxide solvent,and Sr^(2+)was preferentially adsorbed around[PbBr_(6)]^(4−)through strong electrostatic interaction between them,leading to a controllable growth of quasi-2D perovskites by appropriately increasing the formation energy of perovskites.It has been experimentally proved that the growth can almost completely eliminate low-n phases of quasi-2D perovskite films,which exhibited remarkably enhanced photoluminescence.A high electroluminescent efficiency matrix green quasi-2D perovskite-LED(PeLED)with a pixel density of 120 pixels per inch fabricated by inkjet printing technique was achieved,exhibiting a peak external quantum efficiency of 13.9%,which is the most efficient matrix green quasi-2D PeLED so far to our knowledge.

Efficient red perovskite quantum dot light-emitting diode fabricated by inkjet printing

Perovskite quantum dots(PeQDs)are considered potential display materials due to their high color purity,high photoluminescence quantum yield(PLQY),low cost and easy film casting.In this work,a novel electroluminescence(EL)device consisting of the interface layer of long alkyl-based oleylammonium bromide(OAmBr),which passivates the surface defects of PeQDs and adjusts the carrier transport properties,was designed.The PLQY of the OAmBr/PeQD bilayer was significantly improved.A high-performance EL device with the structure of indium tin oxide/poly(3,4-ethylenedioxythiophene)polystyrene sulfonate/poly(bis(4-phenyl)(2,4,6-trimethylphenyl)amine)/OAmBr/PeQDs/2,2′,2′′-(1,3,5-benzinetriyl)-tris(1-phenyl-1H benzimidazole)/LiF/Al was constructed using a spin-coating method.A peak external quantum efficiency(EQE)of 16.5%at the emission wavelength of 646 nm was obtained.Furthermore,an efficient matrix EL device was fabricated using an inkjet printing method.A high-quality PeQD matrix film was obtained by introducing small amounts of polybutene into the PeQDs to improve the printing process.The EQE reached 9.6%for the matrix device with 120 pixels per inch and the same device structure as that of the spin-coating one.

A Dielectric Ink Combining Acrylate and Cyanate Moieties for Inkjet 3D Printing with Good Thermal Stability

Inkjet 3D printing has potential in the additive manufacturing of electronic circuits and devices.However,inks that can be used for printing layers with T5%>300℃ or hardness>200 MPa have been rarely reported.Cyanate ester(CE)polymers have excellent thermal stability,high strength,and low shrinkage compared to other common dielectric inks for inkjet 3D printing,but cannot be quickly shaped by ultraviolet(UV)irradiation or thermal treatment.Combining CEs with UV-curable monomers may be a possible way to accelerate crosslinking,but there are challenges from the adverse effects of the dilution of both monomers.In this study,dielectric inks with acrylate and cyanate moieties were developed.The low viscosity and surface tension of the CE precursor(Bisphenol E cyanate ester)were combined with photocurable acrylate diluent monomers and cross-linker to realize an ink suitable for inkjet 3D printing.An internal dual three-dimensional cross-linked network structure resin was prepared by a combination of photocuring and thermal curing with T5%up to 326.69℃,hardness up to 431.84 MPa,dielectric constant of 2.70 at 8 GHz,and shrinkage of 1.64%.The developed dielectric inks can be applied to the 3D printing of printed circuit boards and other electronic devices that require dielectric properties.

Programmable robotized‘transfer-and-jet’printing for large,3D curved electronics on complex surfaces

Large,3D curved electronics are a trend of the microelectronic industry due to their unique ability to conformally coexist with complex surfaces while retaining the electronic functions of 2D planar integrated circuit technologies.However,these curved electronics present great challenges to the fabrication processes.Here,we propose a reconfigurable,mask-free,conformal fabrication strategy with a robot-like system,called robotized‘transfer-and-jet’printing,to assemble diverse electronic devices on complex surfaces.This novel method is a ground-breaking advance with the unique capability to integrate rigid chips,flexible electronics,and conformal circuits on complex surfaces.Critically,each process,including transfer printing,inkjet printing,and plasma treating,are mask-free,digitalized,and programmable.The robotization techniques,including measurement,surface reconstruction and localization,and path programming,break through the fundamental constraints of 2D planar microfabrication in the context of geometric shape and size.The transfer printing begins with the laser lift-off of rigid chips or flexible electronics from donor substrates,which are then transferred onto a curved surface via a dexterous robotic palm.Then the robotic electrohydrodynamic printing directly writes submicrometer structures on the curved surface.Their permutation and combination allow versatile conformal microfabrication.Finally,robotized hybrid printing is utilized to successfully fabricate a conformal heater and antenna on a spherical surface and a flexible smart sensing skin on a winged model,where the curved circuit,flexible capacitive and piezoelectric sensor arrays,and rigid digital–analog conversion chips are assembled.Robotized hybrid printing is an innovative printing technology,enabling additive,noncontact and digital microfabrication for 3D curved electronics.

New Silica Coating Pigment for Inkjet Papers from Mining Industry Sidestreams

Silica is commonly used as an ingredient in the coatings of inkjet papers because of its capability to provide a coating layer structure combining a high pore volume, into which all the applied inkjet ink can transfer, and a suitable pore size distribution for very quick ink absorption. Nowadays, the production of silica pigment is quite expensive, and therefore, it would be advantageous to find a cheaper raw material source. In this study, the raw material was Greek olivine from magnesite mine sidestreams. The silica pigment was produced at laboratory scale by using nitric acid as a solvent. The target of this work was to clarify how this produced silica pigment is suited for inkjet coating pigments. The coating colors were applied by a laboratory rod coater on fine base paper and white-top kraftliner, and the coated surfaces were printed with a home and office area inkjet printer. The results showed that the produced olivine-based silica pigment has a potential in matt inkjet coatings. The coating of the produced silica pigment increased the print density, decreased the print-through, and diminished the bleeding of fine paper and white-top kraftliner board. However, further development work is needed to improve the pigment brightness to a more acceptable level, and to control the particle size at the nitric acid dissolution.

Electrohydrodynamic direct-writing of conductor–insulator–conductor multi-layer interconnection

A multi-layer interconnection structure is a basic component of electronic devices, and printing of the multi-layer interconnection structure is the key process in printed electronics. In this work, electrohydrodynamic direct-writing （EDW） is utilized to print the conductor-insulator--conductor multi-layer ~nterconne^ction structure. Silver ink is chosen to print the conductor pattern, and a polyvinylpyrrolidone （PVP） solution is util^zed to f^bricate the insulator layer between the bottom and top conductor patterns. The influences of EDW process parameters on the line width of the printed conductor and insulator patterns are studied systematically. The obtained ~es^l~s show that the line width of the printed structure increases with the increase of the flow rate, but decreases with the increase of applied voltage and PVP content in the solution. The average resistivity values of the bottom and top silver conductor tracks are determined to be 1.34 × 10-7 Ω.m and 1.39×10-7 Ω.m, respectively. The printed PVP layer between the two conductor tracks is well insulated, which can meet the insulation requirement of the electronic devices. This study offers an alternative, fast, and cost-effective method of fabricating conductor-insulator-conductor multi-layer interconnections in the electronic industry.

Extrusion-Based 3D-Printed Supercapacitors:Recent Progress and Challenges

Supercapacitors have been regarded as promising power supplies for future electronics due to their high power density,superior stability,easy integration,and safety.Extrusion-based three-dimensional printing technologies hold promise to satisfy the demands for integrated and flexible supercapacitors because of their highly versatile manufacturing process.In this review article,a comprehensive and timely review of these state-of-theart technologies is presented.We start with a brief introduction of fundamental concepts of supercapacitors,including energy storage mechanisms and device structures.Then,the latest progress of extrusionbased three-dimensional printing technologies(e.g.,fused deposition modeling,inkjet printing,and direct ink writing)along with their applications for manufacturing supercapacitors is summarized.The choice of printable materials(e.g.,graphene,carbon nanotubes,metal oxides,and MXenes),printing process,and the resulted electrochemical performances of supercapacitors are especially emphasized.Finally,the development of extrusion-based three-dimensional printing supercapacitors is summarized,with existing challenges diagnosed,possible solutions proposed,and future outlooks forecasted.We hope this review can offer insights to further improve the performance of three-dimensional-printed supercapacitors for practical applications.

Inkjet printed large-area flexible circuits:a simple methodology for optimizing the printing quality

In this work, a simple methodology was developed to enhance the patterning resolution of inkjet printing, involving process optimization as well as substrate modification and treatment. The line width of the inkjetprinted silver lines was successfully reduced to 1/3 of the original value using this methodology. Large-area flexible circuits with delicate patterns and good morphology were thus fabricated. The resultant flexible circuits showed excellent electrical conductivity as low as 4.5 Ω/□ and strong tolerance to mechanical bending. The simple methodology is also applicable to substrates with various wettability, which suggests a general strategy to enhance the printing quality of inkjet printing for manufacturing high-performance large-area flexible electronics.