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Results for “Layer-by-Layer Fabrication”

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At least 19 records

A Top-Down Strategy to Engineer ActiveLayer Morphology for Highly Efficient and Stable All-Polymer Solar Cells

A major challenge hindering the further development of all-polymer solar cells (all-PSCs) employing polymerized small-molecule acceptors is the relatively low fill factor (FF) due to the difficulty in controlling the active-layer morphology. The issues typically arise from oversized phase separation resulting from the thermodynamically unfavorable mixing between two macromolecular species, and disordered molecular orientation/packing of highly anisotropic polymer chains. Herein, a facile top-down controlling strategy to engineer the morphology of all-polymer blends is developed by leveraging the layer-by-layer (LBL) deposition. Optimal intermixing of polymer components can be achieved in the two-step process by tuning the bottom-layer polymer swelling during top-layer deposition. Consequently, both the molecular orientation/packing of the bottom layer and the molecular ordering of the top layer can be optimized with a suitable top-layer processing solvent. A favorable morphology with gradient vertical composition distribution for efficient charge transport and extraction is therefore realized, affording a high all-PSC efficiency of 17.0% with a FF of 76.1%. The derived devices also possess excellent long-term thermal stability and can retain >90% of their initial efficiencies after being annealed at 65 °C for 1300 h. In conclusion, these results validate the distinct advantages of employing an LBL processing protocol to fabricate high-performance all-PSCs.

14 SOLAR ENERGY↗

Rational Regulation of Layer‐by‐Layer Processed Active Layer via Trimer‐Induced Pre‐Swelling Strategy for Efficient and Robust Thick‐Film Organic Solar Cells

Thick-film (>300 nm) organic solar cells (OSCs) have garnered intensifying attention due to their compatibility with commercial roll-to-roll printing technology for the large-scale continuous fabrication process. However, due to the uncontrollable donor/acceptor (D/A) arrangement in thick-film condition, the restricted exciton splitting and severe carrier traps significantly impede the photovoltaic performance and operability. For this work, combined with layer-by-layer deposition technology, a twisted 3D star-shaped trimer (BTT-Out) is synthesized to develop a trimer-induced pre-swelling (TIP) strategy, where the BTT-Out is incorporated into the buried D18 donor layer to enable the fabrication of thick-film OSCs. The integrated approach characterizations reveal that the exceptional configuration and spontaneous self-organization behavior of BTT-Out trimer could pre-swell the D18 network to facilitate the acceptor's infiltration and accelerate the formation of D/A interfaces. This enhancement triggers the elevated polarons formation with amplified hole-transfer kinetics, which is essential for the augmented exciton splitting efficiency. Furthermore, the regulated swelling process can initiate the favorable self-assembly of L8-BO acceptors, which would ameliorate carrier transport channels and mitigate carrier traps. As a result, the TIP-modified thin-film OSC devices achieve the champion performance of 20.3% (thin-film) and 18.8% (thick-film) with upgraded stability, among one of the highest performances reported of thick-film OSCs.

36 MATERIALS SCIENCE↗

Scalable Layer-by-Layer Electrospray-Assisted Interfacial Polymerization: Enabling Large-Area Polyamide Membrane Fabrication

Layer-by-layer electrospray-assisted interfacial polymerization (LBL-EAIP) has recently been proposed as an alternative approach for fabricating polyamide membranes with precisely controlled thickness and polymerization degree, showing great potential for reverse osmosis (RO) membrane synthesis. In this article, we report a scale-up strategy for LBL-EAIP to enable its practical application in RO membrane manufacturing. A multi-jet electrospray apparatus was developed, and the device configuration and process parameters were carefully adjusted to produce polyamide-on-polyethersulfone thin film composite (TFC) membranes with consistently high salt rejection and water permeance across the membrane area. Specifically, an average 97.1% NaCl rejection from a 2000 ppm NaCl feed was achieved with an area-to-area deviation of 1%, along with a deionized water permeance of 0.90 ± 0.11 LMH/bar at 15 bar feed pressure. In addition, a Fourier-transform infrared spectroscopy (FTIR)-based analytical method was developed for semi-quantitative assessment of membrane thickness and compositional uniformity, enabling rapid mapping of film microstructure and chemical variations. This work provides a pathway to scale up LBL-EAIP technology, bridging the gap between laboratory-scale innovation and industrial-scale manufacturing.

Feng, Yue (ORCID:0000000221343980)↗

Vacuum-Free, All-Solution, and All-Air Processed Organic Photovoltaics with over 11% Efficiency and Promoted Stability Using Layer-by-Layer Codoped Polymeric Electrodes

Nonfullerene organic photovoltaics (OPVs) have achieved a breakthrough in pushing the efficiency beyond 15%. Although this sheds light on OPV commercialization, the high cost associated with the scalable device fabrications remains a giant challenge. Herein, a vacuum-free, all-solution and all-air processed OPV is reported that yields 11.12% efficiency with a fill factor of 0.725, due to the usages of high-merit polymeric electrodes and modified active blends. The design principle toward the high-merit electrodes is to induce heavy acid doping into the matrices for a raised carrier concentration and mobility, make a large removal of insulating components in the whole matrices rather than surfaces, and restrain the formation of large-domain aggregates. A unique layer-by-layer doping is developed to enable the polymeric electrodes with record-high trade-offs between optical transmittance and electrical conductivity. Moreover, solvent vapor annealing is proposed to boost device efficiency and it has the advantages of finely adjusting the active blend morphology and raising the electron mobility. The resulting devices are highly efficient and most (≈91%) of the initial efficiency are maintained in 30 day storage. Finally, this work indicates bright future for making cost-effective all-solution processed OPVs in air.

14 SOLAR ENERGY↗

Highly Efficient Layer-by-Layer Processed Quaternary Organic Solar Cells with Improved Charge Transport and Reduced Energy Loss

We report how to improve charge transport properties and reduce energy losses are the two main challenges of organic solar cells (OSCs). Herein, a new device fabrication strategy that combines the layer-by-layer (LBL) method and a quaternary active layer is demonstrated to realize highly efficient photovoltaic performance of the OSCs based on PM6:PM7/Y6:O1-2F. The introduction of the second donor, PM7,forms a cascade energy-level alignment with PM6 that facilitates effective charge transfer. The second acceptor, O1-2F, which is poorly miscible with the donors, helps to reduce the miscibility between the donors and acceptors, and thus delivers a more desirable vertical phase separation of the active layer. Furthermore, the alloy acceptor of O1-2F and Y6 can optimize the horizontal and vertical morphology of the active layer, forming an effective charge separation and continuous charge transport channel. As a result, the PM6:PM7/Y6:O1-2F system shows a distinct increase in charge mobility and a reduced nonradiative lossΔVnrof 0.231 V compared to the PM6/Y6 system, achieving a high-power conversion efficiency of18.23%. The results indicate that the quaternary LBL OSCs are promising for future large-scale and industrial manufacture of the OSCs.

14 SOLAR ENERGY↗

Layer-by-Layer-Processed Organic Solar Cells with 18.02% Efficiency Enabled by Regulating the Aggregation of Bottom Polymers

The fabrication of organic solar cells (OSCs) by a layer-by-layer (LBL) method has attracted growing attention in recent years. As already known, the pre-aggregates of conjugated polymers in solution have a profound impact on their microstructure morphology in films. Herein, by simply controlling the solution temperature and annealing processes, the pre-aggregation behavior of D18 polymer in solution can be fine-tuned and the microstructure of D18 bottom layer is well manipulated. The optimized D18 bottom layer can effectively regulate L8-BO upper-layer-forming suitable networks for efficient charge transportation. In addition, a vertical phase separation with a special D/D:A/A structure (P-i-N-type component distribution) is also formed. As a result, compared to the 16.43% power conversion efficiency (PCE) of the bulk heterojunction devices, such control enables bilayer OSC devices based on the polymer D18 and L8-BO to deliver an enhanced PCE of 18.02% with simultaneously improved short-circuit current density, open-circuit voltage, and fill factor. Importantly, it is also demonstrated in these results that the LBL deposition process utilizing the pre-aggregation of polymer and its fiber-network-forming ability is a very promising approach to improve charge dynamics, suppress carrier recombination, and fabricate highly efficient OSCs.

14 SOLAR ENERGY↗

An experimental investigation of the effectiveness of Ar-CO 2 shielding gas mixture for the wire arc additive process

Wire arc additive manufacturing (AM) is the process by which a large, metallic structure is built layer-by-layer using a welding arc to melt a wire feedstock. A novel opportunity exists to alter the shielding gas composition to fabricate distinct geometrical features without altering the other AM parameters. In this paper, shielding gases with varied concentrations of Argon (Ar) and CO 2 was used to deposit three distinct geometric shapes (walls, infill, and overhang) using a wire-based additive manufacturing system utilizing the gas metal arc welding (GMAW) surface tension transfer (STT) process. Computer-aided design (CAD) models were sliced with a custom-built slicer, and the sliced algorithm was converted into optimal robotic toolpaths. A custom virtual instrument (VI) was built in LabVIEW to compare the temperature profiles on the surface during each deposition process. After each deposition, the geometric features were scanned, and the surface waviness value was evaluated. Tensile and Charpy impact coupons were extracted from the wall geometries in the longitudinal and transverse directions and tested. The results indicated that a higher CO 2 content produced higher melt pool temperatures to an extent, while lower contents of CO 2 resulted in a dimensionally accurate geometry. The data also indicated that the 2%/98% CO 2 /Ar blend produced scatter in tensile strength and the analysis of variance (ANOVA) shows significant difference. However, the intermediate range of CO 2 (5–10%) resulted in uniform tensile properties. Altogether, these results indicate that a 5%/95% CO 2 /Ar blend is the ideal shielding gas for lowering process temperatures and improving mechanical properties in wire arc additive manufacturing using the gas metal arc welding surface tension transfer process. Additionally, varying concentrations of Ar/CO 2 can be used within the same part in order to modify the local properties or process parameters such as strength, toughness, temperature, or dimensional features. This may improve overall manufacturing quality without sacrificing specific properties.

42 ENGINEERING↗

Melt Pool and Heat Treatment Optimization for the Fabrication of High-Strength and High-Toughness Additively Manufactured 4340 Steel

Additively manufactured (AM) components offer superior design flexibility compared to their conventionally manufactured counterparts, and optimizing processing parameters is key to achieving high-quality depositions with desirable and predictable mechanical properties. This study was focused on 4340 steel fabricated using laser powder bed fusion (LPBF), and 42 laser power and scan speed combinations have been systematically investigated to determine an optimized melt pool geometry that would ensure fully-dense parts. The AM material was compared with a wrought 4340 equivalent and studied in two customized heat treated conditions, optimized for strength and toughness, respectively. The microstructures of the as-fabricated and heat treated AM and wrought materials were characterized to assess differences introduced by the layer-by-layer fabrication process and subsequent heat treatment. Tensile properties of both materials were also evaluated and demonstrate that the AM materials offer equal or superior properties compared to the wrought equivalents. Differences in fracture surface morphologies indicate the distinct failure mechanisms associated with the materials’ characteristic microstructures, and the role of inclusions in the failures was studied to elucidate these differences. Complementary to the experimental investigations, the dataset was leveraged to make recommendations for future design of experiments to optimize AM build parameters in other material systems. A statistical Monte Carlo analysis was used to predict the interpolation error produced using reduced datasets and to enable informed processing parameters selection. These findings are discussed to make recommendations for the use of AM materials for high-integrity structural applications.

36 MATERIALS SCIENCE↗

In-situ quantification of the surface roughness for facile fabrications of atomically smooth thin films

Here in this work we present an in-situ technique to quantify the layer-by-layer roughness of thin films and heterostructures by measuring the spectral profile of the reflection high-energy electron diffraction (RHEED). The characteristic features of the diffraction spot, including the vertical to lateral size ratio c/b and the asymmetrical ratio c 1 /c 2 along the vertical direction, are found to be quantitatively dependent on the surface roughness. The quantitative relationships between them are established and discussed for different incident angles of high-energy electrons. As an example, the surface roughnesses of LaCoO 3 films grown at different temperatures are obtained using such an in-situ technique, which are confirmed by the ex-situ atomic force microscopy. Moreover, the in-situ measured layer-by-layer roughness oscillations of two LaCoO 3 films are demonstrated, revealing drastically different information from the intensity oscillations. The experiments assisted with the in-situ technique demonstrate an outstanding high resolution down to similar to ~0.1 Å. Therefore, the new quantitative RHEED technique with real-time feedbacks significantly escalates the thin film synthesis efficiency, especially for achieving atomically smooth surfaces and interfaces. It opens up new prospects for future generations of thin film growth, such as the artificial intelligence-assisted thin film growth.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Extrusion parameter control optimization for DIW 3D printing using image analysis techniques

Material extrusion is a well-recognized facet of additive manufacturing that involves the fabrication of parts through the deposition of structural material from an extrusion head from a bulk supply. In the subdivision of Direct Ink Writing (DIW) additive manufacturing, challenges arise when the structural material is flowable, synchronous extrusion control and tool movement becomes critical for achieving high-quality parts with low defect populations. DIW techniques are most used in laboratory settings using expensive custom instruments and may require specialized 3D slicing software. Here, in this study, the fabrication of an inexpensive, consumer-friendly progressive cavity pump dispensing system is detailed, in which can create high-quality parts by executing G-code commands produced from a commercial slicing software. The precision and repeatability of the movement-synchronized material extrusion is demonstrated through a series of optimization schemes, entailing the alteration of various control parameters, which directly affect the extrusion properties demonstrated during a print. In situ diagnostics were implemented to evaluate the results of the established optimization experiment. Using a machine vision technique, images of the optimization prints are processed. Following this, a supervised machine learning model was trained to autonomously judge whether or not the extrusion parameters produced a passing or failing result. The machine learning scheme serves as a preliminary benchmark for future layer-by-layer evaluation of more complex DIW parts. The construction of the printer and development of in situ characterization capabilities demonstrates the ability for this printer to create high-fidelity DIW parts for a fraction of the price of other systems.

42 ENGINEERING↗

Island scanning pattern optimization for residual deformation mitigation in laser powder bed fusion via sequential inherent strain method and sensitivity analysis

Laser powder bed fusion (L-PBF) has emerged as one of the mainstream additive manufacturing approaches for fabricating metal parts with complex geometries and intricate internal structures. However, large deformation associated with rapid heating and cooling can lead to build failure and requires post-processing which may increase manufacturing cost and prolong the production period. Here in this work, an island scanning pattern design method is proposed to optimize the scanning direction of each island in order to reduce part deformation after cutting off the build platform. The objective of this optimization is to minimize the upward bending of the part after sectioning, which allows the part deformation to satisfy the tolerance requirement or reduce the post heat treatment time. Inherent strain method is employed in the sequential finite element analysis consisting of layer-by-layer activations and sectioning for fast residual distortion prediction. Full sequential sensitivity analysis for the formulated optimization is provided to update the island scanning directions. To show the feasibility and effectiveness of the proposed method, the scanning patterns of a block structure and a connecting rod were designed and parts were fabricated using an open architecture L-PBF machine. The fabrication experiments demonstrated that the residual deformation of both parts fabricated by optimized scanning pattern can be reduced by over 50% compared to the initial scanning patterns, which demonstrate the effectiveness of the proposed method.

36 MATERIALS SCIENCE↗

In situ laser profilometry for material segmentation and digital reconstruction of a multicomponent additively manufactured part

In addition to its ability to produce geometrically complex parts, additive manufacturing offers a unique opportunity to collect data about a component while it is being fabricated. However, there has only been limited effort to characterize parts morphologically and compositionally in situ. In this article, we present a layer-by-layer, laser profilometry-based in situ characterization technique as a method to digitally reconstruct a multi-material part. Data collected by the laser profilometer yields height maps and grayscale images which are voxelized using purpose-built software to volumetrically reconstruct the part. Additionally, the same part was also analyzed using X-ray computed tomography (CT) which was not able to resolve the different compositional regions within the part, but captured the filament morphology. The part was then bisected to compare the digital reconstruction to the actual part morphology and composition. Overall, the digital reconstruction was in good agreement with both the CT and bisected images. Deviations between the digital reconstruction and the CT/bisected images are likely the result of image segmentation settings or material shifts after data was collected. The in situ characterization method demonstrated here sets the stage for real time process monitoring and paves the way for additively manufactured parts that are “born qualified.”

36 MATERIALS SCIENCE↗

The impact of infill percentage and layer height in small-scale material extrusion on porosity and tensile properties

We report material extrusion additive manufacturing is prone to introducing porosity within the structure due to the layer-by-layer construction using elliptical beads of material. This open porosity ultimately plays a role in determining the mechanical properties of printed parts. The shape, size, and amount of porosity within a printed part is influenced by a variety of factors, including nozzle diameter, infill percentage, layer height, raster orientation, and print speed. While several studies have investigated these and other parameters’ effects on mechanical performance and porosity, better understanding the interconnected relationships is crucial in balancing the various input parameters to achieve maximum strength. This work initially examined the influence of key print parameters (infill percentage and layer height) on the internal porosity of a printed Acrylonitrile Butadiene Styrene (ABS) part. Then, the print parameters and internal porosity were statistically correlated to final mechanical properties. Porosity was further classified as either open or closed to differentiate between connected voids in the mesostructure from isolated voids within the material itself. Mechanical performance increased with an increasing density and infill percentage, displaying a 224 % increase in elastic modulus and a 150 % increase in ultimate tensile strength. The contribution of layer height was found to be conditional upon the infill percentage.

3D Printing↗

Online thermal profile prediction for large format additive manufacturing: A hybrid CNN-LSTM based approach

Large format additive manufacturing (LFAM) is an advanced 3D printing technique that efficiently fabricates large-scale components through a layer-by-layer extrusion and deposition process. Accurate surface layer temperature monitoring is essential to prevent manufacturing failures and ensure final product quality. Traditional physics-based offline approaches for simulating thermal behavior are often inefficient and complex, posing challenges on real-time, in-situ monitoring. Here, to address this, we propose a data-driven hybrid CNN-LSTM model to predict sequential thermal images of arbitrary length using real-time infrared thermal imaging. In this approach, a Convolutional Neural Networks (CNN) is trained offline to capture spatial features, reduce dimensional complexity, and enhance time efficiency, while a stacked Long Short-Term Memory (LSTM) is applied online to capture temporal information for improved prediction of future thermal behavior in subsequent printing layers. Model performance is evaluated using MSE, SSIM, and PSNR metrics and is benchmarked against stacked LSTM and convolutional LSTM models, demonstrating superior accuracy and applicability. Additionally, to mitigate noise from moving extruders and gantry backgrounds in thermal images, a fine-tuned semantic segmentation model is implemented offline to extract printing geometry, enabling precise temperature tracking along the tool path for further thermal analysis. The frameworks developed in this study significantly advance temperature monitoring, thermal analysis, and in-situ manufacturing control for LFAM, bridging the gap between theoretical modeling and practical application.

Geometry extraction↗

High compressive energy absorption and shape recovery behavior of additively manufactured textile-inspired cylindrical braided metamaterials

Mechanical metamaterials (MMs) are engineered structures with unique mechanical properties that arise from their unique spatial arrangement or lattice-like structure. The most commonly designed MMs such as honeycomb and re-entrant auxetics are prone to failure at the sharp corners and weak joints due to the increased stress concentration under deformation. To mitigate this challenge, braided MM structures involving intertwining threads of nylon—forming curved unit cells—have been studied. These textile-inspired cylindrical braided metamaterials (CBMMs) with contrasting unit cells, namely diamond and regular CBMMs, were fabricated by 3D printing. The layer-by-layer deposited structure built by fused filament fabrication delivered an assembly of overlapped threads that are fused at the contact point. To understand deformation behavior of these MMs, finite element models were developed for various load scenarios including quasi-static compression, cyclic and creep loads at room temperature. Stress distribution, deformation mechanisms, and failure modes were analyzed and validated by experiments to analyze the geometries and associated performance. The diamond CBMMs showed stress softening at 30 % compressive strain, withstanding a load of ∼440 N, whereas the regular CBMMs at 50 % strain experienced ∼250 N. The diamond CBMMs delivered higher creep resistance under sustained load and better energy absorption under cyclic loading than the regular CBMMs. The latter, however, exhibited 94 % shape recovery in contrast to 88 % recovery in former prototype during their first cyclic load. In conclusion, this study helps design mechanical lightweight devices that endure significant sustained load and exhibit enhanced energy absorption and shape recovery characteristics in cyclic loading.

Creep↗

Effect of different manufacturing methods on polyamide reverse-osmosis membranes for desalination: Insights from molecular dynamics simulations

Membranes are a key technology platform for a broad application of energy-efficient separations. To best serve the separation demands of industry, the manufacturing processes for these membranes are garnering increasing attention. In particular, for water desalination, the industry leading polyamide (PA) reverse osmosis (RO) membranes can be manufactured via molecular layer-by-layer (mLBL) deposition, interfacial polymerization (IP), and 3D-printing technique. However, the influence of different manufacturing methods on PA membrane’s properties is far from understood. Here, in this study, we present the high-pressure transport behavior of water and salt ions for PA membranes formed with IP, mLBL, and 3D-printing through non-equilibrium molecular dynamics simulations. Studies show that membranes fabricated with 3D-printing have similar performances to those manufactured using mLBL, quantified by water permeability, rejection of salt ions, structural integrity, and porosity features. However, the membranes formed with IP exhibit faster water transport, lower rejection, worse structural integrity, and more inhomogeneous network pores than those constructed using mLBL and 3D-printing. The unconnected water-accessible space governs water transport for PA membranes formed with mLBL and 3D-printing, which offers the impermanent open-closed pores that enable water to jump through PA membranes. In contrast, the permeated water-enterable space plays a prominent role in water movement across the PA membrane formed with IP, providing a continuous transport channel at high pressure. Importantly, we observe the more significant compaction features at high pressure for PA membranes formed with IP than mLBL and 3D printing. In short, these findings provide a comprehensive understanding of existing membrane preparation technologies. It also provides a guide for developing the new membrane preparation process at the molecular level.

3D-printing↗

Phase stability and mechanical properties of wire + arc additively manufactured H13 tool steel at elevated temperatures

Wire + arc additive manufacturing (WAAM) is considered an innovative technology that can change the manufacturing landscape in the near future. WAAM offers the benefits of inexpensive initial system setup and a high deposition rate for fabricating medium- and large-sized parts such as die-casting tools. Here, AISI H13 tool steel, a popular die-casting tool metal, is manufactured by cold metal transfer (CMT)-based WAAM and is then comprehensively analyzed for its microstructural and mechanical properties. Location-dependent phase combinations are observed, which could be explained by nonequilibrium thermal cycles that resulted from the layer-by-layer stacking mechanism used in WAAM. In addition, remelting and reheating of the layers reduces welding anomalies (e.g., pores and voids). The metallurgical characteristics of the H13 strongly correlate with the mechanical properties. The combinations of phases at different locations of the additively manufactured part exhibit a periodic microhardness profile. Martensite, Retained Austenite, Ferrite, and Carbide phases are found in combination at different locations of the part based on the part’s temperature distribution during additive deposition. Moreover, the tensile properties at elevated temperatures (23 °C, 300 °C, and 600 °C) are comparable to those from other WAAM and additive manufacturing (AM) processes. The X-ray diffraction results verify that the microstructural stability of the fabricated parts at high temperatures would allow them to be used in high temperatures.

36 MATERIALS SCIENCE↗

Flexible all-organic nanocomposite films interlayered with in situ synthesized covalent organic frameworks for electrostatic energy storage

Poly(vinylidene fluoride)-based terpolymers, known for having the largest dielectric constant among the existing dielectric polymers, are attractive materials for electrostatic film capacitors used in lightweight electrification systems. However, the potential of these terpolymers in film capacitor applications remains constrained by their low electrical insulating and mechanical strengths. To address these limitations, we introduced rigid covalent organic framework (COF) nanospheres into the thin films of soft terpolymers via in situ synthesis and a facile layer-by-layer solution casting method, whereby multilayer films consisting of two polymer outer layers and a COF-containing middle layer were readily obtained. The resultant all-organic thin films exhibit simultaneously high dielectric constant, enhanced breakdown strength, superior energy density (~25 J cm –3 ) at efficiencies over 80%, along with greatly improved mechanical self-supporting capability and excellent mechanical flexibility. Here, this work demonstrates the unprecedented use of COF for electrostatic energy storage, uncovering its potential for flexible electronic applications operating under high electric fields.

25 ENERGY STORAGE↗