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The growing demand for flexible and wearable hybrid electronics has triggered the need for advanced manufacturing techniques with versatile printing capabilities. Complex ink formulations, use of surfactants/contaminants, limited source materials, and the need for high‐temperature heat treatments for sintering are major issues facing the current inkjet and aerosol printing methods. Here, the nanomanufacturing of flexible hybrid electronics (FHE) by dry printing silver and indium tin oxide on flexible substrates using a novel laser‐based additive nanomanufacturing process is reported. The electrical resistance of the printed lines is tailored during the print process by tuning the geometry and structure of the printed samples. Different FHE designs are fabricated and tested to check the performance of the devices. Mechanical reliability tests including cycling, bending, and stretching confirm the expected performance of the printed samples under different strain levels. This transformative liquid‐free process allows the on‐demand formation and in situ laser crystallization of nanoparticles for printing pure materials for future flexible and wearable electronics and sensors.

 

Direct printing of functional materials, structures, and devices on various platforms such as flexible to rigid substrates is of interest for applications ranging from electronics to energy and sensing to biomedical devices. Current additive manufacturing (AM) and printing processes are either limited by the available sources of functional materials or require to be in the form of precisely designed inks. Here, a novel laser‐based additive nanomanufacturing (ANM) system capable of in situ and on‐demand generations of nanoparticles that can serve as nanoscale building blocks for real‐time sintering and dry printing a variety of multifunctional materials and patterns at atmospheric pressure and room temperature is reported. The ability to print different functional materials on various rigid and flexible platforms is shown. This nonequilibrium process involves pulsed laser ablation of targets and in situ formation of pure amorphous nanoparticles’ stream that are guided through a nozzle onto the surface of the substrate, where they are sintered/crystallized in real‐time. Further, the process–structure relationship of the printed materials from nanoscale to microscale is shown. This new ANM concept opens up an opportunity for printing advanced functional materials and devices on rigid and flexible substrates that can be employed both on the earth and in space.

 

The reliability of additively manufactured flexible electronics or so-called printed electronics is defined as mean time to failure under service conditions, which often involve mechanical loads. It is thus important to understand the mechanical behavior of the printed materials under such conditions to ensure their applicational reliability in, for example, sensors, biomedical devices, battery and storage, and flexible hybrid electronics. In this article, a testing protocol to examine the print quality of additively nanomanufactured electronics is presented. The print quality is assessed by both tensile and electrical resistivity responses during in-situ tension tests. A laser based additive nanomanufacturing method is used to print conductive silver lines on polyimide substrates, which is then tested in-situ under tension inside a scanning electron microscope (SEM). The surface morphology of the printed lines is continuously monitored via the SEM until failure. In addition, the real-time electrical resistance variations of the printed silver lines are measured in-situ with a multimeter during tensile tests conducted outside of the SEM. The protocol is shown to be effective in assessing print quality and aiding process tuning. Finally, it is revealed that samples appearing identical under the SEM can have significant different tendencies to delaminate. 

Additively manufactured electronics (AMEs), also known as printed electronics, are becoming increasingly important for the anticipated Internet of Things (IoT). This requires manufacturing technologies that allow the integration of various pure functional materials and devices onto different flexible and rigid surfaces. However, the current ink-based technologies suffer from complex and expensive ink formulation, ink-associated contaminations (additives/solvents), and limited sources of printing materials. Thus, printing contamination-free and multimaterial structures and devices is challenging. Here, a multimaterial additive nanomanufacturing (M-ANM) technique utilizing directed laser deposition at the nano and microscale is demonstrated, allowing the printing of lateral and vertical hybrid structures and devices. This M-ANM technique involves pulsed laser ablation of solid targets placed on a target carousel inside the printer head for in-situ generation of contamination-free nanoparticles, which are then guided via a carrier gas toward the nozzle and onto the surface of the substrate, where they are sintered and printed in real-time by a second laser. The target carousel brings a particular target in engagement with the ablation laser beam in predetermined sequences to print multiple materials, including metals, semiconductors, and insulators, in a single process. Using this M-ANM technique, various multimaterial devices such as silver/zinc oxide (Ag/ZnO) photodetector and hybrid silver/aluminum oxide (Ag/Al2O3) circuits are printed and characterized. The quality and versatility of our M-ANM technique offer a potential manufacturing option for emerging IoT. 

Interest in layered two-dimensional (2D) materials has been escalating rapidly over the past few decades due to their promising optoelectronic and photonic properties emerging from their atomically thin 2D structural confinements. When these 2D materials are further confined in lateral dimensions toward zero-dimensional (0D) structures, 2D nanoparticles and quantum dots with new properties can be formed. Here, we report a nonequilibrium gas-phase synthesis method for the stoichiometric formation of gallium selenide (GaSe) nanoparticles ensembles that can potentially serve as quantum dots. We show that the laser ablation of a target in an argon background gas condenses the laser-generated plume, resulting in the formation of metastable nanoparticles in the gas phase. The deposition of these nanoparticles onto the substrate results in the formation of nanoparticle ensembles, which are then post-processed to crystallize or sinter the nanoparticles. The effects of background gas pressures, in addition to crystallization/sintering temperatures, are systematically studied. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), photoluminescence (PL) spectroscopy, and time-correlated single-photon counting (TCSPC) measurements are used to study the correlations between growth parameters, morphology, and optical properties of the fabricated 2D nanoparticle ensembles.