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Aerosol jet printing is a compelling technology for hybrid electronics, combining digital and noncontact patterning with broad materials compatibility, resolution as fine as ≈10 microns, and a high standoff distance of 1–5 mm. Despite its growing popularity in research environments, a robust process understanding and improved manufacturing control are essential for achieving the reliability and predictability required for broader adoption in advanced applications. Herein, recent developments in process monitoring using in‐line light scattering measurements are discussed, including their mechanistic foundations, experimental validation, relevance for process control and reliability, and value as a diagnostic tool for fundamental studies. Experimental measurements confirm the correlation between measured light scattering and deposition rate. Building on this platform, feedback from the real‐time measurement is coupled with printer software to support automated closed‐loop control via a simple proportional‐integral‐derivative software control loop. Combined with the utility of these measurements as a diagnostic to accelerate ink formulation and support fundamental process science experiments, this in‐line measurement provides a useful tool to improve print reliability with the potential to advance the adoption and capabilities of this method in conformal, flexible, and hybrid electronics applications. 

Abstract Aerosol jet printing offers high resolution, broad materials compatibility, and digital patterning for flexible, conformal, and hybrid electronics. However, limited throughput, instability, and complex optimization requirements inhibit translation to industrial applications. An in‐line heater integrated on a custom printer is demonstrated to modulate droplet evaporation in the aerosol phase, thereby decoupling the deposition rate of functional solids and liquid ink to enable taller, narrower features with aspect ratios reaching 0.29 for a single line. Heating the printhead from room temperature to 80 °C reduced the sensitivity of resolution to deposition rate by ≈90%, improving reliability. With this strategy, increasing the linear deposition rate by 10x results in a modest increase of 27% in line width, compared to a four‐fold increase without heating, permitting higher throughput without sacrificing print quality. Providing a control for in‐line drying independent of ink formulation enables rapid, straightforward design of new materials and processes. This ability to engineer drying of droplets prior to impingement provides a versatile tool to meet complex fabrication challenges, as demonstrated here for both high aspect ratio printing and conformal patterning on rough and three‐dimensional surfaces. 

Abstract Aerosol jet printing is a popular digital additive manufacturing method for flexible and hybrid electronics, but it lacks sophisticated real‐time process control schemes that would enable more widespread adoption in manufacturing environments. Here, an optical measurement system is introduced to track the aerosol density upstream of the printhead. The measured optical extinction, combined with the aerosol flow rate, is directly related to deposition rate and accurately predicts functional materials properties such as the electrical resistance of printed graphene films. This real‐time system offers a compelling solution for process drift and batch‐to‐batch variability, rendering it a valuable tool for both real‐time control of aerosol jet printing and fundamental studies of the underlying process science.