Nanoparticles of various materials are known to exhibit excellent mechanical, chemical, electrical, and optical properties. However, it is difficult to deposit and transform nanoparticles into large two-dimensional and three-dimensional structures, such as thin films and discrete arrays. Electrospray technology and laser heating enable the deposition of these nanoparticles through the dual role of microdroplets as nanoparticle carriers and superlenses. The main goals of this dissertation are to delineate the electrospray modes, to achieve subwavelength focusing, and to enable a process for the deposition of nanoparticles into microlayers and discrete nanodots (a nanodot is a cluster of nanoparticles) on rigid and flexible substrates. This additive manufacturing process is based on the electrospray generation of water microdroplets that carry nanoparticles onto a substrate and the laser sintering of these nanoparticles. The process involves injecting nanoparticles (contained inside electric field-driven water microdroplets) into a hollow laser beam. The laser beam heats the droplets, causing the water to evaporate and the nanoparticles to sinter and form deposit of material on the substrate. The electrohydrodynamic inkjet printing of nanoparticle suspensions has been accomplished by the operation of an electrospray in microdripping mode and it allows the deposition of monodisperse microdroplets containing nanoparticles into discrete nanodot arrays, narrow lines, and thin films. For flow rates with low Reynolds number, the mode changes from dripping to microdripping mode, and then to a planar oscillating microdripping mode as the electric capillary number, Cae increases. The microdripping mode which is important for depositing discrete array of nanodots is found to occur in a narrow range, 2 ≤ Cae ≤ 2:5. The effect of the physical properties on the droplet size and frequency of droplet formation is more precisely described by the relative influence of the electric, gravity, viscous, and capillary forces. A scaling analysis is derived from a fundamental force balance and has yielded a parameter based on the electric capillary number, capillary number, and Bond number. Results for different nanoparticle suspensions with a wide range of physical properties show that the normalized radius of droplet, can be correlated using this parameter in both dripping and microdripping modes. The same parameter also correlates the normalized frequency of droplet formation, N*d as an increasing function in the microdripping mode. Viscosity affects the shape of the cone by resisting its deformation and thus promoting a stable microdripping mode. Reduction in surface tension decreases the droplet size in the electrospray modes. However, the capillary size and electrical conductivity have minimal effect on the size of the ejected droplets. Electrical conductivity affects the transition between microdripping and oscillating microdripping modes. Based on this analysis, it is possible to design the electrospray to produce uniform monodisperse droplets by manipulating the voltage at the electrode, for any desired nanoparticle concentration of a suspension to be sintered on a substrate. For the fabrication of nanodots, a laser beam of wavelength λ = 1064 nm was focused to a diameter smaller than its wavelength. When the microdroplets did not carry nanoparticles, the subwavelength focusing of the laser yielded nanoholes smaller than its wavelength. Results show that tiny features with high resolution can be created by loading microdroplets with nanoparticles and squeezing the laser beam to subwavelength regions. Nanodots of silicon and germanium with diameters between 100 - 500 nm have been deposited on a silicon substrate. This study demonstrates an interdisciplinary mechanism to achieve subwavelength focusing in a laser process. In this process, the microdroplets serve as both a nanoparticle carrier and a superlens that focuses a laser beam to subwavelength diameters up to λ/10, thus overcoming the diffraction limit. The microdroplets are generated from a suspension of nanoparticles using an electrospray technique and the superlens characteristic of these microdroplets is attributed to three optical phenomena such as Maxwell's fish eye lens or Luneberg lens, evanescent waves by laser scattering, and evanescent waves by the total internal reflection principle. A microfluidic cooling effect can also contribute to creating subwavelength features. In summary, this work describes a new laser-assisted additive manufacturing process for the fabrication of nanodots and microlayers using nanoparticles of different materials. In this process, microdroplets from an electrospray are used as nanoparticle carriers and superlenses to focus the laser to a diameter smaller than its wavelength. While this process is demonstrated to produce subwavelength holes and nanodots, the process is scalable to produce narrow lines and thin films of semiconductor materials by an additive manufacturing technique. This process extends the application of infrared lasers to the production of nanostructures and nanofeatures, and, therefore, provides a novel technology for nanomanufacturing.
Doctor of Philosophy (Ph.D.)
College of Engineering and Computer Science
Mechanical and Aerospace Engineering
Length of Campus-only Access
Doctoral Dissertation (Open Access)
Castillo Orozco, Eduardo, "Electrospray and Superlens Effect of Microdroplets for Laser-Assisted Nanomanufacturing" (2018). Electronic Theses and Dissertations, 2004-2019. 6424.