Structural and surface correlations to the optical properties of nonthermal plasma-produced silicon nanoparticles

University of Minnesota Ph.D. dissertation. June 2011. Major: Mechanical Engineering. xi, 150 pages. Advisor: Uwe Kortshagen. 1 computer file (PDF); ix, 150 pages, appendices A-F.Nanomaterials have diverse capabilities to enable new technology and to deepen our understanding of our world, providing exciting prospects for scientists and the public alike in a vast span of uses. In the past decade, however, the potential held by nanotechnology has been reframed in the context of helping to slow global climate change and to alter the ways in which we use our energy to reflect more efficient technology and renewable energy sources. Silicon is a standout material in this new framework: as a nanomaterial, silicon can emit light when exposed to an applied voltage or ultraviolet optical excitation source. Silicon nanocrystals also exhibit size-dependent light emission, due to quantum confinement. This thesis is an exploration of the synthesis and processing parameters that affect the optical performance of silicon nanocrystals produced in a nonthermal plasma reactor. The efficiency of this light emission is sensitive to both synthesis environment and post-synthesis treatment. The work presented here is an attempt to deepen our understanding of the effects of different reactor and treatment parameters on the light emission efficiency from silicon nanoparticles, such that the luminescence behavior of the nanoparticles can be specifically engineered. Being able to fine-tune the structure, surface, and optical characteristics of the silicon nanocrystals is key in maximizing their use in luminescence applications. For all of the experiments described here, a nonthermal plasma flow-through reactor has been used to create the silicon nanoparticles. Silane gas is dissociated in the plasma and fragments come together to form silicon clusters, then grow to create nanoparticles. The nanoparticles were collected from the reactor for further processing, characterization, and experiments. The first discovery in this project was that by adjusting the power to the plasma reactor, the crystallinity of the silicon particles can be tuned: low power results in amorphous silicon nanoparticles, and high power yields crystalline nanoparticles. Even more important, the crystallinity of a nanoparticle ensemble relates directly to the photoluminescence (PL) efficiency, or quantum yield, from the ensemble: crystalline silicon nanoparticle samples, after alkyl functionalization, exhibit PL efficiencies of 40% or greater, while amorphous samples emit light with very poor efficiency (