Optical Properties and Ensemble Characteristics of Size Purified Silicon Nanocrystals

Nanotechnology is at the forefront of current scienti c research and nanocrystals are being hailed as the `arti cial' atoms of the 21st century. Semiconducting silicon nanocrystals (SiNCs) are prime candidates for potential commercial applications because of silicon's already ubiquitous...

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Bibliographic Details
Main Author: Miller, Joseph Bradley
Format: Others
Published: North Dakota State University 2018
Online Access:https://hdl.handle.net/10365/27408
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Summary:Nanotechnology is at the forefront of current scienti c research and nanocrystals are being hailed as the `arti cial' atoms of the 21st century. Semiconducting silicon nanocrystals (SiNCs) are prime candidates for potential commercial applications because of silicon's already ubiquitous presence in the semiconductor industry, nontoxicity and abundance in nature. For realization of these potential applications, the properties and behavior of SiNCs need to be understood and enhanced. In this report, some of the main SiNC synthesis schemes are discussed, including those we are currently experimenting with to create our own SiNCs and the one utilized to create the SiNCs used in this study. The underlying physics that governs the unique behavior of SiNCs is then presented. The properties of the as-produced SiNCs are determined to depend strongly on surface passivation and environment. Size puri cation, an important aspect of nanomaterial utilization, was successfully performed on our SiNCs though density gradient ultracentrifugation. We demonstrate that the size-puri ed fractions exhibit an enhanced ability for colloidal self-assembly, with better aligned nanocrystal energy levels which promotes greater photostability in close-packed lms and produces a slight increase in photoluminescence (PL) quantum yield. The qualities displayed by the fractions are exploited to form SiNC clusters that exhibit photostable PL. An analysis of SiNC cluster (from individual nanocrystals to collections of more than one thousand) blinking and PL shows an improvement in their PL emitting `on' times. Pure SiNC lms and SiNC-polymer nanocomposites are created and the dependence of their PL on temperature is measured. For such nanocomposites, the coupling between the `co ee-ring' e ect and liquid-liquid phase separation is also examined for ternary mixtures of solvent, polymer and semiconducting nanocrystal. We discover that with the right SiNC-polymer concentration and polymer molecular weight, phase separation can be supressed; we use this to build a prototype nanocomposite printing device. Finally, the nanocrystals are PEGylated and introduced into an aqueous biological environment to demonstrate their potential for use in biological labelling and sensing devices. The development of superlattice structures from monodisperse SiNC fractions and their use in solid-state lighting and solar cell applications are also explored.