An ability to engineer the structure of semiconductor nanowires is essential for tuning their optical, electrical, and thermal transport properties. While manipulation of growth conditions offers an empirical route to control both the orientation of nanowire growth and the stacking of individual atomic layers, a fundamental understanding of chemical bonding that underlies these changes remains unclear and limits rational control of the process. In this talk, we will discuss our recent real-time in-situ spectroscopic studies of Si nanowires synthesized via the vapor-liquid-solid (VLS) mechanism and highlight the importance of adsorbed hydrogen atoms in controlling nanowire structure. The use of this knowledge to fabricate user-programmable nanowire superstructure will also be presented.

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