Bulk and Local Electron Transport and Optical Properties of Aluminum-doped Zinc Oxide.

摘要

ZnO is a promising transparent conducting oxide (TCO) because its components are naturally abundant and inexpensive; and ZnO can be synthesized by several methods as thin films and nanostructures. Doping ZnO with Al (to form what is called AZO) significantly increases electrical conductivity while retaining high optical transparency, making AZO ideal for use as transparent electrodes in optoelectronic devices. However, the electrical conductivity of AZO has not exceeded that of indium tin oxide (ITO), the most widely-utilized TCO. A systematic study of bulk and local electrical and optical properties of AZO is needed to improve conductivity while maintaining transparency.;To this end, we conducted bulk magnetotransport measurements on AZO, which indicated that its electron mobility was significantly lower than that of single-crystal ZnO, primarily due to electron scattering at AZO grain boundaries. To further understand this detrimental effect, we directly probed these grain boundaries with a scanning tunneling microscope. These measurements are the first investigation of a broad spectrum of grain boundary traps in AZO, which include shallow states near the conduction band edge that may limit electron mobility, and deeper states that may deplete carriers.;Because optical properties can affect transparency in devices, we characterized AZO through a combination of photoluminescence and scanning tunneling microscope cathodoluminescence (STM-CL). STM-CL, which probes only the surface, shows a dramatic narrowing of emission lines compared to bulk photoluminescence. We attribute this to different charge states of oxygen vacancies preferentially located near the surface. This observed difference is especially of interest in understanding transport across interfaces.;Finally, we present one application of AZO: a monolayer quantum dot (QD) light-emitting device with AZO electrodes that uses atomic layer deposited insulating oxide to fill the interstices among QDs. This combination of conducting and insulating oxide structures forces tunnel injected hot carriers through QDs and allows for chemical treatment of ligands without QD agglomeration. This device serves as a model for a new class of all-oxide, high current density QD devices.;These investigations further the understanding of carrier conduction and surface optical properties of AZO and will contribute to optimization for TCO device applications.