Graduation Year

2010

Document Type

Dissertation

Degree

Ph.D.

Degree Granting Department

Physics

Major Professor

Sarath Witanachchi, Ph.D.

Committee Member

Pritish Mukherjee, Ph.D.

Committee Member

Hariharan Srikanth, Ph.D.

Committee Member

Xiaomei Jiang, Ph.D.

Keywords

thin films, lead selenide quantum dots, nanoparticles, multiple exciton generation, exciton dissociation, solar cells

Abstract

This work describes an experimental investigation of methods of synthesis, determination of structural and physical properties, and analysis and correlation of the properties to the structures of semiconductor quantum dots and quantum dot-polymer hybrid structures. These structures are investigated for applications in flexible solar cell devices. The main synthesis process used in the work was a Laser-Assisted Spray (LAS) process that was developed in our laboratory to deposit surfactant-free PbSe quantum dot (QD) films directly on a substrate. The QD films formed by this technique are in close contact with each other forming a percolation path for charge transport. Analytical instruments that include Atomic Force Microscopy (AFM) and Transmission Electron Microscopy (TEM) were used for structural characterization while optical absorption spectroscopy and photoluminescence were used for determining the quantum confinement of charge carriers in PbSe QDs. In addition, charge transport across lithographically patterned paths was used to determine the transport characteristics and generation of photocurrent in the fabricated structures.

Absorption spectroscopy confirmed the quantum confinement of PbSe QDs deposited by LAS deposition. Room temperature current-voltage measurements across a 2 micrometer tunnel junction formed by the QDs produced a power-law dependence of the form I ∝ V2.19 that describes a percolation path of dimensionality slightly above two-dimensional. Absence of surfactants in LAS deposited films improved the conductivity by more than three orders of magnitude. Temperature dependent conductance studies showed thermally activated transport at high temperatures and temperature independent tunneling followed by previously unobserved metallic conduction at low temperatures.

The LAS system was successfully modified by incorporating two spray nozzles to transport aerosols of two different precursors, one containing the QDs and the other containing the polymer. This new co-deposition system was successfully used to deposit QDs/Polymer hybrid structures. The TEM and XRD studies of LAS co-deposited films were shown to be uniformly distributed and crystalline. The photo-current experiments of QD/polymer hybrid composites showed clear evidence of enhanced carrier generation and transport as a result of intimate contact between quantum dots (QDs).

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