Colloidal quantum dots (CQD) are used in the fabrication of efficient, low-cost solar cells synthesized in and deposited from solution. Breakthroughs in CQD materials have led to a record efficiency of 7.0%. Looking forward, any path toward increasing efficiency must address the trade-off between short charge extraction lengths and long absorption lengths in the near-infrared spectral region. Here we exploit the localized surface plasmon resonance of metal nanoparticles to enhance absorption in CQD films. Finite-difference time-domain analysis directs our choice of plasmonic nanoparticles with minimal parasitic absorption and broadband response in the infrared. We find that gold nanoshells (NS) enhance absorption by up to 100% at λ = 820 nm by coupling of the plasmonic near-field to the surrounding CQD film. We engineer this enhancement for PbS CQD solar cells and observe a 13% improvement in short-circuit current and 11% enhancement in power conversion efficiency.

Colloidal quantum dots (CQD) are used in the fabrication of efficient, low-cost solar cells synthesized in and deposited from solution. Breakthroughs in CQD materials have led to a record efficiency of 7.0%. Looking forward, any path toward increasing efficiency must address the trade-off between short charge extraction lengths and long absorption lengths in the near-infrared spectral region. Here we exploit the localized surface plasmon resonance of metal nanoparticles to enhance absorption in CQD films. Finite-difference time-domain analysis directs our choice of plasmonic nanoparticles with minimal parasitic absorption and broadband response in the infrared. We find that gold nanoshells (NS) enhance absorption by up to 100% at λ = 820 nm by coupling of the plasmonic near-field to the surrounding CQD film. We engineer this enhancement for PbS CQD solar cells and observe a 13% improvement in short-circuit current and 11% enhancement in power conversion efficiency.

In this thesis, three specific research contributions to the use of non-uniform electric field driven colloidal assembly are described. The first relates to experimental work using dielectrophoretic and electrohydrodynamic forces (electroosmosis) to shape three-dimensional colloidal structures. Formation and stabilization of close-packed three-dimensional structures from colloidal silica was demonstrated, using gelation of pluronic F-127 to preserve medium structure against suspension evaporation. Stabilization of ordered structures was shown to be a significant challenge, with many of the conventional techniques for immobilizing colloidal crystals being ineffective. Secondly, the significance of electrohydrodynamic flows resulting from electric and particle concentration (entropic) gradients during the assembly process was demonstrated using numerical simulations based on a thermodynamic framework. These simulations, as well as experimental validation of assembly and the presence of fluid flows, showed that assuming equilibrium behavior (stationary fluid flow), a common assumption for most modelling work to date in these systems, is inappropriate at all but the most dilute concentration cases. Finally, the relevance of multiparticle effects on electric-field induced phase transitions of dielectric colloids was demonstrated. The effect of multiparticle/multiscattering effects on the suspension permittivity were accounted for using semi-empirical continuum permittivity formulations which have been previously shown to describe a wide variety of solid packing structures, including face-centered cubic and other colloidal crystal structures. It was shown that multiparticle effects have a significant impact on both the coexistence (slow phase separation) and spinodal (fast phase separation) behavior of dielectric suspensions, which has not been demonstrated to date using a continuum framework. / Thesis (Ph.D, Chemical Engineering) -- Queen's University, 2012-01-30 14:17:23.747

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Thesis (M.S.) in Biological Engineering--University of Maine, 2008. / Includes vita. Includes bibliographical references (leaves 39-42).

Thesis (M.Phil.)--Hong Kong University of Science and Technology, 2005. / Includes bibliographical references. Also available in electronic version.

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