Date of Award

Spring 1-1-2012

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Physics

First Advisor

Arthur J. Nozik

Second Advisor

Daniel S. Dessau

Third Advisor

Steven T. Cundiff

Fourth Advisor

Markus B. Raschke

Fifth Advisor

Charles T. Rogers

Abstract

Photovoltaics are limited in their power conversion efficiency (PCE) by very rapid relaxation of energetic carriers to the band edge. Therefore, photons from the visible and ultraviolet parts of the spectrum typically are not efficiently converted into electrical energy. One approach that can address this is multiple exciton generation (MEG), where a single photon of sufficient energy can generate multiple excited electron-hole pairs. This process has been shown to be more efficient in quantum dots than bulk semiconductors, but it has never been demonstrated in the photocurrent of a solar cell.

In order to demonstrate that multiple exciton generation can address fundamental limits for conventional photovoltaics, I have developed prototype devices from colloidal PbS and PbSe quantum dot inks. I have characterized both the colloidal suspensions and films of quantum dots with the goal of understanding what properties determine the efficiency of the solar cell and of the MEG process. I have found surface chemistry effects on solar cells, photoluminescence, and MEG, and I have found some chemical treatments that lead to solar cells showing MEG. These devices show external quantum efficiency (EQE) greater than 100% for certain parts of the solar spectrum, and I extract internal quantum efficiency (IQE) consistent with previous measurements of colloidal suspensions of quantum dots.

These findings are a small first step toward breaking the single junction Shockley-Queisser limit of present-day first and second generation solar cells, thus moving photovoltaic cells toward a new regime of efficiency.

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